สิทธิบัตรเรื่ องเต็มจากฐาน EPO Worldwide (http://gb.espacenet.com) ปี 1934-2005
เกี่ยวกับ "Essential
Oil"
1. AR241201 - 31.01.1992
DEVICE TO EXTRACT WITH WATER STEAM ESSENTIAL OIL FROM A VEGETABLE MATTER.
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AR241201
Applicant(s):
LEGAST ETIENNE (CH)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
AR19860304996 (19860821)
Priority Number: AR19860304996 (19860821)
Family: AR241201
1/1651
2. AU2260900 - 15.06.2000
EXTRACTION OF ESSENTIAL OIL FROM CYPRESS PINE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU2260900
Inventor(s):
COLLINS VINCENT JOSEPH (--)
Applicant(s):
COLLINS VINCENT JOSEPH (--); COLLINS MARYANN (--)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
AU20000022609D (20000324)
Priority Number: AU20000022609 (20000324)
Family: AU2260900
2/1651
3. AU3300502 - 06.06.2002
EXTRACTION OF ESSENTIAL OIL FROM CYPRESS PINE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU3300502
Inventor(s):
COLLINS VINCENT JOSEPH (--)
Applicant(s):
MARYANN COLLINS (--); COLLINS VINCENT JOSEPH (--)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
AU20020033005D (20020410)
Priority Number: AU20020033005 (20020410)
Family: AU3300502
3/1651
4. AU4096497 - 17.09.1998
A PROCESS FOR THE SIMULTANEOUS PRODUCTION OF ARTEMISNIN AND ESSENTIAL OIL
FROM THE PLANT ARTEMISIA ANNUA
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU4096497
Applicant(s):
COUNCIL SCIENT IND RES (--)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
AU19970040964D (19971010)
Priority Number: IN1997CA00652 (19970317)
Family: AU4096497
4/1651
5. AU4545197 - 22.06.2000
ESSENTIAL OIL AND METHODS OF USE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU4545197
Inventor(s):
HOOD JOHN JAMES DAVID (--)
Applicant(s):
JOHN JAMES DAVID HOOD (--)
IP Class 4 Digits: A61K; C11B; C23F
IP Class:
A61K35/78; C11B9/00; C23F11/00
Application Number:
AU19970045451 (19971020)
Priority Number: AU1996PO03167 (19961023); WO1997AU00701 (19971020); AU19970045451
(19971020)
Family: AU721156
5/1651
6. AU4581796 - 12.09.1996
CENTRIFUGE FOR RECOVERY OF ESSENTIAL OIL FROM CITRUS FRUIT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU4581796
Inventor(s):
HEYDEN-LINDEN JOSEF VON (DE); KOHLSTETTE WERNER (DE); KREIMER
JOHANNES DIPL ING (DE); JAHN NORBERT (DE); MACKEL WILFRIED DIPL ING (DE)
Applicant(s):
WESTFALIA SEPARATOR AG (DE)
IP Class 4 Digits: C11B; A23L; B04B
IP Class:
C11B9/02; A23L1/222; B04B1/08; B04B11/06; B04B1/12; B04B1/10
E Class: C11B9/02; A23L1/222B; B04B1/08
Application Number:
DE19951008334 (19950309)
Priority Number: DE19951008334 (19950309)
Family: DE19508334
Equivalent:
BR9600958; ES2127676; IT1287536; ITGE960016; JP8257438
Abstract:
PROCESS FOR RECOVERING ESSENTIAL OIL FROM CITRUS FRUIT, IN WHICH AN OIL-WATER
MIXT. RECOVERED FROM AN EXTRACTOR, CONSISTING OF CA. 86% WATER, 10% PEEL
RESIDUES, PECTIN AND MUCILAGEOUS SUBSTANCES. 3% OIL EMULSION AND 1% SOLID
MATERIAL, IS PROCESSED IN A SINGLE CENTRIFUGE IN WHICH THE MIXT. IS SEPD. INTO
THREE PHASES OF OIL, WATER AND MUCILAGEOUS SUBSTANCES, THESE PHASES BEING
WITHDRAWN CONTINUOUSLY FROM THE CENTRIFUGE DRUM WHILE THE SOLID RESIDUAL
MATERIAL (PECTIN AND PEEL RESIDUES) IS CENTRIFUGED OUT OF THE DRUM
DISCONTINUOUSLY.Description:
6/1651
Die Erfindung bezieht sich auf ein Verfahren zur Gewinnung von Essenzцl aus Zitrusfrьchten, bei
dem das aus einem Extraktor ablaufende Цl-Wasser- Gemisch, das aus ca. 86% Wasser, 10%
Schalenresten, Pektinen und Schleimstoffen, 3% Цlemulsion und aus 1% Fettstoffen besteht, durch
zentrifugale Behandlung in verschiedene Phasen aufgetrennt wird.
Es ist ein Verfahren dieser Art bekannt, bei dem zwei Zentrifugen zum Einsatz kommen (Druckschrift
der Firma Westfalia Separator AG Nr. 9997-9139-000, "Separatoren, Dekanter und Prozesslinien fьr
die Citrus- Verarbeitung", Abb. 35, Seite 25).
Bei dem bekannten Verfahren wird das aus dem Extraktor ablaufende Цl- Wasser-Gemisch in einer
ersten Zentrifuge in eine wasserhaltige Цlphase mit mindestens 60% Цl und in eine цlhaltige
Wasserphase mit Schleimstoffen und Feststoffen aufgetrennt.
Das aus der Zentrifuge ablaufende Wasser wird zu 60% in den Prozess zurьckgefьhrt, um den
Wasserverbrauch zu reduzieren. Die restlichen 40% Wasser mьssen entsorgt und durch
Frischwasser ersetzt werden, was zu einer allgemein bekannten Abwasserproblematik fьhrt.
Ausserdem enthдlt dieses Wasser noch Цlanteile, die sich als Цlverluste auswirken. Dadurch wird
nur eine Ausbeute von 83 bis 85% Цl erzielt.
Da das aus der Zentrifuge ablaufende Wasser durch die mechanische Beanspruchung beim
Durchlauf durch die Zentrifuge stark mit Feinstoffen und Pektinen emulgiert, lдsst sich das Цl auch
durch eine Behandlung in einer weiteren Zentrifuge nicht mehr abtrennen.
Der Erfindung liegt die Aufgabe zugrunde, das zentrifugale Trennverfahren und die zur
Durchfьhrung dieses Trennverfahrens verwendete Zentrifuge so auszubilden, dass die Цlausbeute
erhцht und die Abwassermenge verringert wird.
Diese Aufgabe wird beim Verfahren dadurch gelцst, dass ausschliesslich eine Zentrifuge verwendet
wird, mit der eine Auftrennung in drei flьssige Phasen, nдmlich Цl, Wasser und Schleimstoffe
(Anteile von Wasser, pektinen und kleineren Schalenresten) vorgenommen wird und diese Phasen
kontinuierlich aus der Schleudertrommel der Zentrifuge abgezogen werden, wдhrend die ferner
anfallenden Feststoffe (Anteile von pektinen und grцsseren Schalenresten) diskontinuierlich aus der
Schleudertrommel abgeschleudert werden.
7/1651
Der separate Abzug der Schleimstoffe (Wasser plus Pektine plus Schalenreste) bewirkt eine
erhebliche Reduzierung dieser Stoffe im abgetrennten Wasser, so dass bei dem
erfindungsgemдssen Verfahren 90% des Wassers in den Prozess zurьckgefьhrt werden kцnnen.
Dadurch wird nicht nur der Frischwasserverbrauch reduziert, sondern es wird auch die mit dem
Abwasser abgeschiedene Цlmenge erheblich vermindert und eine Цlausbeute von 95 bis 96%
ermцglicht.
Weiterhin kцnnen auch die Kosten fьr das Eindampfen des Abwassers erheblich verringert werden.
Bei dem bekannten Verfahren wurde als erste Zentrifuge, der das aus dem Extraktor ablaufende ЦlWasser-Gemisch nach diversen Vorbehandlungen zugefьhrt wurde, mit einer Schleudertrommel
ausgerьstet, bei der die Zufьhrkanдle eines Verteilers in Steigekanдle eines vom Verteiler
getragenen Tellereinsatzes mьnden. Die Trennzone fьr das zugefьhrte Цl-Wasser- Gemisch liegt
somit in diesen Steigekanдlen. Das abgetrennte wasserhaltige Цl wandert radial einwдrts und wird
durch in der Nдhe der Drehachse liegende Kanдle aus der Schleudertrommel abgeleitet. Das
abgetrennte цlhaltige Wasser mit den Schleimstoffen wandest radial auswдrts und wird durch die
vom peripheren Bereich der Schleudertrommel ausgehenden Kanдle abgeleitet. Die Schleimstoffe
und Цlbestandteile fьhren in der Wasserphase zur Bildung einer Emulsion, durch die der
Tellereinsatz verstopfen kann. Ausserdem muss ein grosser Anteil der Wasserphase wegen der
hohen Belastung mit Цl und Schleimstoffen aus dem Prozess herausgefьhrt und durch
Frischwasser ersetzt werden.
Wegen der Stossempfindlichkeit des Цl-Wasser-Gemisches hat sich eine nachtrдgliche
Behandlung der Wasserphase durch einen zweiten Zentrifugalvorgang bei dem bekannten Verfahren
als unwirksam herausgestellt. Durch einen zweiten Zentrifugalvorgang ist eine derart hohe
Beanspruchung der Wasserphase durch mechanische Einwirkung und Lufteinschlag vorhanden,
dass die dadurch bewirkte Emulsionsbildung sich nicht mehr auftrennen lдsst.
Bei der Zentrifuge wird diese Aufgabe durch die kennzeichnenden Merkmale des Patentanspruches
2 gelцst.
Die einzige Zentrifuge, die beim erfindungsgemдssen Verfahren eingesetzt wird, weist eine
Schleudertrommel auf, die sich in ihrem konstruktiven Aufbau erheblich von der Schleudertrommel
der Zentrifugen unterscheidet, die beim bekannten Verfahren verwendet wurden.
8/1651
Bei der erfindungsgemдssen Zentrifuge ist der Trennraum der Schleudertrommel durch einen
Trennteller in eine untere und eine obere Abteilung unterteilt, wobei in der unteren Abteilung ein
erster Tellereinsatz vorgesehen ist, dessen Aussendurchmesser kleiner ist als die durch die
Zufьhrkanдle des Verteilers definierte Trennzone. Der zentrale Bereich des ersten Tellereinsatzes
steht mit Ableitkanдlen fьr die Цlphase in Verbindung. Der periphere Bereich des ersten
Tellereinsatzes ist ьber den Umfang des Trenntellers mit dem peripheren Bereich eines zweiten
Tellereinsatzes in der oberen Abteilung verbunden, dessen zentraler Bereich mit Ableitkanдlen fьr
eine geklдrte Wasserphase in Verbindung steht, wobei vom peripheren Bereich des Feststoffraumes
Kanдle radial einwдrts zur Ableitung der Schleimstoffe fьhren.
Eine Verstopfung des Tellereinsatzes durch Schleimstoffe wird unterbunden, weil die Trennzone in
der ersten Abteilung ausserhalb des Tellereinsatzes vorgesehen ist, so dass die Schleimstoffe den
Tellereinsatz nicht durchstrцmen.
Die separate Ableitung der Schleimstoffe und die Klдrung der Wasserphase in dem Tellereinsatz der
zweiten Abteilung fьhren zu einer wesentlich geringer belasteten Wasserphase, die zu 90% in den
Prozess zurьckgefьhrt werden kann.
Durch die Trennung der drei Phasen Цl, Wasser und Schleimstoffe in ausschliesslich einem
zentrifugalen Trennvorgang wird die mechanische Beanspruchung des Produktes und die damit
verbundene Emulsionsbildung gering gehalten.
Weitere Ausgestaltungen der Zentrifuge ergeben sich aus den Unteransprьchen.
Ein Ausfьhrungsbeispiel der Zentrifuge ist in der Zeichnung dargestellt und wird im folgenden auch
zur Verdeutlichung des Verfahrens beschrieben.
Die um eine vertikale Achse 1 drehbar gelagerte Schleudertrommel 2 weist einen Einlaufraum 3 fьr
ein Цl-Wasser-Gemisch auf, der ьber Kanдle 4 mit einem Trennraum 5 in Verbindung steht.
Der Trennraum 5 der Schleudertrommel wird durch einen Trennteller 6 in eine obere Abteilung 7 und
in eine untere Abteilung 8 unterteilt.
9/1651
In der unteren Abteilung 8 ist ein erster Tellereinsatz 9 vorhanden, der von einem Verteiler 10
getragen wird und dessen Aussendurchmesser kleiner ist als die Trennzone 11, die durch den
unteren konischen Teil des Verteilers 10 bestimmt wird.
Der zentrale Bereich des ersten Tellereinsatzes 9 steht mit Ableitkanдlen 12 fьr die Цlphase in
Verbindung, die ьber eine Schдlscheibe 13 aus einer Schдlkammer 14 kontinuierlich abgezogen
wird.
An der Peripherie des ersten Tellereinsatzes 9 sind zur besseren Mitnahme der abgetrennten
Wasserphase Rippen 15 vorgesehen, die sich von der Unterseite des den ersten Tellereinsatz 9
ьberragenden Teils des Trenntellers 6 nach unten erstrecken, in Richtung auf einen Kolbenschieber
16, durch den im Trommelmantel vorgesehene Austragцffnungen 17 fьr die sich in einem
Konzentratraum 18 sammelnden Feststoffe geschlossen und fьr eine Entleerung des
Konzentratraumes geцffnet werden kцnnen.
Der Aussendurchmesser des Trenntellers 6 und des auf dem Trennteller 6 lagernden zweiten
Tellereinsatzes 19 sind wesentlich grцsser als der Aussendurchmesser des ersten Tellereinsatzes.
Hierdurch wird eine effizientere Klдrung der Wasserphase erreicht.
Der Aussendurchmesser des zweiten Tellereinsatzes 19 bzw. des Trenntellers 6 kann das 1,5-fache
bis 2-fache des Aussendurchmessers des ersten Tellereinsatzes 9 sein. Der periphere Bereich des
ersten Tellereinsatzes 9 ist ьber den Umfang des Trenntellers 6 oder ьber Steigekanдle 20, die in
unmittelbarer Nachbarschaft des Aussenumfanges des Trenntellers 6 bzw. des zweiten
Tellereinsatzes 19 liegen mit dem peripheren Bereich des zweiten Tellereinsatzes 19 in der oberen
Abteilung 7 verbunden. Der zentrale Bereich des zweiten Tellereinsatzes 19 steht mit Ableitkanдlen
21 fьr eine geklдrte Wasserphase in Verbindung. Diese geklдrte Wasserphase gelangt durch die
Kanдle 21 in eine Schдlkammer 22, aus der sie mittels einer Schдlscheibe 23 aus der
Schleudertrommel 2 abgezogen wird.
Zum kontinuierlichen Abzug der Schleimstoffe aus dem Konzentratraum 18 ist ein Ableitteller 24
vorgesehen, der mit dem Trommeldeckel 25 Kanдle 26 bildet, die seitlich durch zwischen dem
Trommeldeckel 25 und dem Ableitteller 24 vorgesehene Rippen begrenzt werden. Die dem
Konzentratraum 18 zugewandten Цffnungen 27 dieser Kanдle liegen gegenьber den
Austragцffnungen 17 der Schleudertrommel 2 nach oben und radial nach innen versetzt.
10/1651
An den Austragцffnungen der Kanдle 26 fьr die Schleimstoffe sind zur Einstellung der
Austragsmenge Dьsen 28 vorgesehen.
Der Trommeldeckel 25 ist mittels eines Verschlussringes 29 gegenьber dem Trommelunterteil 30
festgelegt.
Bezugszeichenliste
1Achse
2Schleudertrommel
3Einlaufraum
4Kanal
5Trennraum
6Trennteller
7Abteilung
8Abteilung
9Tellereinsatz
10Verteiler
11Trennzone
12Ableitkanal
13Schдlscheibe
14Schдlkammer
15Rippe
16Kolbenschieber
17Austragцffnung
18Konzentratraum
19Tellereinsatz
20Steigekanal
21Ableitkanal
22Schдlkammer
23Schдlscheibe
24Ableitteller
25Trommeldeckel
26Kanal
27Цffnung
11/1651
28Dьse
29Verschlussring
30Trommelunterteil
Claims:
1. Verfahren zur Gewinnung von Essenzцl aus Zitrusfrьchten, bei dem das von einem Extraktor
ablaufende Цl-Wasser-Gemisch, das aus ca. 86% Wasser, 10% Schalenresten, Pektinen und
Schleimstoffen, 3% Цlemulsion und aus 1% Feststoffen besteht, durch zentrifugale Behandlung in
verschiedene Phasen aufgetrennt wird, dadurch gekennzeichnet, dass ausschliesslich eine
Zentrifuge verwendet wird, mit der eine Auftrennung in drei flьssige Phasen, nдmlich Цl, Wasser
und Schleimstoffe (Anteile von Wasser, pektinen und kleineren Schalenresten) vorgenommen wird
und diese Phasen kontinuierlich aus der Schleudertrommel (2) der Zentrifuge abgezogen werden,
wдhrend die ferner anfallenden Feststoffe (Anteile von pektinen und grцsseren Schalenresten)
diskontinuierlich aus der Schleudertrommel (2) abgeschleudert werden.
2. Zentrifuge mit einer selbstentleerenden Schleudertrommel, die einen Einlauf, einen Verteiler und
einen mit einem Tellereinsatz versehenen Trennraum aufweist, zur Durchfьhrung des Verfahrens
nach Patentanspruch 1, dadurch gekennzeichnet, dass der Trennraum (5) der Schleudertrommel (2)
durch einen Trennteller (6) in eine untere Abteilung (8) und eine obere Abteilung (7) unterteilt ist,
wobei in der unteren Abteilung (8) ein erster Tellereinsatz (9) vorgesehen ist, dessen
Aussendurchmesser kleiner ist als die durch die Zufьhrkanдle des Verteilers definierte Trennzone
(11), der zentrale Bereich des ersten Tellereinsatzes (9) mit Ableitkanдlen (12) fьr die Цlphase in
Verbindung steht und der periphere Bereich des ersten Tellereinsatzes (9) ьber den Umfang des
Trenntellers (6) oder ьber in unmittelbarer Nachbarschaft des Aussenumfanges des Trenntellers (6)
und eines zweiten Tellereinsatzes (19) vorgesehene Steigekanдle (20) mit dem peripheren Bereich
des zweiten Tellereinsatzes (19) in der oberen Abteilung (7) verbunden ist, dessen zentraler Bereich
mit Ableitkanдlen (21) fьr eine geklдrte Wasserphase in Verbindung steht, wobei vom peripheren
Bereich des Feststoffraumes Kanдle (26) radial einwдrts zur Abteilung der Schleimstoffe fьhren.
3. Zentrifuge nach Anspruch 2, dadurch gekennzeichnet, dass an der Peripherie des ersten
Tellereinsatzes (9) Rippen (15) zur besseren Mitnahme der abgetrennten Wasserphase vorgesehen
sind.
12/1651
4. Zentrifuge nach Anspruch 3, dadurch gekennzeichnet, dass die Rippen (15) sich von der
Unterseite des den ersten Tellereinsatz (9) ьberragenden Teils des Trenntellers (6) erstrecken.
5. Zentrifuge nach Anspruch 2, dadurch gekennzeichnet, dass zur Erzielung einer effizienteren
Klдrung der Wasserphase der Aussendurchmesser des zweiten Tellereinsatzes (19) erheblich
grцsser ist als der Aussendurchmesser des ersten Tellereinsatzes (9).
6. Zentrifuge nach Anspruch 5, dadurch gekennzeichnet, dass der Aussendurchmesser des
Trenntellers (6) und des Tellereinsatzes (19) das 1,5- bis 2-fache des Aussendurchmessers des
ersten Tellereinsatzes (9) ist.
7. Zentrifuge nach Anspruch 2, dadurch gekennzeichnet, dass an den Austragцffnungen der
Kanдle (26) fьr die Schleimstoffe zur Einstellung der Austragsmenge Dьsen (28) vorgesehen sind.
13/1651
7. AU4611497 - 09.12.1999
ESSENTIAL OIL SOLID COMPOSITIONS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU4611497
Inventor(s):
CRAWFORD IAN (--)
Applicant(s):
GUINANE PTY LTD P (--); TEETEEOH RESEARCH GROUP PTY LT (--)
IP Class 4 Digits: C11B; A61L; A01N; C08L
IP Class:
C11B9/00; A01N65/00; A61L9/04; A01N25/18; C08L5/00; C08L95/00
Application Number:
AU19970046114 (19971024)
Priority Number: AU1996PO03780 (19961120); AU1997PO05948 (19970401); WO1997AU00716
(19971024); AU19970046114 (19971024)
Family: AU713618
14/1651
8. AU529041 - 24.03.1981
WHOLE FRUIT PEEL OIL EXTRACTOR
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU529041
Inventor(s):
HOLBROOK FRANKLIN K (--); BUSHMAN RONALD C (--)
Applicant(s):
BROWN INT CORP (--)
IP Class 4 Digits: A23N; B26D
IP Class:
A23N1/00; B26D1/00
E Class: A23N1/00B
Application Number:
US19790038668 (19790514)
Priority Number: US19790038668 (19790514)
Family: AU529041
Equivalent:
AR227149; AU5768180; BR8002964; IL59826; JP1035039; JP1551527;
JP55157689; MX149810; ZA8002080
Abstract:
PARALLEL HORIZONTAL TOOTHED ROLLS FORM BIGHTS THEREBETWEEN FOR RECEPTION OF
NON-SPHERICAL CITRUS FRUIT SUCH AS LEMONS. A BODY OF LIQUID SUBMERGES THE
TOOTHED ROLLS SO THAT PUNCTURING OF THE PEEL OF THE FRUIT TAKES PLACE BELOW
THE LIQUID LEVEL. GROUPS OF THE TOOTHED ROLLS ARE TURNED IN THE SAME DIRECTION
BUT AT PROGRESSIVELY SLOWER SPEEDS. ADJACENT TOOTHED ROLLS ARE RECIPROCATED
AXIALLY IN OPPOSITE DIRECTIONS TO CHANGE THE ORIENTATION OF THE FRUIT WITH
RESPECT TO THE TOOTHED ROLLS. THE ROLLS MAY BE PUSHED AND PULLED FROM ONE SIDE
OF THE MACHINE THROUGH A CAM OPERATED DEVICE OR THEY MAY BE PUSHED FROM BOTH
ENDS BY MECHANISM ON OPPOSITE SIDES OF THE MACHINE.Description:
15/1651
This invention relates to apparatus for extracting citrus peel oil from whole fruit. Devices of this
general type are shown in the prior patents to Bushman U.S. Pat. Nos. 3,707,176, Holbrook
3,954,032, and in Bushman and Holbrook Pat. No. 4,070,959. In each of these prior patents parallel
toothed rolls are disclosed which are horizontal and which form bights between them. The peel of
whole fruit in the bights is punctured by the toothed rolls below water level in an open top chamber.
The peel oil, which is very volatile, is trapped in the water and is later separated therefrom by
conventional means. The toothed rolls are turned under power.
When lemons or other non-spherical citrus fruit are used in such a machine, the lemons tend to turn
in the bights about their long axes and resist turning end over end about their short axes, with the
result that only a central band around each lemon is thoroughly punctured and the remainder of the
surface of the lemon is not punctured to the same degree.
In accordance with this invention, adjacent toothed rolls are not only rotated but are axially shifted to
cause the non-spherical citrus fruit to turn approximately 90 degrees and to cause each fruit to turn
end over end about its short axis. This significantly increases the yield of citrus peel oil because the
entire surface of the fruit, and not just a central band, is contacted by the needle-like points on the
toothed rolls.
In a preferred form of this invention, groups of four adjacent toothed rolls are driven at progressively
decreasing speeds. Independently, adjacent toothed rolls are reciprocated axially in opposite
directions through a cam operated device which operates as a push-pull mechanism engaging one
end of the shaft for each toothed roll. In a modified form of the invention, a cam operated mechanism
pushes each toothed roll alternately from opposite ends of the roll. In another modification, the push
movements take place on both sides of the machine by laterally movable bars operating through
thrust bearings against each of the roll shafts.
Other and more detailed objects and advantages will appear hereinafter.
In the drawings:
FIG. 1 is a side elevation partly broken away, showing a preferred embodiment of this invention.
FIG. 2 is a sectional elevation taken substantially on the lines 2--2 as shown in FIG. 1.
16/1651
FIG. 3 is a side elevation partly broken away, showing a portion of FIG. 1 on an enlarged scale.
FIG. 4 is a sectional elevation partly broken away, taken substantially on the lines 4--4 as shown in
FIG. 3.
FIG. 5 is a sectional plan view partly broken away, taken substantially on the lines 5--5 as shown in
FIG. 3.
FIG. 6 is a side elevation partly broken away, showing a portion of FIG. 1 on an enlarged scale.
FIG. 7 is an end view taken substantially on the lines 7--7 as shown in FIG. 6.
FIG. 8 is a sectional end view taken substantially on the lines 8--8 as shown in FIG. 6.
FIGS. 9, 10 and 11 are views similar to FIGS. 7 and 8, showing end views of successive segments of
the cam shaft.
FIG. 12 is a sectional detail showing the adjustable mounting of the line shafts on the frame.
FIG. 13 is a diagrammatic end elevation showing a modified form of this invention.
FIG. 14 is a diagrammatic plan view showing another modification.
FIG. 15 is a diagrammatic front view partly broken away, showing the device of FIG. 14.
Referring to the drawings, toothed rolls 10 are mounted in parallel horizontal position defining bights
11 between them. The toothed rolls 10 extend between stationary side walls 12 on a frame 13 having
a bottom wall 14. The side walls 12, bottom wall 14 and end walls (not shown) provide an open top
chamber 15 containing water. The water level is slightly above the upper portions of each of the
toothed rolls 10. Citrus fruit, such as lemons, rest in the bights 11 and contacted by the toothed rolls
below the water level.
17/1651
In accordance with the disclosure of the Bushman et al U.S. Pat. No. 4,070,959, the first roll 10a in
each group of four is driven at a relatively high speed, the next adjacent roll 10b at a slower speed,
the next adjacent roll 10c at a still slower speed, and the last roll 10d in each group driven at the
slowest speed. For example, the speed of roll 10b may be 90% of that of roll 10a, while roll 10c turns
at 90% of the speed of roll 10b, and roll 10d turns at 90% of the speed of roll 10c.
Power for turning all of the toothed rolls 10 is provided by a motor 17 which is mounted on the frame
13 and suspended below the bottom wall 14 of the chamber 15. Driving sprocket 18 fixed on the
motor shaft is connected by chain 19 to drive the sprocket 20 fixed on the transverse line shaft 21.
Another driving sprocket 22 also fixed to the motor shaft is connected by chain 23 to drive the
sprocket 24 on another line shaft 25. Idler sprockets 26 may be provided if desired. Chain and
sprocket connections drive other similar line shafts from the line shafts 21 and 25.
Each line shaft is connected by sprockets and chain to turn a group of four toothed rolls 10 in the
same direction at different speeds. The chains 29 extending between sprockets 27, 30, 32 and 28,
31, 37 drive the toothed rolls 10 at the desired relative speeds. The driven sprockets 30 and 31 are
fixed to roll shafts 16 carried in axially spaced bearings 38 on the frame 13. A second set of
sprockets 27a and 28a are fixed on each line shaft and arranged to drive a second set of sprockets
30a and 31a also fixed to the roll shafts 16. This extra set of sprockets 27a, 30a, 32a and 28a, 31a
and 37a makes it possible to vary the relative speeds between the line shafts 21 and the roll shafts
16 simply by moving the chains 29 to engage the extra sprockets instead of the first-mentioned set.
The height of the line shafts 21 may be shifted by reason of their adjustable mounting on the frame
13, as shown in FIG. 12. The line shaft bearing housings 34 are secured to the frame 13 by means of
bolts 35 extending through vertical slots 36 in the frame 13.
In accordance with this invention, means are provided for causing relative axial reciprocating
movement of adjacent toothed rolls in order to change the orientation of the lemons with respect to
the tooth rolls. As shown in the drawings, this means includes a plurality of barrel cams 40 which are
mounted on a segmental cam shaft 41 and serve to drive mechanism which causes axial
reciprocation of the toothed rolls 10. An electric motor drives the segmental cam shaft 41 through the
chain and sprocket drive 43. As best shown in FIGS. 3 and 4, each barrel cam 40 has a track 44
which receives a cam follower roller 45 mounted on the swinging end of a crank arm 46. The crank
arm 46 is fixed to the upper end of a vertical rock shaft 47 carried in axially spaced bearings 48. Also
fixed on the rock shaft 47 are a spaced pair of double arm drivers 49 and 50. Rollers 51 are mounted
18/1651
at the swinging ends of the double arm drivers and each is received within a circumferential groove
52 in an extension piece 53 fixed to one end of a roll shaft 16.
From this description it will be understood that the turning of the cam shaft 41 and barrel cams 40
causes the crank arms 46 to cause oscillating movement of the rock shafts 47 as the follower rollers
45 move back and forth in the cam track 44. These oscillating movements of the rock shafts 47
cause the spaced double arm drivers 49 and 50 to reciprocate adjacent roll shafts 16. The side
guides 33 prevent lemons from contacting the side walls 12.
As shown in FIG. 2, axial movement of the toothed roll 10 causes the sprockets 30 and 31 to move
between two positions, each of which is misaligned to a small degree with respect to the driving
sprockets 27 and 28 on the line shaft 21. The misalignment is so small, however, that no difficulty is
encountered when the sprockets 30 and 31 move from the full line position to the phantom line
position.
As best shown in FIG. 6, the cam shaft 41 is made up of several axially aligned segments put
together end to end. Thus, cam shaft segment 41a is connected by coupling 54 and key 55 to the
adjacent cam shaft segment 41b. The cam shaft segments are all duplicates and each has two
adjacent barrel cams 40 mounted in the same relative angular position and two additional barrel
cams 40a fixed at a 90 degree position. The angular staggering of the pairs of barrel cams and the
angular staggering of the cam shaft segments 41 serve to equalize the load on the motor 42. When
five cam shaft segments are employed, each segment is spaced from its neighbor by one-fifth of a
revolution, namely, 72 degrees. This is graphically illustrated in FIGS. 7-11. Thus, the cam shaft
segments are all duplicates and the barrel cams are all duplicates, but the cam shaft segments are
angularly staggered and the pairs of barrel cams 40 are angularly staggered. The result is that the
load on the driving motor 42 is the same for all anxular positions of the toothed rolls 10. Accordingly,
the motor 42 may be started and stopped in any position of the toothed rolls.
It should be noted that rotation of the toothed rolls 10 is powered and controlled by the motor 17
whereas axial reciprocation of the toothed rolls 10 is powered and controlled by the motor 42. The
speeds of the motors 17 and 42 may be independently adjusted by conventional means.
Apparatus for feeding whole citrus fruit to the toothed rolls is preferably of the type disclosed in the
copending application of McKinney Ser. No. 000,029 filed Jan. 2, 1979.
19/1651
In the modified form of the invention shown in FIG. 13, the toothed rolls 60 and roll shafts 61 are
similar to those previously described. However, cam mechanism is mounted on both sides of the
machine so that each roll shaft is pushed axially in one direction and then pushed axially in the other
direction. This is accomplished by means of pairs of eccentrics 63 and 64 which are fixed on parallel
horizontal shafts 65 and 66 mounted on opposite sides of the machine. A motor 67 drives through
chains and sprockets to turn the eccentric shafts 65 and 66 in timed relationship. Apparatus for
rotating the toothed rolls 60 is similar to that previously described but is omitted for clarity of
illustration.
In the second modified form of the invention shown in FIGS. 14 and 15, the toothed rolls 68 are
similar to those described above, but the mechanism for reciprocating them axially is different. A
thrust bearing 69 is provided at each end of each roll shaft 70. Laterally movalbe parallel horizontal
bars 71 and 72 support the thrust bearings 69 for alternate toothed rolls 68. A similar mounting is
provided for the other toothed rolls 73, the laterally movable bars 74 and 75 carrying the thrust
bearings 76 for the toothed rolls 73.
Mechanism is provided for reciprocating the parallel bars 71 and 72 laterally to push alternate
toothed rolls 68 in the same axial direction. The same mechanism acts to shift the parallel bars 74
and 75 to cause axial movement of the other toothed rolls 73. The mechanism comprises a crank 77
having an eccentric driving pin 78 engaging transverse shifter members 79. The members 79 are
pivotally connected at opposite ends to crank arms 80 fixed on vertical rock shafts 81. An upper
crank arm 82 on the rock shaft 81 is pivotally connected to the upper bar 71. Similarly, a crank arm
83 on each rock shaft 81 is pivotally connected to the lower bar 74. Duplicate shift mechanisms are
provided along the length of the device.
From this description it will be understood that the toothed rolls 68 and 73 are alternately pushed in
opposite directions by means of the upper bars 71, 72 and by means of the lower bars 74, 75.
Apparatus for rotating the toothed rolls 68 and 73 is similar to that previously described in connection
with the preferred embodiment, but such roll-rotating apparatus is omitted from the drawings in FIGS.
14 and 15 for clarity of illustration.
Having fully described our invention, it is to be understood that we are not to be limited to the details
herein set forth but that our invention is of the full scope of the appended claims.
Claims:
We claim:
20/1651
1. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
fruit, means for turning said rolls in the same direction, and means for causing relative axial
reciprocating movement of said rolls to change the orientation of the fruit with respect to the rolls.
2. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
fruit, means for turning said rolls in the same direction, and means for axially reciprocating at least
one of said rolls to change the orientation of the fruit with respect to the rolls.
3. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
fruit, means for turning said rolls in the same direction, and means for axially reciprocating both of
said rolls in opposite directions to change the orientation of the fruit with respect to the rolls.
4. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a series of parallel horizontal toothed rolls forming a plurality of bights therebetween
for reception of fruit, means for turning said rolls in the same direction but at progressively slower
speeds, and means for causing relative axial reciprocating movement of said rolls to change the
orientation of the fruit with respect to the rolls.
5. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a series of parallel horizontal toothed rolls forming a plurality of bights therebetween
for reception of fruit, means for turning said rolls in the same direction but at progressively slower
speeds, and means for axially reciprocating at least one of said rolls to change the orientation of the
fruit with respect to the rolls.
6. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a series of parallel horizontal toothed rolls forming a plurality of bights therebetween
for reception of fruit, means for turning said rolls in the same direction but at progressively slower
speeds, and means for axially reciprocating both of said rolls in opposite directions to change the
orientation of the fruit with respect to the rolls.
21/1651
7. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a plurality of series of parallel horizontal toothed rolls forming a plurality of bights
therebetween for reception of fruit, means for turning said rolls in each series in the same direction
but at progressively slower speeds, and means for axially reciprocating adjacent rolls in each series
in opposite directions to change the orientation of the fruit with respect to the rolls.
8. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
fruit, a body of liquid partially submerging said rolls so that puncturing of the peel of the fruit by said
toothed rolls takes place below the level of the liquid, means for turning said rolls in the same
direction but at different speeds, and means for causing relative axial reciprocating movement of
said rolls to change the orientation of the fruit with respect to the rolls.
9. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
fruit, chain and sprocket means for turning said rolls in the same direction but at different speeds,
and cam-controlled means for causing relative axial reciprocating movement of said rolls to change
the orientation of the fruit with respect to the rolls.
10. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
fruit, a body of liquid partially submerging said rolls so that puncturing of the peel of the fruit by said
toothed rolls takes place below the level of the liquid, means for turning said rolls in the same
direction, a power driven cam, and means including a cam follower for causing relative axial
reciprocating movement of said rolls to change the orientation of the fruit with respect to the rolls.
11. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a plurality of series of parallel horizontal toothed rolls forming a plurality of bights
therebetween for reception of fruit, means for turning said rolls in each series in the same direction
but at progressively slower speeds, a power driven cam, and means including a cam follower for
axially reciprocating adjacent rolls in each series in opposite directions to change the orientation of
the fruit with respect to the rolls.
12. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
22/1651
fruit, means for turning said rolls in the same direction, cam-controlled means for causing relative
axial reciprocating movement of said rolls to change the orientation of the fruit with respect to the
rolls, said means including a power driven barrel cam having a circumferential track, a rock shaft
having a crank arm with a cam follower engaging said track, and means on said rock shaft for
reciprocating said toothed rolls axially in opposite directions.
13. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a plurality of parallel horizontal toothed rolls forming bights therebetween for
reception of fruit, power means for turning said rolls in the same direction, means for causing relative
axial shifting movement of said rolls to change the orientation of the fruit with respect to the rolls, said
means including a horizontal segmental cam shaft extending at right angles with respect to said rolls,
each cam shaft segment having two spaced pairs of barrel cams fixed thereto, the barrel cams all
being duplicates, one pair being mounted at 90 degree angular spacing with respect to the other
pair, coupling means connecting the cam shaft segments in axial alignment and in angularly spaced
relationship, and means including a follower engaging each barrel cam for reciprocating two
adjacent toothed rolls in opposite directions.
14. Apparatus for extracting peel oil from whole non-spherical citrus fruitsuch as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
fruit, each toothed roll including a roll shaft, means for turning said roll shafts in the same direction,
cam-controlled means for causing relative axial reciprocating movement of said rolls to change the
orientation of the fruit with respect to the rolls, said means including parallel rotary drive shafts at
right angles to said toothed rolls, and a plurality of spaced eccentrics fixed to each of said drive
shafts, each eccentric being positioned to engage one end of each roll shaft to push that roll shaft
axially in one direction, and power means for rotating said drive shafts in timed relationship.
15. Apparatus for extracting peel oil from whole non-spherical citrus fruit such as lemons, comprising,
in combination: a pair of parallel horizontal toothed rolls forming a bight therebetween for reception of
fruit, each toothed roll including a roll shaft, means for turning said roll shafts in the same direction,
cam-controlled means for causing relative axial reciprocating movement of said rolls to change the
orientation of the fruit with respect to the rolls, said means comprising a first pair of parallel horizontal
bars, means whereby each bar operatively engages one end of alternate roll shafts, a second pair of
parallel horizontal bars each having means for engaging one end of the remaining roll shafts, and
power means for laterally reciprocating both pairs of parallel bars in timed relationship.
23/1651
9. AU5336390 - 20.09.1990
MEMBRANE ENCAPSULATED ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU5336390
Inventor(s):
WANG YING (CA); YANG QILIAN (CA)
Applicant(s):
INT APPLIED SCIENCES INC (US)
IP Class 4 Digits: A61K
IP Class:
A61K7/46
E Class: A61K8/92C; A61Q13/00; A61K8/11C; A61K8/891
Application Number:
WO1990CA00085 (19900314)
Priority Number: CN19890101383 (19890315)
Family: WO9010436
Equivalent:
CN1045599
Cited Document(s):
US4725575; US4089800; EP0304416
Abstract:
A PERFUMING AGENT WHICH CONTAINS ONE OR MORE OF AN ESSENTIAL OIL CAPSULE
HAVING A CORE OF ESSENTIAL OIL ENCAPSULATED WITHIN A MEMBRANE, THE ESSENTIAL OIL
CAPSULE BEING DISPERSED IN AN AQUEOUS SOLUTION CONTAINING A SURFACTANT. A
METHOD OF PREPARING THE PERFUMING AGENT AND THE USE OF THE PERFUMING AGENT
TO SCENT A SUBSTRATE IS ALSO PROVIDED.Description:
24/1651
TITLE:- NEHBRANE ENCAPSULZkTED ESSENTIAL QIL
FIELD OF THE INVENTION
This invention generally relates to the fields of perfuming and membrane technology.
BACKGROUND OF THE INVENTION
Generally, essential oils are volatile materials produced from odorous plant material by water or
steam distillation or by expressing. Examples of natural essential oils used in perfume include
ambergris, benzoin, cast oreum, civet, clove leaf oil, galbanum, jasmine absolute, labdanum, mate,
melilot, mimosa, musk tonquin, myrrh, oakmoss or mousse de chine, olibanum, opopanax, orris,
patchouli, rose, rosemary oil, sandalwood oil, vetivert oil and violet leaves absolute Many essential
oils are also made synthetically.
Perfuming agents applied to substrates such as air fresheners contain an essential oil and ethanol
solvent.
Ethanol is used since the essential oil generally is not soluble in water. A disadvantage with
perfuming agents employing ethanol is that both the ethanol and any alcohol and fusel oil in the
ethanol give off an odour which may affect the quality of the fragrance. Furthermore, ethanol may
irritate skin which limits its usefulness in a perfuming agent.
Traditional methods of extending the release time of a small amount of essential oil in a perfuming
agent include the addition of a carrier liquid such as polyethenol resiap oleic. acid an glycerol to the
perfuming agent. These techniques, however, do not give the desired amount of control over the
release of the fragrance.
A more recent method includes the addition of a surfactant to the perfuming agent to dissolve the
essential oil on the surfactant to form minute capsules having a diameter of less than 0.05 micron.
The capsules separate out of the ethanol solution, thereby reducing the quantity present using thismethod which gives rise to the problem of an overly-fast release.rate of the essential oil with a
resultant undesirab-le scent
It is desirable, therefore, to increase the release time of perfuming agents and to produce perfuming
agents without the use of ethanol to both increase the quality of the perfuming agent and any
substrate treated with this agent, preferably at a reasonable manufacturing cost.
SUMMARY OF THE INVENTION
25/1651
The present invention provides a perfuming agent comprising one or more of an essential oil
capsule having a core of essential oil encapsulated within a membrane, the essential oil capsule
being dispersed in an aqueous solution containing a surfactant.
The invention also provides; a- method of preparing a perfuming agent having one or- more of an
essential oil capsule dispersed in an aqueous solution containing a surfactant, the method
comprising encapsulating an essential oil within a membrane, the encapsulating being effected by
forming the membrane by contacting the essential oil with an aqueous solution containing a
membrane forming material, a surfactant and a solvent capable of dissolving one or both of the
essential oil or membrane forming material to form an essential oil droplet; crosslinking the
membrane forming material to produce a membrane about the essential oil droplet by subjecting the
essential oil droplet to a cross-linking agent; and allowing the solvent to evaporate to form an
essential oilcapsule.
The invention further relates to the use of the perfuming agent of the invention to scent a variety of
substrates; for example, cloth, wallpaper, silk flowers, dried natural flowers, shirts and air fresheners.
BRIEF DESCRIPTION OF THE DRAWINGS
The invention will now be described. by reference to the appended drawings in which:
Figure 1 diagrammatically shows the components of the perfuming agent of the invention during
formation; and,
Figure 2 diagrammatically shows a formed essential oil capsule of the invention.
DETAILED DESCRIPTION OF THE INVENTION
As mentioned hereinbefore, the present invention provides a perfuming agent comprising one or
more of an essential oil capsule having a core of essential oil encapsulated within a membrane, the
essential oil capsule being dispersed in an aqueous solution containing a surfactant. Essential oils
which may be used in the perfuming agent are rose oil, lilac oil or any other variety of non-water
soluble essential oils. The essential oils obtained from natural products or synthetic essential oil may
be used in the perfuming agent of the invention.
The surfactant which may be used in the perfuming agent of the invention is typically odourless.
Examples of suitable surfactants include dodecyl sodium sulfate (DSS), sodium alkylsulfonate,
polythene oxide, polyethenol, sodium oleate and sodium napthylate.
26/1651
The essential oil capsules have a low surface tension, generally about 40 dyne per centimetre2 so
that they have generally good absorbability.
The essential oil capsules contain molecular interstices on their- surfaces through which the
essential.
oil can permeata Preferably, the size of the molecular interstices may be selected so as to give a
relatively even rate of fragrance release.
The diameter of the essential oil capsules is typically in the range of .05 to 50 microns and
correspondingly, the surface area of the essential oil capsules is large. Thus, the capsules contain a
relatively large amount of essential oil so that a substrate on which such capsules is deposited will
be able to release fragrance over a longer period of time than a substrate treated directly with an
essential oil in alcohol. Also, when alcohol is not used as the solvent, there is no negative effect from
the smell of the alcohol on the scent of the essential oil.
The perfuming agent of the present invention is prepared by encapsulating the essential oil with a
membrane. The encapsulation is effected by forming the membrane by contacting the essential oil
with an aqueous solution containing a membrane-forming material, a surfactant and a solvent
capable of dissolving one or bothof the essential oil or membrane-forming material to form an
essential oil droplet. The membrane forming material is crosslinked to produce a membrane about
the essential oil droplet by subjecting the essential oil droplet to a cross- linking agent. The solvent is
then.allowd-to evaporate.to form an essential oil capsule
The essential oils and surfactants which may be used in the method of the invention have been
described above.
Suitable membrane-forming material which may be used in the method of the invention include
organosilane or organosilicone rubber, in particular, methyl siloxane, ethyl siloxane or ethenyl
siloxane. Typically, the concentration of the membrane forming material is from about 5 to 35% by
weight.
Suitable crosslinking agents which may be used in the process of the invention include phosphoric
acid, ethyl silicic acid, organic zinc. Typically-the concentration of crosslinking agents is froiabout os% by-- weight
27/1651
Suitable solvents which may be used in the process of the invention include petroleum ether and
benzene typically in concentrations of from about 30 to 85% by weight.
A detailed description of the formation of a preferred perfuming agent of the invention will now be
discussed.
The surfactant is first dissolved in water to prepare a water/surfactant solution. A second solution is
prepared by combining the membrane forming material, the crosslinking agent, the-solvent and the
essential oil
The essential oil may be rose oil or any other variety of non-water soluble essential oil in a
concentration of from 5 to 35% by volume. The water/surfactant solution may be stirred in a mixer at
approximately 100 revolutions per minute for from about 1 to 120 minutes. The second solution is
added to the water/surfactant solution slowly while stirring and stirring is continued for 1 to 20 hours
after all of the second liquid has been added. After a period between about 1 to 20 hours has
elapsed, the resulting mixture may be passed through a filter in a separating funnel to separate out
the water and surfactant.
The filter should stop the passage of particles greater than approximately 20 microns. In this manner,
a concentrated solution of perfuming agent is formed. During- this process, the weight ratio of the
water/surfactant and second liquid is controlled from 100:10 to 100:200.
Microscopic examination of membrane encapsulated essential oil droplets produced using the
above method shows them to be approximately 5 to 25 microns in size and having a membrane
thickness of approximately 2 - 3 microns.
The content of essential oil inside the capsules is from 70 - 90% of the total volume of the capsules.
The perfuming agent of the present invention may be used to spray or coat for example, cloth,
wallpaper, paper, silk flowers, dried natural flowers and shirts. Various- sizes of molecular interstices
on the surface polymer membrane may be used to give fragrance release times from.
5 to 100 days
In accordance with the objects and principles of the invention, and the accompanying drawing, a
perfuming agent generally designated 2 is provided. In Figure 1, an essential oil droplet 11 is shown
28/1651
surrounded by a solvent 13 containing membrane forming material 12. The solvent 13, membrane
forming material 12 and essential oil droplet 11 are suspended within a water/surfactant solution 15.
Reference 14 indicates a surfactant layer.
Once the solvent evaporates from the system shown in
Figure 1, the water and essential oil, which are immiscible, are separated by a layer of membrane 16.
The membrane generally has the shape of a hollow space with the essential oil droplet 11 contained
therein. Outside of the membrane 16 is the water and surfactant solution 15. The essential oil
capsules. dispersed in the water and surfactant solution is referred to herein as a perfuming agent.
The present invention may be further illustrated .by reference to the following examples.
Example A
A perfuming agent with a lilac scent was prepared using the solutions described below
A water/surfactant solution was made by dissolving 0.25 g of dodecyl sodium sulfate in 99.75 g-of
water.
A second solution was prepared by combining 10 g dimethyl siloxane, 10 g ethyl silicic acid, 0.5 g
zinc dodecylate, 10 g lilac essential oil and 28.5 g petroleum ether. The second liquid was stirred for
twelve hours at a temperature of 600C and a stirring speed of 40 rpm.
The water surfactant solution was first stirred in a mixer at approximately 100 revolutions per minute
from 1 to 120 minutes. The second solution was added to the water/surfactant solution slowly while
stirring. The mixture was stirred for 1 to 20 hours after which it was passed through a filter.
(approximateiy 2Q > } in a separating funnel ta-separate out the water and surfactant
Example B
A perfuming agent with an otto of rose style essential oil was prepared using the solutions described
below:
A water/surfactant solution was prepared by dissolving 1 g sodium alkyl sulfonate in 99 g of water.
A second solution was prepared by combining 1.0 g of essential oil, 10 g diethenyl siloxaner 10 g
of 15% phosphoric acid solution and 25 g of benzene. The second solution was stirred for 16 hours
at 650C and a stirring speed of 60 rpm.
29/1651
The method of preparing the perfuming agent was as described in Example A.
Example C
A perfuming agent with jasmin essential oil was prepared using the solutions described below:
A water/surfactant solution was prepared by dissolving 0.5 g polyethenyl oxide in 99.5 g water.
A second solution was prepared by combining 5 g of jasmin essential oil, 3 g of diethenol
metholcyloxane, 5 g of phosphoric acid solution and 17 g of benzene The.
second solution was stirred for 10 hours at a temperature of 650C and a stirring speed of 40 rpm.
The method of preparing the perfuming agent was as described in Example A.
It is to be understood that variations to the above specific examples may be apparent to one skilled
in the relevant art without departing from the spirit and scope of the present invention. Claims:
We Claim:
1. A perfuming agent comprising one or more of an essential oil capsule having a core of essential oil
encapsulated within a membrane, the essential oil capsule being dispersed in an aqueous solution
containing a surfactant.
2. The perfuming agent as claimed in claim 1, wherein the essential oil capsule has a diameter of
from about 0.05 to 50 microns.
3. The perfuming agent as claimed in claim 1, wherein the membrane has a thickness of between
about 2 to 3 g and consists of crosslinked organosilane or organosilane rubber.
4. The perfuming agent as claimed in claim I, wherein the volume of essential oil in the essential oil
capsule is from 70 to 90 % of the total volume of the essential oil capsule.
30/1651
5. A method of preparing a perfuming agent having one or more of an essential oil capsule
dispersed in an aqueous solution containing a surfactant, which comprises encapsulating an
essential oil within a membrane, the encapsulating being effected by forming the membrane by
contacting the essential oil with an aqueous solution containing a membrane forming material, a surfactant and a.
solvent capable of dissolving. onQJor.-h3tS o-the.essential oil or membrane forming material to form
an essential oil droplet; crosslinking the membrane forming material to produce a membrane about
the essential oil droplet by subjecting the essential oil droplet to a cross-linking agent; and allowing
the solvent to evaporate to form an essential oil capsule.
6. The method as claimed in claim 4 wherein the essential oil is an non-water soluble essential oil.
7. The method as claimed in claim 6, wherein the essential oil is rose oil, lilac oil or jasmin oil.
8. The method as claimed in claim 5, wherein the surfactant is selected from the group consisting of
dodecyl sodium sulfate (DSS), sodium alkylsulfonate, polythene oxide, polyethenol, sodium oleate
and sodium napthylate.
9. The method as claimed in claim 5, wherein the membrane forming material is selected from the
group consisting of organosilane and organosilicone rubber.
10. The. method as claimed in claim 8, whereinthe membrane forming material is selected from the
group consisting of organosilane and organosilicone rubber.
11. The method as claimed in claim 9, wherein the membrane material is selected from the group
consisting of methyl silane, ethyl siloxane or ethenyl siloxane.
12. The method as claimed in claim 9 or 10, wherein the concentration of the membrane forming
material is between about 5 to 35%.
13. The method as claimed in claim 9, 10 or 11, wherein the crosslinking agent is phosphoric acid,
ethyl, silica acid or organic zinc 14. The use of a perfuming agent as claimed in claims 1 to 4, to
scent a substrate.
31/1651
15. The use as claimed in claims 14, wherein the substrate is cloth, wallpaper, silk flowers, dried
natural flowers, shirts or air fresheners.
32/1651
10. AU582047 - 04.11.1987
COMPOSITION AND METHOD TO INHIBIT THE GROWTH OF ORGANISMS BY THE USE OF BISBIGUANIDO HEXANES AND ESSENTIAL OIL MIXTURE COMBINATIONS.
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU582047
Inventor(s):
PIANOTTI ROLAND S (--)
Applicant(s):
WARNER LAMBERT CO (US)
IP Class 4 Digits: A61K
IP Class:
A61K7/22
E Class: A61K8/37; A61Q11/00; A61K8/49H2; A61K8/34; A61K8/34F; A61K8/43
Application Number:
EP19870810268 (19870428)
Priority Number: US19860859113 (19860502)
Family: AU582047
Equivalent:
AU7187887; DK223387; FI871918; JP62289511; ZA8702857
Cited Document(s):
GB1365030; DE1964196; FR2440189
Abstract:
NOVEL ANTIMICROBIAL COMPOSITIONS HAVING A SYNERGISTIC COMBINATION OF A BISBIGUANIDO HEXANE COMPOUND AND A MIXTURE OF AT LEAST TWO ESSENTIAL OILS AND A
METHOD FOR TREATING TEETH TO INHIBIT OR PREVENT DENTAL CARIES AND
PLAQUE.Description:
COMPOSITION AND METHOD TO INHIBIT THE GROWTH OF ORGANISMS BY THE USE OF BISBIGUANIDO HEXANES AND ESSENTIAL OIL MIXTURE COMBINATIONS
33/1651
This invention relates to a novel synergistic antibacterial oral composition to promote oral hygiene
which contains in combination a bis-biguanido hexane compound and a mixture of at least two
essential oils. Such compositions are useful against the bacteria most commonly associated with the
formation of dental plaque and caries such as Streptococcus sanguis and Streptococcus mutans
respectively.
Bis-biguanido hexane compounds are well known in the art. These materials possess antibacterial
activity and have been used in oral compositions to counter dental plaque and caries formation by
bacteria in the oral cavity. The use of these agents at therapeutic levels as the free base or as water
soluble salts has resulted in undesirable cosmetic effects. These effects are the brown staining of
dental enamel and bitter taste associated with its use. Much effort has been devoted towards
overcoming these undersirable effects. Additionally, us of these agents has been reported to cause
disquamation of oral epithelial cells and taste aberrations.
U.S. Patent 4,256,731 to Curtis, et al. discloses oral compositions useful for controlling dental plaque
and gingivitis and for preventing caries comprising a cationic antimicrobial agent such as bisbiguanide and a combination of antistain agents which reduce the staining effect of the cationic
antimicrobial.
U.S. Patent 4,241,049 to Colodney, et al. discloses a dentifrice containing phosphate ion, flavoring oil,
1,6-di-(p-chlorophenyl biguanidohexane) and a water soluble alkaline earth metal salt of a strong
acid to stabilize the dentifrice against separation. Calcium and magnesium chlorides are typical
stabilizers.
U.S. Patent 4,118,474 to Gaffar, et al. discloses combining the antistain additive phosphonoacetic
acid or salts thereof with antibacterial antiplaque agents including bis-biguanido hexanes, such as
chlorhexidine and alexidine in an antibacterial oral composition effective to promote oral hygiene.
U.S. Patent 4,080,441 to Gaffar, et al. discloses an antibacterial oral composition effective to promote
oral hygiene containing an antibacterial antiplaque agent and an additive which reduces staining of
dental surfaces without substantially diminishing the antibacterial and antiplaque activity of the agent.
Bis-biguanido hexanes, such as chlorhexidine and alexidine, and quaternary ammonium salts, such
as benzethonium chloride and cetyl pyridinium chloride, are typical examples of antibacterial agents.
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The antistain additive is a bis-(o-carboxyphenyl)ester of a C 2_8 aliphatic dicarboxylic acid such as
bis(o-carboxyphenyl) succinate.
U.S. Patent 3,937,805 to Harrison discloses the preparation of a dentifrice composition containing an
insolubilized salt of 1,6-di-(p-chlorophenyl biguanido) hexane antimicrobial agent such as the
disarcosinate monomeric salt or monofluorophosphate polymeric salt. The insolubilized salt may be
pre-formed or formed in situ in the dentifrice composition. The insolubilized material is antimicrobially
effective and provides desirable cosmetic effect in that it does not stain teeth upon repeated use and
does not impart an undesirable taste to the oral composition.
U.S. Patent 3,925,543 to Donohue discloses oral products containing bis-biguanido hexane
antibacterial agents which are effective in preventing the accumulation of bacterial plaque and which
do not stain teeth. Incorporation of a suitable reducing agent, such as ascorbic acid, was found to
prevent dental staining while maintaining the activity of the bis-biguanido hexanes in oral products.
The instant invention concerns novel antimicrobial compositions having a synergistic combination of
a bis-biguanido hexane compound and a mixture of at least two essential oils selected from the
group consisting of thymol, eucalyptol, methyl salicylate and menthol. These antimicrobial
compositions reduce dental plaque and caries when incorporated in oral compositions.
As a result of the synergistic combination, the amount of bis-biguanido hexane compound needed to
effectively inhibit the growth of organisms such as S. mutans and S. sanguis has been reduced such
that the dental staining and bitter taste associated with the use of bis-biguanido hexane compounds
has been greatly reduced or eliminated.
The present invention relates to compositions of matter and a method which effectively inhibit or
prevent the formation of dental plaque and dental caries. More specifically, it relates to a
combination of a bis-biguanido hexane compound and a mixture of at least two essential oils
selected from the group consisting of thymol, encalyptol, methyl salicylate and menthol.
A method is provided for treating teeth to inhibit or prevent dental caries and plaque wherein the
teeth are contacted with an effective amount of synergistic combination of bis-biguanido hexane and
a mixture of at least two essential oils selected from the group consisting of thymol, eucalyptol,
methyl salicylate and menthol in an amount sufficient to inhibit growth of S. mutans and S. sanguis
present in the oral cavity in general or on teeth in particular.
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In carrying out the method of the invention, the combination of a bis-biguanido hexane compound
and a mixture of at least two essential oils selected from the group consisting of thymol, eucalyptol,
methyl salicylate and menthol will usually be employed in conjunction with a non-toxic carrier such as
a mouthwash, or a dentifrice such as a powder, paste, gel, liquid or the like.
Any nontoxic, antibacterial, water-soluble salt of the bis-biguanido hexanes may be employed in the
instant invention. The preferred bis-biguanido hexanes are 1, 6-di(p-chlorophenyldiguanido)hexane
and 1, 6-bis (2-ethyl-hexyl biguanido)hexane. The preferred acid addition salts are the digluconate,
diacetate, dihydrogen halides such as fluoride, chloride and bromide, dimonofluorophosphate, and
the like.
In the present invention, the bis-biguanido hexane is present in amounts from about 0.01% to about
10% by weight of the free base form of the compound. Preferably the bis-biguanido hexane is
present from about 0.05% to about 1% by weight of the free base form and most preferably from
about 0.1% to about 0.5%. The preferred bis-biguanido hexane is 1, 6-di(p-chlorophenyl
biguanido)hexane which is also known as chlorhexidine. The preferred salt is the digluconate.
The essential oils of the present invention are selected from the group consisting of thymol,
eucalyptol, methyl salicylate and menthol. At least two essential oils must be present. The essential
oils are collectively present in an amount from about 0.05% to about 10%, preferably from about
0.1% to about 5% and most preferably about 0.2% to about 4% by weight of the composition.
Individually, the essential oils may be present from about 0.025% to about 5% by weight of the
composition and preferably from about 0.05% to about 2%. The weight ratio of the least concentrated
essential oil to each of the other essential oils is from about 1:5 to about 1:1 and preferably from
about 1:3 to about 1:1.
The essence of the present invention is the synergistic effect of inhibiting the growth of bacteria such
as S. mutans and S. sanguis which is achieved when a bis-biguanide hexane and a mixture of at
least two essential oils selected from the group consisting of thymol, eucalyptol, methyl salicylate and
menthol are employed in combination in effective concentrations in the oral cavity. Smaller quantities
of each of these materials are required to obtain effective growth inhibition of bacteria such as S.
mutans and S. sanguis than if each were employed alone. Sufficient quantities of each material are
added to the composition of matter of interest to provide effective amounts of the combination of a
bis-biguanido hexane and a mixture of essential oils in the oral cavity.Since lower quantities of bis-
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biguanido hexane material are used in the synergistic combinations of the present invention, the
amount of staining associated with the use of bis-biguanido hexane compounds will be reduced or
eliminated.
In one form of the invention, the oral preparation may be a liquid such as a mouthwash or rinse. In
such a preparation the vehicle is typically a water-alcohol mixture. Generally the ratio of water to
alcohol is in the range of from about 1:1 to about 20:1, preferably about 3:1 to about 20:1 and most
preferably about 3:1 to about 10:1 by weight. The total amount of water-alcohol mixture in a
mouthwash preparation is typically in the range from about 70% to about 99.9% by weight of the
composition. The pH value of such mouthwash preparations is generally from about 4.0 to about 7.0
and preferably from about 5 to about 6.5. A pH below 4 would be irritating to the oral cavity. A pH
greater than 7 would result in an unpleasant mouth feel.
Oral liquid preparations may also contain surface active agents in amounts up to about 5% and
fluorine-providing compounds in amounts up to about 2% by weight of the preparation.
Surface active agents are organic materials which afford complete dispersion of the preparation
throughout the oral cavity. The organic surface active material may be anionic, non-ionic, ampholytic,
or cationic. Suitable anionic surfactants are water-soluble salts of higher fatty acid monoglyceride
monosulfates, such as the sodium salt of the monosulfated monoglyceride of hydrogenated coconut
oil fatty acids; higher alkyl sulfates, such as sodium lauryl sulfate; alkyl aryl sulfonates, such as
sodium dodecyl benzene sulfonate; higher alkyl sulfonacetates; higher fatty acid esters of 1,2dihydroxy propane sulfonates; and substantially saturated higher aliphatic acyl amides of lower
aliphatic amino carboxylic acids such as those having 12 to 16 carbons at the fatty acid, alkyl or acyl
radicals.
Non-ionic surface active agents include condensates of sorbitan mono-oleate with from 20 to 60
moles of ethylene oxide (e.g., "Tweens" a trademark of ICI United States, Inc.), condensates of
ethylene oxide with propylene oxide, condensates of propylene glycol ( "Pluronics" a trademark of
BASF-Wyandotte Corp.), and amphoteric agents such as quaternized imidazole derivatives.
Other suitable non-ionic surfactants are the condensation products of an alpha-olefin oxide
containing 10 to 20 carbon atoms, a polyhydric alcohol containing 2 to 10 carbons and 2 to 6
hydroxyl groups and either ethylene oxide or a heteric mixture of ethylene oxide and propylene oxide.
The resultant surfactants are heteric polymers having a molecular weight in the range of 400 to about
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1600 and containing 40% to 80% by weight of ethylene oxide, with a alpha-olefin oxide to polyhydric
alcohol mole ratio in the range of about 1:1 to 1:3.
Cationic surface active agents are molecules that carry a positive charge such as cetylpyridinium
chloride.
A fluorine providing compound may be present in the oral preparations of this invention. These
compounds may be slightly water soluble or may be fully water soluble and are characterized by
their ability to release fluroide ions or fluoride containing ions in water. Typical fluorine providing
compounds are inorganic fluoride salts such as soluble alkali metal, alkaline earth metal, and heavy
metal salts, for example, sodium fluoride, potassium fluoride, ammonium fluoride, cuprous fluoride,
zinc fluoride, stannic fluoride, stannous fluoride, barium fluoride, sodium fluorosilicate, ammonium
fluorosilicate, sodium fluorozirconate, sodium monofluorophosphate, aluminum mono-and
difluorophosphate and fluorinated sodium calcium pyrophosphate.
Alkali metal, tin fluoride and monofluorophosphates such as sodium and stannous fluoride, sodium
monofluorophosphate and mixtures thereof are preferred.
The oral preparations of this invention may be substantially solid or pasty in character such as dental
cream, toothpaste or a toothpowder. Solid or pasty oral preparations contain polishing materials.
Typical polishing materials are abrasive particulate materials having particle sizes of up to about 20
microns. Nonlimiting illustrative examples include: water-insoluble sodium metaphosphate,
potassium metaphosphate, tricalcium phosphate, dihydrated calcium phosphate, anhydrous
dicalcium phosphate, dicalcium phosphate, calcium pyrophosphate, magnesium orthophosphate,
trimagnesium phosphate, calcium carbonate, alumina, aluminum silicate, zirconium silicates, silica,
bentonite, and mixtures thereof. Polishing materials are generally present in an amount from about
20% to about 99% by weight of the oral preparation. Preferably, it is present in amounts from about
20% to about 75% in toothpaste, and from about 70% to about 99% in toothpowder.
In clear gels, a polishing agent of colloidal silica and alkali metal aluminosilicate complexes are
preferred since they have refractive indicies close to the refractive indicies of gelling agent liquid
systems commonly used in dentifrices.
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In a oral liquid preparation such as a mouthwash, the fluorine providing compound is generally
present in an amount sufficient to release up to about 0.15%, preferably about 0.001% to about 0.1%
and most preferably from about 0.001% to about 0.05% fluoride by weight of the preparation.
The oral preparations of the present invention may additionally contain sweetener, flavorants and
colorants.
In the instance where auxiliary sweeteners are utilized, the present invention contemplates the
inclusion of those sweeteners well known in the art, including both natural and artificial sweeteners.
Thus, additional sweeteners may be chosen from the following non-limiting list:
A. Water-soluble sweetening agents such as monosaccharides, disaccharides and
polysaccharides such as xylose, ribose, glucose, mannose, galactose, fructose, dextrose, sucrose,
maltose, partially hydrolyzed starch, or corn syrup solids and sugar alcohols such as sorbitol, xylitol,
mannitol and mixtures thereof.
B. Water-soluble artificial sweeteners such as the soluble saccharin salts, i.e., sodium, or calcium
saccharin salts, cyclamate salts, acesulfame-K and the like, and the free acid form of saccharin.
C.Dipeptide based sweeteners such as L-phenylalanine methyl ester and materials described in
U.S Patent No. 3,492,131 and the like.
In general, the amount of sweetener will vary with the desired amount of sweeteners selected for a
particular oral preparation. This amount will normally be 0.01% to about 40% by weight. The watersoluble sweeteners described in category A above, are preferably used in amounts of from 5% to
about 40% by weight, and most preferably from about 10% to about 20% by weight of the final
composition. In contrast, the artificial sweeteners described in categories B and C are used in
amounts of about 0.005% to about 5.0% and most preferably about 0.05% to about 2.5% by weight
of the final composition. These amounts are ordinarily necessary to achieve a desired level of
sweetness independent from the flavor level achieved from flavorants.
Suitable flavorings include both natural and artificial flavors, and mints such as peppermint, citrus
flavors such as orange and lemon artificial vanilla, cinnamon, various fruit flavors, both individual and
mixed, and the like are contemplated. The flavorings are generally utilized in amounts that will vary
depending upon the individual flavor, and may, for example, range in amounts of about 0.1% to
about 6% by weight of the final composition.
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The colorants useful in the present invention, include the pigments which may be incorporated in
amounts of up to about 2% by weight of the composition. Also, the colorants may include other dyes
suitable for food, drug and cosmetic applications, and known as F.D. & C. dyes and the like. The
materials acceptable for the foregoing spectrum of use are preferably water-soluble. Illustrative
examples include the indigo dye, known as F.D & C. Blue No. 2, which is the disodium salt of 5,5indigotindisulfonic acid. Similarly, the dye known as F.D & C. Green No. 1, comprises a
triphenylmethane dye and is the monosodium salt of 4-[4-N-ethyl-psulfobenzylamino)diphenylmethylene]-[1-(N-ethyl-N-p-sulfoniumbenzyl)-2,5-cyclohexadienimine].A
full recitation of all F.D & C. and D. & C colorants useful in the present invention and their
corresponding chemical structures may be found in the Kirk-Othmer Encyclopedia of Chemical
Technology, 3rd Edition, in volume 6, at pages 561-595, which text is accordingly incorporated
herein by reference.
The present invention is further illustrated by the following examples. All parts and percentages in the
examples and throughout the specification and claims are by total weight unless otherwise indicated.
The following definitions and procedures are utilized throughout the examples.
MINIMAL GROWTH INHIBITORY CONCENTRATION
The minimal inhibitory concentration (MIC) of the test compound is the minimum concentration of
compound required to inhibit growth of the test organism. The MIC is determined by serially diluting
the test solution through tubes of sterile broth. The tubes are inoculated and incubated at 37 DEG C
for 48 hours. At the end of the incubation time, growth is checked macroscopically. The lowest
concentration of test compound to inhibit growth is the MIC.
CHECKERBOARD TITRATION
This technique is used to assess antibacterial activity of combinations. The 'checkerboard' is the
pattern found by multiple combinations of two antimicrobial agents in concentrations equal to, above,
and below their minimal inhibitory concentration for the organism being tested. The checkerboard
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consists of columns which contain the same amount of one antimicrobial which is diluted along the xaxis and rows which each contain the same amount of the antimicrobial (diluted along the y-axis).
Thus each tube is a unique combination of the two agents.
A method of quantitating synergy is the 'fractional inhibitory concentration' (FIC) index. For each row,
the FIC index is calculated from the lowest concentration of agent necessary to inhibit growth. The
FIC of each agent is derived by dividing the concentration of the agent present in that tube by the
minimal inhibitory concentration of the organism to that agent alone. The FIC index is then the sum of
these values for both agents at that point.
Fractional Inhibitory Concentration Index is used as a measure of synergy. When the FIC index is
equal to or less than 0.5, the combination is synergistic. When the FIC index is greater than 0.5 but
less than 2.0 the combination is additive. When the FIC index is greater than 2.0 the combination is
antagonistic. The FIC index is calculated as follows:
where:
MIC(A) is the concentration of antimicrobial A in a tube which is the lowest inhibitory concentration in
its row from the checkerboard titration. MICA is the MIC of the organism to antimicrobial A alone.
FICA is the fractional inhibitory concentration of antimicrobial A. MIC(B) MICB, and FICB are defined
in the same fashion for antimicrobial B.
Vehicle:
1.5 grams of benzoic acid is dissolved in one liter of 28.5% enthanol in water (v/v).
EXAMPLE 1
Inventive Experiments 1, 2, 3 and 4
This example illustrates the Minimum Inhibitory Concentration (MIC) and Fractional Inhibitory
Concentration (FIC) index of a mixture of essential oils, and chlorhexidine alone and in combination
for the bacterium Streptococcus mutans ATCC 25175. The experiment was repeated four times.
All four experiments demonstrate synergy between chlorhexidine and the mixture of essential oils as
determined by an FIC index of less than or equal to 0.5.
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EXAMPLE 2
Non-Inventive Experiments A, B, C, and D
This example illustrates the Minimum Inhibitory Concentration (MIC) and Fractional Inhibitory
Concentration (FIC) index of Chlorhexidine, and individual essential oils alone and in combinations of
individual essential oils with chlorhexidine for the bacterium Streptococcus mutans ATCC 25175.
None of the tested combinations demonstrates synergy as determined by the FIC index. All
combinations have an FIC index greater than 0.5.
EXAMPLE 3
Inventive experiments 5, 6 and 7
This example illustrates the Minimum Inhibitory Concentration (MIC) and Fractional Inhibitory
Concentration (FIC) index of a mixture of essential oils, and chlorhexidine alone and in combination
for the bacteria Streptococcus sanguis ATCC 19558, Actinomyces viscosus T14V and Candida
albicans ATCC 18804.
The tested combinations show synergy for S. sanguis and C. albicans and a strong additive effect
for A. viscosus as determined by the FIC index.
EXAMPLE 4
This example demonstrates a mouthrinse of the present invention prepared by mixing together the
following ingredients:
The final pH of the above mouthrinse is adjusted to between 4.1 and 4.3 with sodium hydroxide. This
mouthrinse shows improved antimicrobial activity.
42/1651
This invention being thus described, it will be obvious that the same may be varied in many ways.
Such variations are not be regarded as a departure from the spirit and scope of the invention and all
such modifications are intended to be included within the scope of the following claims. Claims:
1. An antibacterial oral composition comprising an oral vehicle, an antibacterial bis-biguanido
hexane compound and a mixture of at least two essential oils selected from the group consisting of
thymol, eucalyptol, methyl salicylate and menthol.
2. The oral composition of Claim 1 wherein the antibacterial bis-biguanido hexane compound is a
pharmaceutically acceptable water soluble salt of a compound selected from the group consisting of
chlorhexidine and alexidine.
3. The oral composition of the claims 1 or 2, wherein the antibacterial bis-biguanido hexane
compound is present in an amount from about 0.01% to about 10% by weight of the composition
based on the free base form of said compound.
4.The oral composition according to anyone of the claims 1 to 3, wherein the mixture of essential oils
is present in an amount from about 0.05% to about 10% by weight of the composition.
5. The oral composition according to anyone of the claims 1 to 4, wherein the oral vehicle comprises
a liquid vehicle having a pH value of about 4.0 to about 7.0.
6. The oral composition according to anyone of the claims 1 to 5, wherein the oral vehicle is an
aqueous-alcohol combination and said antibacterial oral composition is a mouthwash having a pH
value of about 4.0 to about 7.0.
7. The mouthwash composition of Claim 6 wherein the bis-biguanido hexane compound is a watersoluble pharmaceutically acceptable chlorhexidine salt present in an amount from about 0.01% to
about 10% based on its free base weight and the mixture of essential oils are present in an amount
from about 0.05% to about 10% all percents are by weight of the total composition.
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8. A method of improving oral hygiene comprising applying to the oral cavity an effective amount of
an antibacterial oral composition as defined in Claim 1.
9. The method of Claim 8 wherein said antibacterial oral combination is contacted with an organism
selected from the group consisting of Streptococcus mutans, Streptococcus sanguis, and mixtures
thereof.
44/1651
11. AU7040498 - 30.09.1999
ANTIFUNGAL AND ANTIBACTERIAL COMPOSITIONS CONTAINING MELALEUCA ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU7040498
Inventor(s):
ANDRIOLLI ADRIANO (IT); PANNI FAUSTO (IT)
Applicant(s):
ANDRIOLLI ADRIANO (IT); PANNI FAUSTO (IT); FARMILA FARMA MILANO (IT)
IP Class 4 Digits: A61K
IP Class:
A61K35/78
E Class: A61K35/78
Application Number:
WO1998EP01708 (19980324)
Priority Number: WO1998EP01708 (19980324)
Family: AU7040498
Cited Document(s):
FR2705571; FR2748204; GB2293547
Abstract:
THE PRESENT INVENTION RELATES TO PHARMACEUTICAL COMPOSITIONS FOR THE SYSTEMIC
ADMINISTRATION OF MELALEUCA ESSENTIAL OIL.Description:
ANTIFUNGAL AND ANTIBACTERIAL COMPOSITIONS CONTAINING
MELALEUCA ESSENTIAL OIL
The present invention relates to pharmaceutical compositions for the systemic administration of
Melaleuca essential oil.
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The plants belonging to the genus Melaleuca are a known source of essential oils which have been
used for a long time in the topical treatment of infections sustained by fungi or bacteria. In particular,
the use of an essential oil extracted by steam distillation of fresh leaves of Melaleuca alternifolia,
which is a shrub growing exclusively in Australia, is widely diffused.
Melaleuca alternifolia oil (Tea tree oil) is characterized by a low concentration of 1,8 cineole ( 36%),
and is commercially available in a stabilized form which fulfils such Pharmacopoeias
standardizations as by the
British Pharmaceutical Codex 1949 (p. 597-598),
Martindale, The Extra Pharmacopoeia, 28th Ed., 1982 (p.
678) and The Dispensatory of the United States of
America, 25th Ed., (p. 1610).
The composition of Melaleuca alternifolia oil is reported, for example, in J. Agric., Food Chem. 1989,
37,1330.
The interest in this active ingredient of the traditional medicine has increased recently, as proved by
the numerous Patent applications concerning specific therapeutical or cosmetic uses. ~
JP-A-4198131, for example, discloses compositions for the treatment of wounds and burns; GB-A2293547 describes the use of Melaleuca oil for the treatment of infections of the oral cavity, gingivitis
and periodontitis; JP-A-6345616 discloses cosmetic uses as a deodorant and UV filter; finally, JP4074138 describes the use of Melaleuca essential oil as a promoter of the transdermal absorption of
medicaments.
All of the traditional, known uses as well as the recent Patent applications cited above claim
exclusively the topical administration of Melaleuca essential oil.
Now it has surprisingly been found that Melaleuca oil, when administered systemically and in
particular orally, exerts bacteriostatic and antifungal effects without causing toxic side-effects.
Therefore, the present invention relates to pharmaceutical compositions which can be administered
systemically, containing a Melaleuca essential oil as the active ingredient.
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The compositions of the invention can be prepared according to conventional techniques and
excipients, as described for example in Remington's Pharmaceutical
Sciences Handbook, Mack Pub.. Co., NY.
The compositions of the invention can be administered in forms suitable for the oral, parenteral or
rectal administrations, the oral route being preferred. Suitable oral formulations include soft-or hardgelatin capsules, granulates, sugar-coated pills and the like.
The essential oil can be prepared from plants of the genus Melaleuca belonging to the species
alternifolia, cajpuli, quinquenervia, uncinata, bracteata, optionally in a mixture thereof. The use of
the stabilized essential oil of Melaleuca alternifolia is particularly preferred.
The unit dosages can range from 10 to 100 mg of oil, preferably from 20 to 80 mg, most preferably
from 30 to 60 mg of oil per 15 kg of body weight of the patient, to be administered one or more times
daily.
The treatment can be prolonged up to 15-30 days.
The compositions of the invention proved to be useful in the treatment of mycosis due to Candida,
Aspergillus, Trycophyton and of infections of the urinary and respiratory tracts sustained by
Grampositive or Gram-negative bacteria.
The following examples further illustrate the invention.
EXAMPLE 1
Soluble granulat
Unitary formulation
Cane sugar g 2.400
Lactose O. P. g 2.355
Glucose solids g 0.100
Bitter cocoa g 0.050
Liquorice dry extract g 0.050
Melaleuca oil g 0.040
Sodium saccharin g 0.005
Total g 5.
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EXAMPLE 2
Capsules
Melaleuca alternifolia oil mg 40
Liquorice root powder mg 10
Lactose O. P. mg 170
Maize starch mg 70
Alcohol BG 96 mg 0.008
Magnesium stearate mg 10
mg 300 gelatin capsules size 1.
Claims:
CLAIMS 1. Pharmaceutical compositions systemically administrable containing Melaleuca essential
oil as active ingredient.
2. Compositions according to claim 1, containing essential oil of Melaleuca alternifolia.
3. Compositions according to claim 1 or 2 which can be administered orally.
4. Oral compositions according to claim 3 in the form of capsules, tablets, granulates.
5. Compositions according to any of the above claims containing 20 to 80 mg of essential oil.
48/1651
12. AU723540 - 31.08.2000
EXTRACTION OF ESSENTIAL OIL FROM CYPRESS PINE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU723540
Inventor(s):
COLLINS VINCENT JOSEPH (--)
Applicant(s):
COLLINS VINCENT JOSEPH (--); COLLINS MARYANN (--)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
AU20000022609 (20000324)
Priority Number: AU20000022609 (20000324); AU19980075075 (19980708)
Family: AU723540
49/1651
13. AU7270796 - 13.07.2000
ESSENTIAL OIL EVAPORATOR
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU7270796
Inventor(s):
DAVEY AMANDA MARTHA (--); DAVEY PETER WILLIAM (--)
Applicant(s):
DAVEY AMANDA MARTHA (--); DAVEY PETER WILLIAM (--)
IP Class 4 Digits: A61L
IP Class:
A61L9/03
Application Number:
AU19960072707 (19961111)
Priority Number: AU19960072707 (19961111); AU1995PN06491 (19951110); WO1996AU00710
(19961111)
Family: AU721801
50/1651
14. AU728188 - 21.09.1999
PROCESS FOR THE SIMULTANEOUS PRODUCTION OF ARTEMISNIN AND ESSENTIAL OIL FROM
THE PLANT ARTEMISIA ANNUA
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=AU728188
Inventor(s):
JAIN DHARAM CHAND (IN); TANDON SUDEEP (IN); KUMAR SUSHIL (IN);
BHAKUNI RAJENDRA SINGH (IN); BHATTACHARYA ASISH KUMAR (IN); KAHOL ATUL PRAKASH
(IN); SHARMA RAM PRAKASH (IN); SIDDIQUE MOHAMMED SHAFIQUE (IN)
IP Class 4 Digits: A61K
IP Class:
A61K35/78
E Class: A61K35/78
Application Number:
US19970944865 (19971006)
Priority Number: IN1997DE00652 (19970317)
Family: AU728188
Equivalent:
CA2218444; IN188174
Abstract:
THIS INVENTION RELATES TO A NOVEL PROCESS FOR THE DUAL PRODUCTION OF ESSENTIAL
OIL AND ARTEMISININ FROM THE PLANT ARTEMISIA ANNUA, SAID PROCESS COMPRISING
EXTRACTING THE PLANT WITH HEXANE, PARTITIONING THE HEXANE EXTRACT BETWEEN
HEXANE AND ACETONITRILE, HYDRODISTILLATION OF HEXANE RESIDUE AND MARC TO YIELD
ESSENTIAL OIL, FURTHER FRACTIONATION OF ACETONITRILE SOLVENT BETWEEN HEXANEBENZENE MIXTURE TO REMOVE ARTEMISINIC ACID, CHROMATOGRAPHING OF THE
ACETONITRILE PHASE TO PRODUCE SUBSTANTIALLY PURE ARTEMISININ, THE ARTEMISINIC
ACID IS REDUCED TO OBTAIN DIHYDRO ARTEMISINIC ACID WHICH IS THEN OXIDISED IN A
SINGLE STEP TO FORM ARTEMISININ.Description:
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FIELD OF THE INVENTION
The present invention relates to a process for the simultaneous production of essential oil and
artemisinin from the plant Artemisia annua. More particularly, the invention is related to a process for
the production of essential oil and artemisinin and conversion of artemisinic acid into artemisinin.
BACKGROUND OF THE INVENTION
Artemisia annua L. (Asteraceae) is a herb of Asiatic and Eastern European origin that has been also
naturalised in USA. This species is receiving considerable attention because of the antimalarial
activity of artemisinin of formula (1) a sesquiterpene lactone endoperoxide which is present in its
aerial parts. In clinical trials, mainly performed in southeast Asia, artemisinin and a series of semisynthetic derivatives have been proved to be effective against Plasmodium parasites with resistance
to the commonly used antimalarial drugs. Now, efforts are being made to make these drugs cheaply
available worldwide. In addition, A. annua is valued for its essential oil which has characteristic sweet
aroma. Its application in perfumery, cosmetics, aromatherapy and as an antimicrobial,
dermatological, fungicidal agents may provide an additional market for essential oil.
Artemisinic acid of formula (2) is the bio-synthetic precursor of artemisinin, which are generally
present in greater quantity that artemisinin in A. annua plant. Artemisinic acid can be converted into
artemisinin in good yield, thereby artemisinin amount obtained directly from the plant is increased 3-4
folds.
PRIOR ART REFERENCES OF THE INVENTION
So far, no prior art literature has provided a method for the simultaneous isolation of artemisinin and
essential oil from A. annua plant without destroying any of them. At present, the herb A. annua is
processed for obtaining the essential oil by hydrodistillation method (Woerdenbag, H. J. ; Pras, N;
Chen, N. G., Bang Bui-Thi; Bos, R., Uden Wim Van; Pham Van Y; Boi, N. V; Batterman, S. and Lugt. C.
(1994), Artemisinin related sesquiterpenes and essential oil in Artemisia annua, during vegetation
period in Vietnam, Planta Medica, 60, 272-75). In this process, the fresh herb and water are heated in
Clevenger apparatus at 100 DEG C. for 3-4 hrs. The steam distillate is condensed and essential oil is
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collected but in this process artemisinin gets destroyed. As artemisinin is a thermally labile
compound, it gets decomposed during hydrodistillation .
In another process, to isolate artemisinin and other biogentic precursors, the dried plant material is
extracted with non polar solvent (hexane), partitioning the hexane extract between hexane and
acetonitrile, followed by chromatographying the acetonitrile phase over silica gel, elution with solvent
afforded different fractions, which on concentration and crystallization yielded artemisinin, artemisinic
acid, arteannuin B, but no essential oil is recovered in this process. Klayman, D. L. ; Lin, A. J. Acton,
N; Scovill, J. P.; Hoch, J. M.; Michous, W. K.; Theoharidis, A. D. and Dobek, A. S. J. Nat. Prods. 47,
(1984) 715. Another disadvantage in the above process is that the artemisinic acid being
predominant, it tends to elute with artemisinin, thus affecting the purity of the desired compound.
An improved method for the isolation of artemisinc acid from A. annua plant (Vonwiller, S. C., Hayne,
R. K, King, G. and Wang, H. Planta medica 59, 562-563 (1993) was reported. In this process,
methanolic extract of A. annua were partitioned between water and ether solvent. Ether residue was
treated with base to separate artemisinic acid fraction from artemisinin. The basic solution was
neutralized and further methylation of residue stirring with acid. After methylation the same base
extraction process was repeated to obtain artemisinic acid. The residue left after base extraction was
chromatographed to obtain artemisinin which afforded 57% of yield. In this process, total extract was
treated with base which destroyed some amount of artemisinin. The solvent namely ether used in the
process is low boiling and highly inflammable.
Artemisinic acid is the most abundant metabolite of A. annua and its conversion to artemisinin would
increase the yield of artemisinin. Roth, R. J and Acton, N., J. Chem. Edu. 68,612 (1991) have
prepared dihydroatermisinic acid by using excess quantity of NaBH4 and NiCl2 6H2 O in methanol.
Dihydroartemisinic acid was photo-oxidised at (-) 78 DEG C. in dichloro methane or at 0 DEG C. in
solvent acetone with methylene blue as photosynthesiser and oxygen was passed through the
solution with irradiating with high intensity lamp. The solution was evaporated and the residue was
taken up in the ether and filtered the solution to remove dye. The solvent was evaporated, residue
was re-dissolved in pet. ether, containing a few drops of trifluoroacetic acid and the photolysate was
left for four days to afford 17-30% artemisinin. In this process, photo oxidation was carried out at low
temperature and also used number of solvents, chemical and process steps.
BRIEF DESCRIPTION OF THE DRAWINGS
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FIG. 1A shows the chemical formula 1 which is the chemical substance artemisinin.
FIG. 1B shows the chemical formula 2, which is the chemical substance artemisinc acid.
SUMMARY OF THE INVENTION
The present invention provides a simple and efficient process for the simultaneous production of
artemisinin and essential oil from the plant A. annua and also a method for better recovery of
artemisinic acid and artemisinin without the use of chromatography and finally conversion of
artemisinc acid into artemisinin.
NOVELTY OF THE INVENTION
1. In the prior art, essential oil is obtained by hydro-distillation of fresh/dried plant material in which
artemisinin gets destroyed and the essential oil is obtained after 3 hrs. contact with steam, whereas
in this present invention, the dried plant material is extracted with n-hexane and the extract is
partitioned with aqueous acetonitrile. In this step, fatty material is seperated from artemisinin, so that
purification and recovery of artemisinin is improved as well as essential is obtained by
hydrodistillation of marc and hexane residue obtained in the partition step in which no artemisinin is
present. Therefore, in this process, no loss of artemisinin takes place. For the first time, 50% essential
oil is obtained from the marc of the plant. The quality of the oil is better and less time is required for
hydrodistillation. For the first time, the applicants have achieved the simultaneous production of
artemisinin and essential oil without destroying either of them.
2. In the previous process artemisinic acid was seperated from aqueous acetonitrile phase by the
treatment with sodiumcarbonate or chromatography. In this process, artemisinin present also gets
decomposed and only 57% artemisinin was recovered. But in the present invention, artemisinic acid
will be seperated from artemisinin before treatment with base, so that both the compounds are
recovered in 90% yield.
3. The conversion of artemisinic acid (obtained from A. annua) into artemisinin results in the best
utilization of the compounds obtained during the process as well as increases the yield of artemisinin
from the plant. As the synthesis of artemisinin is not economically viable plant remains the sole
source for its large scale production. In the present improved process, conversion takes place in
only two steps instead of the three steps as used in the prior art. The present process does not use
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any catalyst, photosynthesiser and oxygen. The reaction takes place at room temperature and work
up of the reaction is very simple to obtain artemisinin.
SUMMARY OF THE INVENTION
The process of the present invention consists of the following steps:
(i) drying and powdering A. annua plant,
(ii) extracting the said powdered herb of A. annua with hexane,
(iii) reducing the hexane extract from step (ii) above to 5-20% of its original volume under vacuum;
(iv) partitioning the hexane extract between hexane and acetonitrile water mixture;
(v) evaporation of the hexane phase obtained in step (iv) to dryness,
(vi) hydrodistillation of hexane residue from the step (v) and Marc (extracted plant material) to yield
essential oil,
(vii) removal of water from aqueous acetonitrile phase obtained from step (iv),
(viii) further fractionation of resultant acetonitrile phase after removal of water as obtained from step
(vii) between hexane-benzene mixture to obtain hexane-benzene extract and acetonitrile phase,
(ix) treating hexane-benzene fraction obtained from step (viii) with a base followed by neutralization,
extraction with chloroform, drying and crystallisation to obtain artemisinic acid,
(x) converting artemisinic acid obtained from step (ix) into artemisinin by reduction and photo
oxidation,
(xi) chromatographying of the evaporating acetonitrile residue obtained from step (viii) over silica gel
with hexane,
(xii) evaporation of the different fractions obtained from step (xi) and crystallization of the said
fractions containing artemisinin obtained from step (xi) and thereby producing substantially pure
artemisinin.
DETAILED DESCRIPTION OF THE INVENTION
In accordance with the method of the invention, employing n-hexane solvent for extraction of the
plant in which complete extraction of artemisinin and other bio-precursors and 50% of essential oil.
The step of partitioning separates the fatty material from other products containing artemisinin,
whereas defatting of crude extract with n-hexane, alcohol etc., results in the loss of artemisinin and
filteration of fat is a difficult operation which is avoided in this process. In the previous process, the
hydrodistillation of plant material to obtain essential oil, due to high temperature artemisinin gets
destroyed during operations but here the applicants have separated the artemisinin fraction from
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fatty material which on hydrodistillation yield essential oil. In this process, the remaining essential oil
in plant which is not extracted during hexane extraction which is to be identified and recovered from
the extracted plant material (Marc) by hydrodistillation. The hydrodistillation of marc and
concentrated hexane residue took less time and size of distillation unit is drastically reduced which is
required during fresh plant extraction. During drying, the structure changes of the cells of plant
material favour the diffusion of the oil components out of them.
The partitioning step in liquid-liquid extraction done in Karr type column at particular flow rate and
stirring, transfer the artemisinin and two major sesquiterpene, in the acetonitrile phase (polar solvent)
with concomitant reduction of in the amount of extract, i.e. of the order of 20-24% of the original
hexane extract in the single operation.
The acetonitrile phase rich in artemisinic acid only 10% of the acid isolated by crystallization before
chromatography. Here in this process, complete extraction or artemisinic acid by partitioning
between acetonitrile and hexane-benzene mixture, which reduced the bulkness of the acetonitrile
extract further by 50%. Using the method of the present invention, the second partitioning step which
remove artemisinic acid prior to elution of artemisinin without chromatography, enhancing the
purification of artemisinin, less consumption of silica gel, time and solvent and economize the cost of
the drug-artemisinin. In the Vonwiller process, artemisinic acid was isolated from the ether extract by
treatment with a base. In the ether extract, artemisinin which was also present get decomposed
during the base extraction. Here the applicants have separated the artemisinic acid fraction from
artemisinin.
In the chromatography step of the invention, ratio of (1:3)(solute to adsorbent) was discovered to
yield excellent results. In the known process, a ratio of 1:10 has been required. In the solvent system
of the invention, n-hexane was found to be quite effective rather than 10-20% ethyl acetate in nhexane mixture. The silica gel used as a packing material in the example here is silica gel-H. (Mesh
size-200). The elution of compounds done under reduced pressure. In this way elution of artemisinin
by n-hexane rather than 15% ethyl acetate-hexane mixture, arteannuin B was covered by 5% ethyl
acetate hexane mixture. By way of chromatography step of the process of elution, artemisinin was
obtained from the oily greenish yellow fraction eluted with hexane and purification of artemisinin was
carried by crystallization from ethyl acetate-hexane (1:4). In accordance with the description herein
used, solvent, silica gel and time for chromatography reduced drastically.
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Accordingly, the present invention provides a novel process for the simultaneous production of
essential oil and artemisinin from the Artemisia annua, said process comprising (i) drying and
powdering A. annua plant; (ii) extracting the said powedered herb of A. annua with hexane; (iii)
reducing the hexane extract obtained from step (ii) above to 5-20% of its original volume under
vacuum; (iv) partitioning the hexane extract between hexane and acetonitrile water mixture; (v)
evaporation of the hexane phase obtained in step (iv) to dryness; (vi) hydrodistillation of hexane
residue obtained from the step (v) and Marc (extracted plant material) to yield essential oil; (vii)
removal of water from aqueous acetonitrile phase obtained from step (iv); (vii) further fractionation of
resultant acetonitrile phase after removal of water as obtained from step (viii) with a base followed by
neutralization, extraction with chloroform, drying and crystallization to obtain artemisinic acid; (x)
converting artemisinic acid obtained from step (ix) into artemisinin by reduction and photo oxidation;
(xi) chromatographying of the evaporating acetonitrile residue obtained from step (viii) over silica gel
with hexane; (xii) evaporation of the different fractions obtained from step (xi) and crystallization of
the said fractions containing artemisinin obtained from step (xi) and thereby producing substantially
pure artemisinin.
The dried parts of the plant used for the extraction can be selected from any part of the plant,
preferably leaves, infloroscence and small stems and the hexane extract of the A. annua as used in
step (i) is reduced to 10% of its original volume under vacuum. Preferably, the partitioning between
hexane and aqueous acetonitrile phase is done in the ratio of 2:3 in liquid-liquid extraction column
and the aqueous acetonitrile mixture used is in the ratio of 1:1 to 1:5.
In the present process, the single extraction step (ii) is carried out between two phases for 3 hrs.
and the hydrodistillation of Marc (extracted plant material) in step (i) and residue obtained from (iii)
yield essential oil upto 2.0 hrs.
Also, in the present process, further partitioning between acetonitrile and hexane-benzene mixture
after removal of water is done to isolate artemisinic acid and 10-30% benzene used in hexane
solvent was used for the extraction of artemisinic acid.
Preferably, extraction of artemisinic acid is carried out where hexane-benzene mixture is evaporated,
extracted with 5% of sodium carbonate solution and the basic solution is neutralized with 5% HCl
solution, extracting with chloroform, drying the solvent and crystallization with ethyl acetate yielding
artemisinic acid.
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One embodiment of the invention provides a process for the conversion of artemisinic acid into
artemisinin employing steps such as reduction and photo oxidation and the reduction is carried out
by the following steps comprising (i) dissolving artemisinic acid and NiCl2.6h2 O in dry methanol; (ii)
adding sodium borohydride to the resultant solution at 0 DEG C. over a 2 hr. period; (iii) neutralising
the solution obtained in step (ii) with 5% aqueous HCl solution and (iv) isolating and crystallizing the
dihydro artemisinic acid in ethyl acetate to obtain pure dihydro artemisinic acid. However, the step of
photo oxidation is carried out by comprising (i) dissolving the dihydroartemisinic acid in the solvent
dichloromethane-ethyl acetate; (ii) oxidising the solution obtained in the step (i) in the presence of
fluorescent light (40W) daily for two hours upto 8 days; (iii) concentrating the solution obtained in
step (ii) and recrystallizing the residue in hexane to isolate artemisinin.
Preferably, in the present process, the chromatographic step is carried out in SiO2 column
comprising a solute having adsorbent ratio 1:3. The elution with n-hexane solvent is being done
under vacuum at 100-150 mm Hg absolute pressure and the chromatographic absorbent used is
Silica gel H with mesh size 200.
The process of invention is illustrated by the following examples which should not be construed to
limit the scope of the present invention.
The following examples also illustrates the specific embodiments of the method of the invention.
EXAMPLE 1
Dried powdered herb of A. annua (40 kg) was percolated with hexane (60-80 DEG C.) (6.times.200
liter) in a soxhlet for 8 hrs. The extracted solvent was reduced to 20 liter. The non polar phase
(hexane extract) was partitioned with aqueous acetonitrile phase (1:5) presaturated each other in the
liquid-liquid extraction (Karr type) column. After 3 hrs. two phases were separated. The aqueous
acetonitrile phase was back washed using 10% of its separated. The aqueous hexane (2.0 litre).
Evaporation of non polar phase provided (2.20 kg) residue. The residue was boiled in Clevenger
apparatus with 10 litre water for 1.5 hrs, which yielded the essential oil (80 ml). The marc (extracted
plant material) (40 kg) was hydrodistilled in a distillation unit, which yield essential oil (100 ml) in 1 hr.
The water from aqueous acetonitrile phase was removed by adding 1 kg sodium chloride. The
acetonitrile solvent (25.0 litre) was further partitioned between acetonitrile extract and 10% benzenehexane mixture in the same karr type column. After separation of two phases, evaporated the
benzene-hexane mixture yielded (200 gm) of residue. The residue (200 gm) was dissolved in
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chloroform (400 ml) and extracted with 5% Na2 CO3, solution (3.times.500 ml). Basic solution was
neutrilized with 10% HCl solution (400 ml). The neutral solution was extracted with chloroform,
concentrated and crystallization with ehtylacetate yielded artemisinic acid (71.8 gm). The acetonitrile
phase after concentration provide a residue (300 gm) which was filtered over silica gel (900 gm)
under vacuum at 100-150 mm Hg absolute pressure. Artemisinin was obtained from the viscous
greenish yellow fraction elutes with n-hexane. Purification of artemisinin was carried by
recrystallization with ethyl acetate/hexane (1:4) to yield artemisinin (18 gm) Arteannuin B was
obtained from the fraction eluted with 5% acetate in hexane. Evaporation of the fraction and
crystallization yielded arteannuin B (36.5 kg).
The above procedure was repeated two times on the same scale and consistently provided the
same yield of artemisinin and other constituents.
EXAMPLE 2
The process followed as in example 1 in which the organic phase (20 litre) was partitioned with
aqueous acetonitrile phase (1:5, 30 litre) in same extraction column for the same period of time. The
acetonitrile phase after removal of water was dried over anhydrous sodiumsulphate and
concentrated under reduced pressure to yield a residue (0.55 kg). This residue was
chromatographed over silica gel (2.5 kg) and eluted with different ratio of ethyl acetate-hexane.
Artemisinin was obtained from column fractions eluted from 8% ethyl acetate-hexane. Evaporation
and crystallization with hexane ethyl acetate mixture afforded pure artemisinin (18.0 gm) fraction
eluted from 5% ethyl acetate hexane yielded artemisinic acid (70.6 gm) where as 12% ethyl acetate
in hexane fraction afforded arteannuin B (35.8 gm).
EXAMPLE 3
The process of extraction of A. annua was followed as in example 1 in which the hexane phase (20
litre) was partitioned with aqueous acetonitrile phase (1:3, 30 litre) in same extraction column for the
same period of time and speed. After partitioning the hexane phase was concentrated to yield (1.82
kg) residue which on hydrodistillation yielded essential oil (50 ml). The acetonitrile extract was
concentrated after removal of water and yielded viscous mass (0.8 kg). This viscous mass was
chromatographed over silica gel (4.0 kg) and eluted with different ratio of solvent ethyl acetatehexane. Artemisinin was obtained from column fractions eluted with 10% ethyl acetate-hexane.
Evaporation and crystallisation with hexane ethyl acetate mixture afforded pure artemisinin (17.0 gm).
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EXAMPLE 4
Dried herb of A. annua (40.0 kg) was extracted with n-hexane in a soxhlet apparatus. The extracted
solvent was reduced to 20 litre. The hexane soluble fraction (10 litre) was partitioned with aqueous
acetonitrile phase (1:1, 30 litre) in same extraction column. The hexane soluble fraction obtained after
partitioning was evaporated and residue (1.70 kg) was boiled in Clevenger apparatus with 8 litre
water for 3 hrs. which yield the essential oil (40 ml). The acetonitrile phase was concentrated and
yielded viscous mass (1.24 kg) which on chromatograph on silica gel as per example 3 yielded pure
artemisinin (16.2 gm).
EXAMPLE 5
Artemisinic acid is isolated from A. annua extract as in example 1 was used for conversion into
artemisinin. Artemisinic acid (100 mg) was dissolved in 100 ml methanol containing 150 mg
NiCl2.6H2 O, 300 mg of NaBH4 powder was added in small portions over 2 hr. period to a stirred
and cooled solution . After the reaction was completed, excess reducing agent was destroyed by
adding 20 ml of 5% aqueous HCl. The mixture was filtered to remove the insoluble impurities and
then the aqueous methanolic solution was extracted with ether which was washed with water, dried
and concentrated to afford 105 mg of crude dihydroartemisinic acid. Dihydroartemisinic acid (100
mg) was dissolved in dichloromethane-ethyl acetate (7:3, 20 ml), and the reaction mixture was left for
8 days at room temperature and irradiated with fluorescent light (tubelight) (40W) for a period of 2 hrs.
per day. Solvent was removed under vacuum and the residue was recrystallized with n-hexane to
afford artemisinin (25%.
The new process of production of essential oil and artemisinin, the subject matter of this patent,
offered a number of advantages such as:
1. The process for the dual production of artemisinin and essential oil (80%) from A. annua has been
developed for the first time.
2. Consumption of silica gel has decreased due to reduction of charging material upto 10% of its
original hexane extract and ratio of adsorbent to solute is (1:3).
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3. The partitioning step between n-hexane and aqueous acetonitrile phase allowed the selective
transfer of artemisinin and other sesquiterpenes into polar phase leaving non polar constituents in
hexane solvent which results in a better method for the removal of large quantity of fat and other
impurities, whereas removal of fats is difficult operation.
4. Hydrodistillation of extracted plant and hexane residue is a better alternative to recover major
portion of the essential oil than hydrodistillation from fresh herb where artemisinin gets destroyed.
5. In this process, after recovery of essential oil from hexane residue, the applicants also obtained
major fatty acids material which on further purification yield free fatty acids.
6. Isolation of artemisinic acid without chromatography, as by product, can be converted into
artemisinin which will increase overall yield of the artemisinin from the plant by 2-3 folds.
7. Conversion of artemisinic acid into artemisinin in two simple steps without using catalyst, dye, few
solvents and oxygen. The present reaction takes place at room temperature.
8. The process is highly efficient and economical as most of the solvents and adsorbents used in the
process are being recovered and reused.
9. All these advantages are significant economic value for large scale production of antimalarial
drug artemisinin. Claims:
We claim:
1. A process for the simultaneous production of essential oil and artemisinin from the Artemisia
annua, said process comprising
(i) drying and powdering an A. annua plant part to produce a dried and powdered plant or plant part,
(ii) extracting the powdered plant or plant part of A. annua with hexane to produce a hexane extract
and a residual Marc.
(iii) reducing the hexane extract to 5-20% of its original volume under vacuum,
(iv) partitioning the resultant concentrated hexane extract between hexane and acetonitrile water
mixture to produce a hexane phase and an aqueous acetonitrile phase,
(v) evaporating the hexane phase to dryness to obtain a hexane residue,
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(vi) hydrodistilling the hexane residue and residual Marc to yield essential oil,
(vii) removing water from the aqueous acetonitrile phase to produce an acetonitrile phase,
(viii) extracting the acetonitrile phase with a hexane-benzene mixture to obtain a hexane-benzene
extract and a residual acetonitrile phase,
(ix) removing the hexane-benzene solvent to yield a residue
(x) dissolving the residue in chloroform
(xi) extracting the chloroform solution with a base,
(xii) neutralizing the aqueous basic solution,
(xiv) extracting the neutralized aqueous solution with chloroform,
(xiv) evaporating the chloroform and crystallizing the extracted hexane-benzene extract to produce
artemisinic acid,
(xv) reducing and photooxidizing the artemisinic acid,
(xvi) chromatographing the acetonitrile phase over silica gel with hexane and collecting different
eluted fractions,
(xvii) evaporating the different eluted fractions crystallizing said fractions to produce substantially
pure artemisinin.
2. A process claimed in claim 1, wherein dried parts of the plant used for the extraction are selected
from any part of the plant.
3. A process as claimed in claim 1 wherein partitioning between hexane and acetonitrile water
mixture used in step (iv) is done in the ratio of 2:3 in liquid-liquid extraction column.
4. A process as claimed in claim 1 wherein acetonitrile water mixture used in step (iv) is in the ration
of 1:1 to 1:5.
5. A process as claimed in claim 1 wherein partitioning step (iv) is carried out between two phases
for 3 hrs.
6. A process as claimed in claim 1, wherein the time taken for hydrodistillation of Marc ranges
between 30 minutes to 120 minutes.
7. A process as claimed in claim 1, wherein the hexane residue is hydrodistilled for 30 minutes to
120 minutes to obtain the essential oil.
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8. A process as claimed in claim 1 wherein fractionation between acetonitrile and hexane-benzene
mixture after removal of water in step (viii) is done to isolate artemisinic acid.
9. A process as claimed in claim 1 wherein benzene used in hexane-benzene mixture used as
solvent ranges between 10-30%.
10. A process as claimed in claim 1, wherein the base used in step (ix) is a 5% solution of sodium
carbonate.
11. A process as claimed in claim 1 wherein basic solution in step (ix) is neutralized with 5% HCl
solution, extracted with chloroform followed by drying of solvent and crystallisation with ethyl acetate
yielding artemisinic acid.
12. A process as claimed in step (x) of claim 1, wherein reduction in step (x) comprises (i) dissolving
artemisinic acid and NiCl2.6H2 O in dry methanol; (ii) adding sodium borohydride to the resultant
solution at 0 DEG C. over a 2 hr. period; (iii) neutralising the solution obtained in step (ii) with 5%
aqueous HCl solution and (iv) isolating and crystallizing the dihydro artemisinic acid in ethyl acetate
to obtain pure dihydro artemisinic acid.
13. A process as claimed in claim 1, wherein the photo oxidation comprises (i) dissolving the
dihydro artemisinic acid in dichloromethane--ethyl acetate solvent; (ii) oxidising the solution obtained
in step (i) in the presence of fluorescence light daily for two hours up to 8 days; (iii) concentrating the
solution obtained in step (ii) and recrystallizing the residue in hexane to isolate artemisinin.
14. A process as claimed in claim 1 wherein the chromatographic step is carried out in SiO2
columns comprises a solute having adsorbent ration 1:3.
15. A process as claimed in claim 1 wherein the elution with n-hexane solvent is being done under
vacuum at 100-150 mm Hg absolute pressure.
16. A process as claimed in claim 1 wherein chromatographic adsorbent used is Silica gel H with
mesh size of about 200.
17. A process for the simultaneous production of essential oil and artemisinin from the plant A.
annua wherein the yield of essential oil obtained from the marc of the plant is about 50%.
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18. A process for the simultaneous production of essential oil and artemisinin from the plant A.
annua wherein artemisinic acid and artemisinin are recovered in about 90% yield.
19. A process as claimed in claim 2, wherein the dried part of the plant is selected from the group
consisting of leaves, infloroscence and small stems.
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15. BG38718 - 14.02.1986
CONTAINER FOR DISTILLING OF ESSENTIAL OIL RAW- MATERIALS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=BG38718
Inventor(s):
TODOROV (BG); GENEV (BG)
Applicant(s):
TODOROV (BG); GENEV (BG)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
BG19840067227 (19841022)
Priority Number: BG19840067227 (19841022)
Family: BG38718
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16. BG39948 - 15.09.1986
GAS CHROMATOGRAPHY METHOD FOR ANALYSIS OF ESSENTIAL OIL MIXTURE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=BG39948
Inventor(s):
DIMITROV (BG); PETROVA (BG)
Applicant(s):
DIMITROV (BG); PETROVA (BG)
IP Class 4 Digits: C11B; G01N
IP Class:
C11B9/00; G01N30/12
Application Number:
BG19850069945 (19850425)
Priority Number: BG19850069945 (19850425)
Family: BG39948
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17. BG42386 - 15.12.1987
FOAM EXTINGUISHER FOR WASTE WATERS FROM ESSENTIAL OIL- COSMETIC MANUFACTURE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=BG42386
Inventor(s):
PIRONKOV (BG); MINCHEVA (BG); ZGUROVSKA (BG); PENEVA (BG);
PIRONKOVA (BG)
Applicant(s): PIRONKOV (BG); MINCHEVA (BG); ZGUROVSKA (BG); PENEVA (BG);
PIRONKOVA (BG)
IP Class 4 Digits: B01D
IP Class:
B01D19/04
Application Number:
BG19860076312 (19860829)
Priority Number: BG19860076312 (19860829)
Family: BG42386
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18. BG48933 - 14.06.1991
METHOD FOR MICROBIOLOGICAL PREPARING OF ESSENTIAL OIL PRODUCTS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=BG48933
Inventor(s):
KUPENOV LJUBOMIR G (BG)
Applicant(s):
KUPENOV LJUBOMIR G (--)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
BG19890090044 (19891017)
Priority Number: BG19890090044 (19891017)
Family: BG48933
Abstract:
THE METHOD IS APPLIED IN PERFUMERY-COSMETIC, PHARMACEUTICAL AND FOOD
INDUSTRIES. IT ENSURES THE DERIVATION OF ETHERIC-OIL PRODUCTS SUCH AS CONCRETES,
ETHERIC OILS, ABSOLUTE, BIO-PHYTANOLYLES AND RESINOIDES WITH INCREASED OUTPUT
AT A SIGNIFICANTLY HIGHER COEFFICIENT OF USE OF THE ETHERIC OIL RAW MATERIAL. THE
LATTER IS SUBJECT TO FERMENTATION WITH FACULTATIVE ANAEROBIC ARBUTIN-POSITIVE
AND DEVELOPING AT A HIGHER TEMPERATURE STRAIN CANDIDA MALTOSA, REGISTERED IN
NBIMCC UNDER NO. 1777 AT A TEMPERATURE BETWEEN 15 TO 55 DEGREES C, IN THE GIVEN
CASE IN A COMBINATION WITH FUNGUS PENICILLINUM RESTRICTUM NBIMCC NO 398 AND
PENICILLINUM ADAMETZII, REGISTERED UNDER NBIMCC UNDER NO. 1776 AND YEAST
CANDIDA SP., REGISTERED IN NBIMCC UNDER NO.1778, AFTER WHICH THE SOLID AND LIQUID
PHASES TOGETHER OR INDIVIDUALLY ARE SUBJECT TO DISTILLATION AND EXTRACTION OF
THE DISTILLATION WATERS WITH APROTONIC SOLVENTS OR TO EXTRACTION BY APROTONIC
AND PROTONIC ORGANIC SOLVENTS.
68/1651
19. BG98203 - 30.06.1995
METHOD FOR THE PREPARATION OF ESSENTIAL OIL FROM OLEAGINOUS ROSE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=BG98203
Inventor(s):
JANAKIEVA NIKOLINA M (BG); ZHELEVA LARISA JU (SU); OBUSHTAROVA
RUMJANA T (BG); LAFCHIEV KHRISTO B (BG); BALINOVA ANASTASIJA D (BG)
Applicant(s): JANAKIEVA (BG); ZHELEVA (SU); OBUSHTAROVA (BG); LAFCHIEV (BG);
BALINOVA (BG)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
BG19930098203D (19931108)
Priority Number: BG19930098203 (19931108)
Family: BG98203
69/1651
20. CA1026989 - 28.02.1978
ESSENTIAL OIL COMPOSITION AND METHOD OF MAKING SAME
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CA1026989
Inventor(s):
BECK EUGENE E (--)
Applicant(s):
BECK EUGENE E (--)
Application Number:
CA19720152462 (19720925)
Priority Number: CA19720152462 (19720925)
Family: CA1026989
70/1651
21. CA1290612 - 15.10.1991
SOLID ESSENTIAL OIL FLAVOR COMPOSITION AND METHOD OF MANUFACTURE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CA1290612
Inventor(s):
MUTKA JERRY R (US); MILLER DENNIS H (US)
Applicant(s):
SUNKIST GROWERS INC (US)
IP Class 4 Digits: A23L
IP Class:
A23L1/222; A23L1/09
Application Number:
CA19860503795 (19860311)
Priority Number: US19850754105 (19850712)
Family: CA1290612
Abstract:
SOLID ESSENTIAL OIL FLAVOR COMPOSITION AND METHOD OF MANUFACTURE A SOLID
ESSENTIAL OIL FLAVOR COMPOSITION HAVING A HIGH ESSENTIAL OIL CONTENT AND A
PROCESS FOR PREPARING THE PRODUCT ARE DISCLOSED, THE PROCESS INVOLVING
PREPARATION OF A HEATED OR COOKED AQUEOUS MIXTURE OF A SURFAR AND STARCH
HYDROLYSTATE TOGETHER WITH AN EMULSIFIER. A SELECTED ESSENTIAL OIL OR OTHER OILSOLUBLE FLAVOR IS COMBINED AND BLENDED WITH A MIXTURE IN A CLOSED VESSEL UNDER
CONTROLLED PRESSURE CONDITIONS TO FORM A HOMOGENEOUS MELT, THE MELT BEING
EXTRUDED INTO A RELATIVELY COOL SOLVENT, DRIED AND COMBINED WITH A SELECTED
ANTICAKING AGENT TO PRODUCE THE STABLE, RELATIVELY NON-HYGOSCOPIC PARTICULATE
FLAVOR COMPOSITION OF THE INVENTION. THE SELECTED QUANTITY OF ESSENTIAL OIL
FLAVOR BLENDED INTO THE HOMOGENEOUS MELT BEING SUFFICIENT TO YIELD ABOUT 12 TO
35% BY WEIGHT OF ESSENTIAL OIL IN THE ENCAPSULATED SOLID PARTICULATE
COMPOSITION. DURING THE PROCESS, ENCAPSULATION EFFICIENTY IS MAINTAINED
PREFERABLY AT OR ABOVE ABOUT 60%, MORE PREFERABLY ABOVE ABOUT 70% AND MOST
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PREFERABLY ABOVE ABOUT 75 TO 80%. ALSO, THE COOK TEMPERATURE FOR THE PROCESS
IS PREFERABLY MAINTAINED AT OR BELOW A MAXIMUM OF ABOUT 126.DEGREE. C.
72/1651
22. CA2020423 - 03.03.1992
PROCESS FOR TREATING AN AROMATIC PLANT OR HERB, OR A PLANT CONTAINING
ESSENTIAL OILS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CA2020423
Inventor(s):
BAIN JACQUES (FR); DARBONNE LUC (FR)
Applicant(s):
DAREGAL SA (FR)
IP Class 4 Digits: A23L
IP Class:
A23L1/22
E Class: A23B7/022; A23B7/08
Application Number:
US19900548232 (19900705)
Priority Number: FR19890008956 (19890704)
Family: CA2020423
Equivalent:
EP0407299; FR2649297; IE902419; PT94588
Abstract:
A PROCESS FOR TREATING AN AROMATIC PLANT OR HERB OR PLANTS CONTAINING
ESSENTIAL OILS COMPRISES A COMBINATION OF OPERATIONAL PHASES WHICH CONSIST OF
EFFECTING AN ENZYME BLOCKING OF THE HERB OR PLANT; OF A DEEP-FREEZING OF THE
PLANT OR HERB; OF AN IMPREGNATING THE HERB OR PLANT WITH THE PURPOSE OF
SEQUESTERING THE WATER AND FLAVORS WHICH ARE CONTAINED THEREIN; AND OF DRYING
AND DEHYDRATING THE HERB OR PLANT AT MODERATE TEMPERATURES.Description:
BACKGROUND OF THE INVENTION
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The invention relates to the treatment of aromatic plants or herbs, or of plants containing essential
oils (hereinafter named plants).
The plants to which the invention relates are, typically, parsley, chives, thyme, etc., or vegetables.
Spices and dry products are excluded therefrom.
Three main presentation methods are known for such plants: fresh, deep-frozen or dehydrated.
Presentation in the fresh state has the advantage of good organoleptic qualities, but the
disadvantage of a limited preservation period which may be inconvenient. Deep-freezing overcomes
this inconvenience, but involves implementing a costly cold chain which can present the risk of being
interrupted. Dehydrated presentation permits easy preservation for a long time, but the organoleptic
qualities of the plants presented in this manner are generally inferior to those obtained in the fresh
state. These organoleptic qualities consist mainly of texture, color, flavor or taste. To these there is
added functionality, that is to say the possibility of being utilized under the desired conditions.
It is therefore an aim of the invention to present plants such as aromatic plants or herbs, or plants
containing essential oils, in such a way that their organoleptic qualities are identical, or come very
close to, those of the fresh state and, at the same time, they can be preserved under conditions
comparable to those of the dehydrated state, taking into account the advantages which they present.
According to document U.S. Pat. No. 4,514,428, snacks in the form of apple slices are produced by
means of a succession of washing, anti-browning, sugar-impregnation and drying steps. Such a
process, which is very specific, does not allow aromatic plants or herbs, or plants containing
essential oils, to be treated for the object aimed at above.
Document U.S. Pat. No. 4,313,967 relates to a food product which is stable from the microbiological
point of view and which contains a fruit such as grape, date, plum, apricot, apple, peach, cherry or
lemon. This product has a water activity of between 0.008 and 0.93.
The document FOOD TECHNOLOGY, vol. 31, no. 4, April 1977, pages 58 to 64, relates to food
products of medium humidity and discloses the effects of various additives on the water content.
Documents U.S. Pat. No. 3,952,112, U.S. Pat. No. 4,832,969, U.S. Pat. No. 3,694,236, U.S. Pat. No.
4,361,589, GB-A-1,483,805 and U.S. Pat. No. 4,542,033 disclose the use of sorbitol or glycerol as a
humectant for grapes; the production of a dried green vegetable packaged in a black, sealed,
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oxygen-tight bag; the production of a dried food dehydrated by using Xanthomonas; the production
of dried celery by using sugar, followed by drying; and the treatment of whole dried fruits.
SUMMARY OF THE INVENTION
The abovementioned objects are achieved by the invention, namely processes for treating aromatic
plants or herbs, or plants containing essential oils, using combinations of operational phases which
consist of effecting an enzyme blocking of the herb or of the plant; of deep-freezing the herb or the
plant; of impregnating the herb or the plant with the purpose of sequestering the water and the
flavors which it contains; of drying and dehydrating the herb or the plant at a moderate temperature
up to the point where its water activity is lower than approximately 0.6, for a residual water content of
less than 20%.
Enzyme blocking is implemented by bringing the herb or the plant into contact with an aqueous
solution which is composed of additives (stabilizer, antioxidant, agent for reducing the water activity).
Deep-freezing of the herb or the plant is of the IQF (individual quick freezing) type. Sequestration of
the water and the flavors of the herb or the plant is achieved by bringing the latter into contact with
an aqueous solution containing additives (stabilizers, antioxidant, flavor retainer and taste enhancer).
The other characteristics of the invention will emerge from the description to follow.
DESCRIPTION OF THE PREFERRED EMBODIMENTS
The invention relates to treatment processes for aromatic plants or herbs, or plants containing
essential oils, (typically parsley, chives, thyme etc., or also vegetables, with the exception of spices
and dry products).
In principle, these processes have the aim of improving the organoleptic qualities of the herbs or
plants treated in this way and, in combination, permitting their preservation under conditions which
are comparable to those of the dehydrated state.
These processes use combinations of functional operational phases, that is to say, a phase in which
a fresh plant or herb which has recently been harvested is subjected to enzyme blocking (phase I), a
phase in which the herb or the plant is deep-frozen (phase II), a phase in which the water and the
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flavors of the plant are sequestered (phase III), and a phase in which the herb or the plant is dried
and dehydrated at a moderate temperature up to the point where its water activity WA is lower than
approximately 0.6, for a residual water content of less than 20% (phase IV).
The deep-freezing phase II is of the IQF (individual quick freezing) type.
In phases I and III, the herb or the plant is brought into contact with an aqueous solution which
comprises, principally, water and functional additives. This phase of bringing the herb or the plant
into contact with this solution is effected by immersion.
The aqueous solution used in phase I comprises at least 80% of water and, as additives:
At least one stabilizer selected from the group comprising sorbitol, a polyol such as mannitol, xylitol,
glycerol, a sugar such as sucrose, glucose, lactose, maltodextrin of 12.ltoreq.DE to less
than .ltoreq.30 or equivalent, in a proportion of between 5 and 10%.
At least one antioxidant selected from the group comprising ascorbic acid, sodium ascorbate,
alphatocopherol, butylhydroxyanisole, butylhydroxytoluene, sodium sulfite, sodium hydrogen sulfite,
sodium disulfite, potassium disulfite and calcium disulfite or equivalent, in a proportion of between
1.5% and 3%.
At least one agent which reduces the water activity selected from the group comprising calcium
chloride, sodium chloride, orthophosphoric acid, sodium lactate and calcium lactate or equivalent, in
a proportion of between 0.5% and 1%.
All the proportions given in the text are understood to be by weight and extend to those values which
are extreme but close to the limits indicated, around these limits. The lists of substances extend to
the functional equivalents.
The solution used in phase I has a dry-matter content of 7 to 8% approximately (measured by means
of a refractometer), and a pH of between 2.5 and 3.5 approximately (at 20 DEG C.).
The temperature of the aqueous solution used in phase I is between approximately 35 DEG C. and
55 DEG C. and, preferably, it is as close to 35 DEG C. as possible. The duration of the immersion of
the fresh herb or plant is of the order of a few minutes. For example, the durations of immersion can
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be 3, 4 or 6 minutes approximately, for solution temperatures of 55 DEG, 45 DEG and 35 DEG C.,
respectively.
The solution used in phase III comprises at least 60% of water and, as additives:
At least one stabilizer selected from the group comprising sorbitol, a polyol such as mannitol, xylitol,
glycerol, a sugar such as sucrose, glucose, lactose, maltodextrin of 12.ltoreq.DE to less
than .ltoreq.30 or equivalent, in a proportion of between 20 and 40%.
At least one antioxidant selected from the group comprising ascorbic acid, sodium ascorbate,
alphatocopherol, butylhydroxyanisole, butylhydroxytoluene, sodium sulfite, sodium hydrogen sulfite,
sodium disulfite, potassium disulfite and calcium disulfite or equivalent, in a proportion of between
0.20% and 0.45%.
At least one flavor retainer selected from the group comprising gum arabic, carboxymethylcellulose,
modified starch, ethylmaltol or equivalent, in a proportion of between 0.9% and 1.8%.
At least one taste enhancer such as monosodium glutamate or equivalent, in a proportion of between
1 and 2% approximately.
This solution has a dry-matter content (measured by means of a refractometer) of between 25 and
40% approximately. Its pH is between 4.5 and 6.5 approximately (at 20 DEG C.). Its use temperature
is between 10 DEG C. and 50 DEG C. It is preferably equal to, or close to, 20 DEG to 30 DEG C. The
duration of immersion is inversely proportional to the temperature. It is between 15 and 50 min
approximately and, preferably, between 30 and 40 min approximately.
In phase III, the durations of immersion can be as follows, as a function of the temperature of the
solution:
Temperature: 10, 15, 20, 25, 30, 35, 40, 45, 50
Immersion time in minutes: 50, 45, 40, 35, 30, 25, 21, 17, 15.
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Phase I follows an initial state, using a fresh herb or plant which has been harvested recently. This
phase is followed by an intermediate phase in which the herb or the plant is drained once the latter
has been immersed into an aqueous solution of phase I.
Phase III is carried out with agitation. Deep-freezing of the herb or the plant by the IQF method
permits the herb or the plant to be in the divided state.
Phase III is followed by an intermediate sieving phase which allows the herb or the plant to be
separated from the aqueous solution of phase III.
The dehydration and drying phase IV is carried out at a temperature of the herb or the plant during
drying of between 50 DEG and 65 DEG C. approximately. This phase IV allows an appropriate
amount of water to be eliminated by dehydration so that a water activity (WA) of between 0.3 and 0.6
approximately is achieved for a residual water content of 10 to 20% approximately.
Excellent results were obtained by using, in phase I, sorbitol, ascorbic acid and calcium chloride in
the following percentages: 6%, 1.5% and 0.5%, which are added to 92% of water. And, in phase III,
by using sorbitol, gum arabic, monosodium glutamate and ascorbic acid in the following
percentages: 27%, 1.26%, 1.44% and 0.3%.
As regards the aqueous solution of phase III, several tests were carried out which gave excellent
results. These tests emerge from the following table (the values are given in %):
______________________________________
Concentration 25 30 35 40
Water
75 70 65 60
Sorbitol
22.5 27 31.5 36
Gum arabic 1.05 1.26 1.47 1.68
Monosodium glutamate
1.2 1.44 1.68 1.92
Ascorbic acid 0.25 0.3 0.35 0.4
______________________________________
The proportion of treated herb or plant in phase III depends on the concentration of the solution used
in this phase, as well as on the state of the herb or plant (fresh or deep-frozen state). This ratio of
quantity of treated herb or plant to concentration of solution used is generally linear and increasing.
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For the extreme values contemplated, as regards the concentration, i.e. 25% and 40%, the
percentages of the products to be treated are:
in the fresh state, 8 and 13
in the deep-frozen state, 10 and 18.
These figures are indicative.
In a first possible variant, phases I and II are combined with theintermediate draining phase. This
permits the aromatic plants or herbs, or the plants containing essential oils, to be obtained deepfrozen, starting from fresh herbs or plants with improved organoleptic qualities.
In a second possible variant, phase I is combined with a conventional dehydration phase and, in an
intermediate manner, a draining phase. This permits dehydrated aromatic plants or herbs, or
dehydrated plants containing essential oils, to be obtained which likewise have improved
organoleptic qualities.
In a third variant, phase II, phase III and phase IV are combined, with the abovementioned sieving
between phases II and III. This permits dried herbs or plants of medium moisture content to be
obtained. One either starts with herbs or plants which are already deep-frozen, in which case the
initial phase I cannot be effected, or one starts with fresh herbs or plants, and the initial phase I is
effected. In both variants, a herb or plant is obtained which, in comparison with a conventionally
dehydrated product, restores the qualities of a fresh herb or plant upon rehydration, in particular as
regards the color and the flavor. Moreover, the rehydration is virtually instantaneous. To illustrate the
effects obtained by implementing the invention, it can be said that the rehydration rate A (=Pm/Po
where Po=10 g) at 60 DEG C. is of the order of 6 for herbs treated in accordance with the third
variant as against of the order of only 3.5 for conventionally dehydrated herbs.
Claims:
We claim:
1. A process for treating an aromatic plant or herb, or a plant containing essential oils, which
comprises: providing a fresh herb or plant which has been harvested recently; and immersing this
herb or plant in an aqueous solution which comprises at least 80% by weight of water and has
additives including: at least one stabilizer selected from the group comprising sorbitol, a polyol such
as mannitol, xylitol, glycerol, a sugar such as sucrose, glucose, lactose, maltodextrin of
12.ltoreq.DE.ltoreq.30 or equivalent, in a proportion by weight of between 5% and 10%
79/1651
approximately; at least one antioxidant selected from the group comprising ascorbic acid, sodium
ascorbate, alphatocopherol, butylhydroxyanisole, butylhydroxytoluene, sodium sulfite, sodium
hydrogen sulfite, sodium disulfite, potassium disulfite and calcium sulfite, or equivalent, in a
proportion by weight of between 1.5% and 3% approximately; at least one agent which reduces the
water activity selected from the group comprising calcium chloride, sodium chloride,
orthophosphoric acid, sodium lactate and calcium lactate or equivalent, in a proportion by weight of
between 0.5% and 1% approximately; this solution having a dry-matter content of 7 to 8%
approximately, a pH at 20 DEG C. of between 2.5 and 3.5 approximately, a temperature between
approximately 35 DEG C. and 55 DEG C. and, preferably, as close to 35 DEG C. as possible, the
immersion duration being of the order of several minutes.
2. A process for treating an aromatic plant or herb, or a plant containing essential oils, which
comprises: providing a fresh herb or plant which has been harvested recently; immersing this herb or
plant in an aqueous solution which comprises at least 80% by weight of water and has additives
including: at least one stabilizer selected from the group comprising sorbitol, a polyol such as
mannitol, xylitol, glycerol, a sugar such as sucrose, glucose, lactose, maltodextrin of
12.ltoreq.DE.ltoreq.30 or equivalent, in a proportion by weight of between 5% and 10%
approximately: at least one antioxidant selected from the group comprising ascorbic acid, sodium
ascorbate, alphatocopherol, butylhydroxyanisole, butylhydroxytoluene, sodium sulfite, sodium
hydrogen sulfite, sodium disulfite, potassium disulfite and calcium sulfite or equivalent, in a
proportion by weight of between 1.5% and 3% approximately; at least one agent which reduces the
water activity selected from the group comprising calcium chloride, sodium chloride,
orthophosphoric acid, sodium lactate and calcium lactate or equivalent, in a proportion by weight of
between 0.5% and 1% approximately; this solution having a dry-matter content of 7 to 8%
approximately, a pH at 20 DEG C. of between 2.5 and 3.5 approximately, a temperature between
approximately 35 DEG C. and 55 DEG C. and, preferably, as close to 35 DEG C. as possible, the
immersion duration being of the order of several minutes; draining the herb or the plant after
immersion; and deep-freezing the herb or plant which has been drained in this way.
3. The process as claimed in claim 2, wherein the herb or the plant is deep-frozen in accordance
with the IQF "Individual Quick Freezing" process.
4. A process for treating an aromatic plant or herb, or a plant containing essential oils, which
comprises: providing a fresh herb or plant which has been harvested recently; immersing this herb or
plant in an aqueous solution which comprises at least 80% by weight of water and has additives
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including: at least one stabilizer selected from the group comprising sorbitol, a polyol such as
mannitol, xylitol, glycerol, a sugar such as sucrose, glucose, lactose, maltodextrin of
12.ltoreq.DE.ltoreq.30 or equivalent, in a proportion by weight of between 5% and 10%
approximately; at least one antioxidant selected from the group comprising ascorbic acid, sodium
ascorbate, alphatocopherol, butylhydroxyanisole, butylhydroxytoluene, sodium sulfite, sodium
hydrogen sulfite, sodium disulfite, potassium disulfite and calcium sulfite, in a proportion by weight of
between 1.5% and 3% approximately or equivalent; at least one agent which reduces the water
activity selected from the group comprising calcium chloride, sodium chloride, orthophosphoric acid,
sodium lactate and calcium lactate or equivalent, in a proportion by weight of between 0.5% and 1%
approximately; this solution having a dry-matter content of 7 to 8% approximately, a pH at 20 DEG C.
of between 2.5 and 3.5 approximately, a temperature between approximately 35 DEG C. and 55
DEG C. and, preferably, as close to 35 DEG C. as possible, the immersion duration being of the
order of several minutes; draining the herb or the plant after immersion; and deep-freezing the herb
or plant which has been drained in this way.
5. A process for treating an aromatic plant or herb, or a plant containing essential oils, which
comprises: providing a deep-frozen herb or plant; immersing this herb or plant, which has been
deep-frozen in this way, with agitation, in an aqueous solution comprising at least 60% by weight of
water and with additives including: at least one stabilizer selected from the group comprising sorbitol,
a polyol such as mannitol, xylitol, glycerol, a sugar such as sucrose, glucose, lactose, maltodextrin of
12.ltoreq.DE.ltoreq.30 or equivalent, in a proportion by weight of between 15% and 40%
approximately; at least one antioxidant selected from the group comprising ascorbic acid, sodium
ascorbate, alphatocopherol, butylhydroxyanisole, butylhydroxytoluene, sodium sulfite, sodium
hydrogen sulfite, sodium disulfite, potassium disulfite and calcium sulfite or equivalents, in a
proportion by weight of between 0.15% and 0.5% approximately; at least one flavor retainer selected
from the group comprising gum arabic, carboxymethylcellulose, modified starch, ethyl maltol or
equivalents, in a proportion by weight of between 0.9% and 1.8% approximately; at least one taste
enhancer such as monosodium glutamate or equivalent, in a proportion by weight of between 1%
and 2% approximately; this solution having a dry-matter content of 25 to 40% approximately, a pH at
20 DEG C. of between 4.5 and 6.5 approximately, a temperature of between 10 DEG C. and 50 DEG
C. and, preferably, equal to, or close to, 20 DEG to 30 DEG C. approximately, the duration of
immersion, which is inversely proportional to the temperature, being between 15 and 50 minutes
approximately, and preferably between 30 and 40 minutes approximately; sieving the herb or the
plant after immersion; and dehydrating the herb or the plant, which has been sieved in this way.
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6. A process for treating an aromatic plant or herb, or a plant containing essential oils, which
comprises: providing a deep-frozen herb or plant; immersing this herb or plant, which has been
deep-frozen in this way, with agitation, in an aqueous solution comprising at least 60% by weight of
water and with additives including: at least one stabilizer selected from the group comprising sorbitol,
a polyol such as mannitol, xylitol, glycerol, a sugar such as sucrose, glucose, lactose, maltodextrin of
12.ltoreq.DE.ltoreq.30 or equivalent, in a proportion by weight of between 20% and 40%
approximately; at least one antioxidant selected from the group comprising ascorbic acid, sodium
ascorbate, alphatocopherol, butylhydroxyanisole, butylhydroxytoluene, sodium sulfite, sodium
hydrogen sulfite, sodium disulfite, potassium disulfite and calcium sulfite or equivalents, in a
proportion by weight of between 0.2% and 0.45% approximately; at least one flavor retainer selected
from the group comprising gum arabic, carboxymethylcellulose, modified starch, ethyl maltol or
equivalents, in a proportion by weight of between 0.9% and 1.8% approximately; at least one taste
enhancer such as monosodium glutamate or equivalent, in a proportion by weight of between 1%
and 2% approximately; this solution having a dry-matter content of 25 to 40% approximately, a pH at
20 DEG C. of between 4.5 and 6.5 approximately, a temperature of between 10 DEG C. and 50 DEG
C. and, preferably, equal to, or close to, 20 DEG to 30 DEG C. approximately, the duration of
immersion, which is inversely proportional to the temperature, being between 15 and 50 minutes
approximately, and preferably between 30 and 40 minutes approximately; sieving the herb or the
plant after immersion; and drying the herb or plant which has been sieved in this way at a
temperature of between approximately 50 DEG C. and 65 DEG C. up to the point where its water
activity is of the order of 0.3 to 0.6, for a residual water content of the order of 10 to 20%, so as to
obtain a dried herb or plant which rehydrates rapidly and which has improved organoleptic qualities.
7. A process for treating an aromatic plant or herb, or a plant containing essential oils, which
comprises: providing a fresh herb or plant which has been harvested recently; immersing this herb or
plant in an aqueous solution of water and with additives including: at least one stabilizer such as
sorbitol or equivalent, in a proportion by weight of less than 10% approximately; at least one
antioxidant; at least one agent which reduces water activity, such as calcium chloride or equivalent;
this solution having a dry-matter content of 7 to 8% approximately, a pH at 20 DEG C. of between 2.5
and 3.5 approximately, a temperature between approximately 30 DEG C. and 60 DEG C. and,
preferably, as close to 30 DEG C. as possible, the duration of immersion being of the order of several
minutes; draining the herb or the plant after immersion; and deep-freezing the herb or the plant
which has been drained in this way; immersing the herb or plant which has been deep-frozen in this
way in an aqueous solution comprising water with additives including: at least one stabilizer such as
sorbitol or equivalent; at least one antioxidant; at least one flavor retainer such as gum arabic or
82/1651
equivalent; at least one taste enhancer such as monosodium glutamate or equivalent; this solution
having a dry-matter content of 25 to 40% approximately, a pH at 20 DEG C. of between 4.5 and 6.5
approximately, a temperature of between approximately 10 DEG C. and 50 DEG C. and, preferably,
equal to, or close to, 20 DEG to 30 DEG C. approximately, the duration of immersion, which is
inversely proportional to the temperature, being between 15 and 50 minutes approximately, and,
preferably, between 30 and 40 minutes approximately; sieving the herb or the plant after immersion;
and drying the herb or plant which has been sieved in this way at a temperature of between
approximately 50 DEG C. and 65 DEG C. up to the point where its water activity is of the order of 0.3
to 0.6, for a residual water content of the order of 10 to 20%, so as to obtain a dried herb or plant
which rehydrates rapidly and which has improved organoleptic qualities.
8. A process for treating an aromatic plant or herb, or a plant containing essential oils, which
comprises: providing a fresh herb or plant which has been harvested recently; immersing this herb or
plant in an aqueous solution which comprises at least 80% by weight of water and has additives
including: at least one stabilizer selected from the group comprising sorbitol, a polyol such as
mannitol, xylitol, glycerol, a sugar such as sucrose, glucose, lactose, maltodextrin of
12.ltoreq.DE.ltoreq.30 or equivalent, in a proportion by weight of between 5% and 10%
approximately; at least one antioxidant selected from the group comprising ascorbic acid, sodium
ascorbate, alphatocopherol, butylhydroxyanisole, butylhydroxytoluene, sodium sulfite, sodium
hydrogen sulfite, sodium disulfite, potassium disulfite and calcium sulfite or equivalent, in a
proportion by weight of between 1.5% and 3% approximately; at least one agent which reduces the
water activity selected from the group comprising calcium chloride, sodium chloride,
orthophosphoric acid, sodium lactate and calcium lactate or equivalent, in a proportion by weight of
between 0.5% and 1% approximately; this solution having a dry-matter content of 7 to 8%
approximately, a pH at 20 DEG C. of between 2.5 and 3.5 approximately, a temperature between
approximately 35 DEG C. and 55 DEG C. and, preferably, as close to 35 DEG C. as possible, the
immersion duration being of the order of several minutes; draining the herb or the plant after
immersion; deep-freezing the herb or plant, which has been drained in this way; immersing this herb
or plant, which has been deep-frozen in this way, with agitation, in an aqueous solution comprising at
least 60% by weight of water and having additives including: at least one stabilizer selected from the
group comprising sorbitol, a polyol such as mannitol, xylitol, glycerol, a sugar such as sucrose,
glucose, lactose, maltodextrin of 12.ltoreq.DE.ltoreq.30 or equivalent, in a proportion by weight of
between 15% and 40% approximately; at least one antioxidant selected from the group comprising
ascorbic acid, sodium ascorbate, alphatocopherol, butylhydroxyanisole, butylhydroxytoluene,
sodium sulfite, sodium hydrogen sulfite, sodium disulfite, potassium disulfite and calcium sulfite or
83/1651
equivalent, in a proportion by weight of between 0.15% and 0.5% approximately; at least one flavor
retainer selected from the group comprising gum arabic, carboxymethylcellulose, modified starch or
equivalent, ethyl maltol, in a proportion by weight of between 0.9% and 1.8% approximately; at least
one taste enhancer such as monosodium glutamate or equivalent, in a proportion by weight of
between 1% and 2% approximately; this solution having a dry-matter content of 25 to 40%
approximately, a pH at 20 DEG C. of between 4.5 and 6.5 approximately, a temperature of between
10 DEG C. and 50 DEG C. and, preferably, equal to, or close to, 20 DEG to 30 DEG C. approximately,
the duration of immersion, which is inversely proportional to the temperature, being 15 and 50
minutes approximately, and preferably between 30 and 40 minutes approximately; sieving the herb
or the plant after its immersion; and drying the herb or plant which has been sieved in this way at a
temperature of between approximately 50% and 65% up to the point where its water activity is of the
order of 0.3 to 0.6, for a residual water content of the order of 10 to 20%, so as to obtain a dried herb
or plant which can be rehydrated rapidly and has improved organoleptic qualities.
9. The process as claimed in claim 8, wherein the herb or the plant isdeep-frozen in accordance with
the IQF "Individual Quick Freezing" process.
10. A process for treating an aromatic plant or herb, or a plant containing essential oils, which
comprises: providing a fresh herb or plant which has been harvested recently; bringing the herb or
plant into contact with an aqueous solution with additives capable of effecting the enzyme blocking
thereof; deep-freezing the herb or plant; bringing the herb or plant in the deep-frozen state into
contact with an aqueous solution with additives capable of effecting the impregnation of the
defrosted herb or plant with the purpose of sequestering the water and the flavors which it contains;
drying and dehydrating the herb or plant at a moderate temperature up to the point where its water
activity is lower than 0.6 approximately, for a residual water content of less than 20%.
84/1651
23. CA919498 - 23.01.1973
ESSENTIAL OIL EMULSIONS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CA919498
Inventor(s):
NOZNICK P P (US); TATTER C W (US)
Applicant(s):
BEATRICE FOODS CO (US)
Application Number:
CA19690063612 (19690929)
Priority Number: CA19690063612 (19690929); CA19650948974 (19651230)
Family: CA919498
85/1651
24. CA993361 - 12.11.1975
TOOTHPASTES
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CA993361
Applicant(s):
COLGATE PALMOLIVE CO (--)
IP Class 4 Digits: A61K
IP Class:
A61K7/16
E Class: A61K7/16B
Application Number:
GB19730044632 (19730924)
Priority Number: US19720295068 (19721004)
Family: CA993361
Equivalent:
AR198878; AU6043973; BE805562; CH593062; DE2348351; FR2201864; HK14981;
JP49132250; PH11033; ZA7307239
Abstract:
1413642 TOOTHPASTES COLGATE-PALM- OLIVE CO 24 SEPT 1973 [4 OCT 1972] 44632/73
HEADING A5B A TOOTHPASTE CONTAINS FROM 20 TO 60% BY WEIGHT OF ABRASIVE
PARTICLES, PREDOMINANTLY SODIUM BICARBONATE, IN A WATER-GLYCEROL VEHICLE, THE
WATER:GLYCEROL RATIO BEING IN THE RANGE FROM 0.4:1 TO 0.7:1; AND FROM 0.5 TO 1.5%
BY WEIGHT OF AN ESSENTIAL OIL FLAVOURING AGENT.Description:
(54) TOOTHPASTES
(71) We, COLGATF-PALMOLIVE
COMPANY, a Corporation organised under the Laws of the State of Delaware, United
86/1651
States of America, of 300 Park Avenue, New
York, New York 10(r22, United States of
America, do hereby declare the invention for which we pray that a patent may be granted to us, and
the method by which it is to be performed, to be particularly described in and by the following
statement:
This invention relates to toothpastes containing dispersed particles of baking soda (sodium
bicarbonate).
Baking soda has been proposed for use in dentifrices, particularly tooth powders, but such
dentifrices generally have not been well accepted by consumers. The typical dentifrices which have
shown significant consumer acceptance in recent years are toothpastes having a high content of
water-insoluble abrasives such as dicalciuim phosphate or other insoluble phosphates in an
aqueous humectant base.
Several factors have to be taken into account in the development of a practical and effective baking
soda toothpaste likely to be acceptable to consumers. Among these factors are the distinctive
character of baking soda chemically, physically and cosmetically when employed as a toothpaste
ingredient. For example, it is comparatively water-soluble and tends to release carbon dioxide in an
aqueous system, and it has a salty taste. Other factors include the cleaning and polishing power of
the toothpaste, its stability and appearance and the care needed in manufacture.
According to the invention a toothpaste contains from 20 to 60% of abrasive particles, predominantly
sodium bicarbonate, in a waterglycerol vehicle, the water: glycerol ratio being in the range from 0.4:1
to 0.7:1; and from 0.5 to 1.5% of an essential oil flavouring agent.
The above-quoted percentages, and all other proportions specified herein, are by weight based on
the complete toothpaste unless otherwise indicated.
Such a toothpaste is effective in promoting hygiene in the oral cavity. It has acceptable cleaning,
polishing and other desirable characteristics affording a beneficial effect upon parts of the dentition
(which may include the teeth and its surrounding or adjacent elements or structures including plaque,
calculus, gingiva, mucous membranes and saliva). In particular, it tends to leave with the consumer a
desirable sensation of a clean mouth. The toothpaste can be formulated sol that it is stable upon
aging or storage without significant release of carbon dioxide, bubbles or other forms of undesirable
separation or reaction.
87/1651
It is possible to produce and maintain a distinctive granular texture appearance comprising a
substantially dispersed non-crystallineappearing granulate which is due in part to the substantially
homogeneous distribution of a sufficiently high concentration of macroscopic crystalline bicarbonate
particles in an otheruvise smooth, continuous base or matrix, contributing to the appearance, taste
and acceptance by the consumer.
The toothpastes of this invention preferably contain at least 25%, more preferably at least 35%, of
sodium bicarbonate. The sodium bicarbonate is preferably the principle abrasive, by weight The
particle size of the sodium bicarbonate particles may vary; it is preferred that they be largely below
0.4 mm in diameter, with a major proportion by weight being above 0.01 mm in diameter, e.g.
the particles being predominantly of above 150 microns but below 0.4 mm in diameter.
The vehicle in which the sodium. bicarbonate particles are dispersed is preferably aqueous, but its
amount and character are preferably such that the sodium bicarbonate is primarily in the
undissolved solid state in the toothpaste. However, when the teeth are brushed the sodium
bicarbonate particles will tend to dissolve in the saliva.
Although sodium bicarbonate particles are relatively soft as compared to most conventional
abrasive particles used in toothpastes they do exert a mechanical cleaning effect on the teeth. For
instance, in a radioactive dentin abrasion (RDA) test a toothpaste containing about 505/, of sodium
bicarbonate, as the sole abrasive, may show an RDA value of about
100 whereas when the abrasive-free vehicle of that tooth-paste is tested similarly the RDA value is
only in the neighbourhood of 50
Known toothpastes containing relatively high proportion of sodium bicarbonate tend to have too
salty a taste. This may possibly be due to the dissoloution of part of the sodium
bicarbonate in the water-glycol vehicle in
which water-glycerol ratio is about 2: 1.When,
however, this ratio is lowered to about 0.8:1 with a view to reducing the amount of dis
solved sodium bicarbonate, the toothpaste be
comes unstable on an aging at elevated tem
peratures (e.g. 1 100F and 1200F). Thus, in aging tests of such toothpastes the oily flavour
components (e.g. peppermint oil) incorpor
ated in the dentifrice show an increased tend
88/1651
ency to separate from the rest of the denti
frice; such separation has an adverse affect
on appearance and flavour. Surprisingly, it
has been found that when the ratio is decreased
still further, this separating tendency is
markedly reduced while, at the same time, the toothpaste has a desirably less salty taste.
For some reason, unknown to applicants,
the above-noted tendency to flavour oil separa
tion is particularly marked when the sodium bicarbonate particles in the dental cream are
of relatively large size, e.g. having particle
diameters principally above 150 or 200 microns.
Other abrasives may also be present in addition to the sodium bicarbonate. Examples are
finely divided silica, which may be crystal
line or amorphous, (e.g. micronized crystalline
silica or silica gel, such as the silica gels sold as "Syloid 63", "Syloid 74" and "Syloid 244" -Syloid is
a trade mark); alumina, such as hydrated alumina or alpha-alumina; zirconium
silicate; and amorphous or crystalline aluminosilicates. A particularly suitable compatible additional
abrasive is calcium carbonate. The amount of additional abrasive is generally less than the amount of
sodium bicarbonate, e.g. in the range from 5 to 25% of the toothpaste.
Attention is drawn to our co-pending British
Patent Application No. 44631/73 (Serial No.
1,413,641j which claims toothpaste containing abrasives comprising a major proportion of sodium
bicarbonate and a minor proportion of water-insoluble dental abrasive material compatible with the
bicarbonate.
Th toothpastes may also contain a small amount of titanium dioxide powder, which has been found
to have a marked polishing effect on the teeth when used in the sodium bicarbonate toothpaste. The
weight of tianium dioxide particles in the toothpaste is generally only a small fraction, e.g. less than
one tenth, of the weight of sodium bicarbonate, but is generally above 0.1% of the weight of the
toothpaste. For instance, the amount of titanium dioxide may be in the range from 0.2 to 0.6^ of the
89/1651
weight of the toothpaste. The particle size of the titanium dioxide is preferably below 1 micron, e.g.
0.05 to 0.8 micron.Attention is drawn to our co-pending
British Patent Application No. 44633/73
(Serial No. 1,413,643) which claims toothpaste containing a proportion of dispersed particles of
sodium bicarbonate and a smaller proportion of dispersed particles of titanium dioxide.
Examples of suitable flavouring oils, which are water-insoluble, are oils of spearmint, peppermint,
wintergreen, sassafras, clove, sage, eucalyptus, marjoram, cinnamon, lemon and orange, as well as
methylsalicylate. Preferably the amount of flavouring oil is above 0.5 , and below 2C.' e.g. 0.8 to 1.2
'E, such as 0.9 or 1.0 уThe water-glycerol vehicle preferably con
tains a thickening agent (e.g. a gelling agent).
Gelling agents for toothpaste vehicles are well known in the art. These are often high polymers (e.g.
gums or other thickening
agents) which are soluble or swellable in water or other aqueous medium. Sodium carb
oxynethylcellulose has given excellent results.
Other materials are gum tragacanth, gum arabic, gum karaya, sodium alginate, hydroxy
ethyl cellulose, methyl cellulose, ethyl cellulose, carrageen and other polysaccharides, polyvinyl
pyrrolidones or such thickening agents as "Veegum" (a complex magnesium aluminium silicate). The
amount of thickening agent used is preferably sufficient to impart to the mixture the pasty
consistency, body, and the non-tacky nature which are characteristic of conventional
toothpastes.Usually, toothpastes are extrudable from ordinary collapsible toothpaste tubes to form a
ribbon of substantial thickness (e.g. about 3/8 inch) which, if left undisturbed, substantially retains its
original thickness over a period of, say, one minute or more (and does not penetrate substantially into
the bristles of a toothbrush when resting on the ends of such bristles for a similar period); but which
preferably offers no substantial resistance to brushing or to deformation when, for instance, one
touches it lightly with a finger; and which has little tack, in that it does not tend to form a string when
the finger is pulled away from the ribbon.
The proportion of thickening agent is often in the range from 0.5 to 20 such as from 0.8 to 1.5 ., of
the toothpaste.
90/1651
An organic surface active agent is preferably used in the toothpastes of the present in vention to aid
in the propylactic action and in the thorough dispersion of the composition throughout the oral cavity,
and to improve consumer acceptability and detersive and foaming properties. Among the suitable
surface-active agents are water-soluble salts of alkyl sulphates, such as sodium laurvl sulphate or
other suitable alkyl sulphates having
S to 1S carbon atoms in the alkyl group; water-soluble salts of sulphonated mone glycerides of fatty
acids such as sodium coconut monoglycerides sulphonate or other suitable sulphonated
monoglycerides of a fatty acid of 10 to 18 carbon atoms; salts of amides of fatty acids (e.g. 12 to 16
carbon atom acids) with lower aliphatic amino acids (e.g.
taurine or sarcosine) or other amino acids of 2 to 6 carbon atoms, such as sodium-N- methyl-Npalmitoyl tauride, sodium Nlauroyl-, N-myristoyl- or N-palmitoylsarcosinates; water-soluble salts of the
esters of such fatty acids with isethionic acid or with glycerol monosulphate, such as the sodium salt
of the monosulphated monoglyceride of hydrogenated coconut oil fatty acids; watersoluble salts of
olefin sulphonates, e.g. alkene sulphonates or hydroxyalkane sulphonates or mixtures thereof having
12 to 18 carbon atoms in the carbon chain of the molecule; and water-soluble soaps of fatty acids of
12 to 18 carbon atoms, e.g. coconut fatty adds. The cation of the salt may be, for instance, sodium
(which is preferred) potassium or mono-, di-, or triethanolamine. Mixtures of surface-active agents
may be used.A particularly suitable mixture which provides a high foaming powder with little or no
irritating effect is a C,-C,8 alkyl sulphate and a C12Cts fatty acid sarcosinate, e.g. in a ratio of from
1:2 to 2:1, such as about 1: 1, instead of all or part of the sarcosinate, a C1oC18 fatty acid
monoglyceride sulphonate may be present
Other suitable surface-active materials in dude nonionic agents such as condensates of serbian
monostearate with approximately 60 moles of ethylene oxide, condensates of ethylene oxide with
propylene oxide, condensates of propylene glycol (available under the traoemail "Pluronics") and
amphoteric agents such as quaternized imidazole derivatives which are available under the
trademark sCI4'lir?nol" such as "Mironal C2M". Cationic sufface-actisre germicides and antibacterial compounds may also be used.Such compounds include di-isobutyl-phenoxyethoxethyl dim
ethyl benzyl ammonium chloride, benzyl dimethyl stearyl ammonium chloride, tertiary aglines
having one fatty alkyl group (of from 12 to 18 carbon atoms) and two (poly) oxyethylene groups
attached to the nitrogen (typically containing a total of from about 2 to about 50 ethenoxy groups per
molecule) and salts thereof with acids, and compounds of the structure:
wherein R is a fatty alkyl group containing from 12 to 18 carbon atoms, and x, y and z total 3 or
higher, as well as salts thereof with mineral or organic acids.
91/1651
The proportion of surface-active agent is preferably in the range from 0.05 to 5 У of the toothpaste,
more preferably in the range from 1 to 3 %, such as from 1.5 to 2%.
Cationic antibacterial agents may be included in the toothpastes. Such agents include:
N1 - (4 - chlorobenzyl) - N5 - (2,4 - di chlorobenzyl) biguanide;
p-chlorophenyl biguanide;
4-chlorobenzyhydryl biguanide;
4-chlorobenzhydrylguanylurea; N - 3 - lauropropyl - N5 - p - chlorobenzyl - biguanide;
1 - (lauryldimethylammonium) -8-(p- chlorobenzyldimethylammonium) octane dichloride;
5,6-dichloro-2-guanidinobenzimidazole;
N1-p-chlorophenyl-N5-laurylbiguanide; 5 - amino -1,3 - bis (2 - ethylhexyl) - 5 methylhexahydropyrimidine cetyl pyridinium chloride; and their non-toxic acid addition salts,
particularly the fluorides and the dihydrogen fluorides. 1;6-di- (p-chlorophenylbiguanido) hexane is
particularly preferred.These agents may be used in amounts in the range from: 0.01 to 5%.
A sweetening agent may be present Suitable sweetening agents include lactose, maltose, sorbitol,
perillartine, saccharine and ammoniated glycyrrhizin (e.g. its monoammonium salt). At present it is
preferred to use a non-cariogenic type of sweetening agent such as saccharine, e.g. in an amount of
0.1 to 0.2%.
The toothpastes may also contain a fluoridecontaining anticaries agent. There are many watersoluble inorganic salts which are suitable sources of fluoride ions. Among these are sodium,
potassium, ammonium, lithium and amine fluorides. The monofluorophosphate salts are also useful
and include those having the formulae Na4P30flF, K4P,OF, (NEI+)4PsOoKn
Na,KP,OaK, (NH4)NaPsO.JF and Li4P,O5F.
Complex water-soluble fluoride-containing salts such as fluorosilicates (e.g. Na2SiFG),
fluorozirconates (e.g. Na1ZrF), fluorostannites (e.g. KSnFs), fluoroborates (e.g.
NaBF4), fluorotitanates (e.g. NaTiF), and fluorogermanates (e.g. K2GeFG) may also be useful. The
fluoride ion may also be supplied by an organic fluoride which yields fluoride ions in water. Suitable
organic compounds include mono-, di-, and triethanolamine hydrofluorides. These materials may be
present in an effective but non-toxic amount, usually in the range to provide from 0.01 to 1% by
92/1651
weight of the water-soluble fluorine content thereof to the toothpaste Sodium fluoride and sodium
monofluorophosphate are the preferred compounds.
Various other materials may be incorporated into the toothpastes. Examples thereof are colouring
and whitening agents, preservatives, silicones, chlorophyll compounds and mixtures thereof. These
adjuvants are incorporated in the toothpastes in amounts which do not substantially adversely affect
the properties and characteristics desired.
The following Examples illustrate the invention.
Example 1
A toothpaste is prepared by forming a gel by mixing a gelling agent, in this case sodium
catboxymethycellulose ("CMC"), with glycerol and water (in the presence of a sweetener, namely
sodium saccharin, and a preservative, namely sodium benzoate), adding sodium bicarbonate
(baking soda), chalk, and titanium dioxide powder to the gel, then adding a surfactant and
peppermint flavour (rich in peppermint oil) and thereafter degassing the mixture under vacuum.The
proportions used are: 40 У baking soda, 53 chalk, 0.4O. titanium dioxide, 15.4 у water, 33.5%
glycerol, 1 l) sodium lauryl sulphate, 2 , of a solution of 35% sodium N-lauroyl sarcosinate in a
mixture of 35 ; water and 30":t glycerol, 1.1% CMC, 0.9 ' waterinsoluble flavour, 0.5 у sodium
beuzoate and 0.2 у sodium saccharin.
The baking soda power is U.S.P. grade having the following particle size distribution in which
percentages represent the cumulative per cent retained on the named sieve, and sieve sizes are U.S.
Standard: No. 45 sieve (sieve opening 350 microns), trace; No. 70 sieve (sieve opening 310 microns),
27 ,; No.
80 sieve (sieve opening 177 microns), 66.5%
No. 100 sieve (sieve opening 149 microns), 92.5% No. 170 sieve (sieve opening 88 microns), 99 jУ.
The chalk is a grit-free U.S.P. Non Fer
Al Chalk containing at least 98 у CACAO, with no more than 0.2 insoluble in dilute HCl. Its particle
size is such that over 99 У passes through a U.S. Standard No. 325 sieve (sieve opening 44
microns), the particles being principally in the 1 to 10 microns size, the average particle size being
about 3 microns.
93/1651
The titanium dioxide used is a grit-free anatase powder at least 99.0% of which passes through a No.
325 U.S. Standard sieve and whose mean particle diameter (as measured on a Kahn sedimentation
balance) is below 1 micron. Microscopic measurements indicate its average particle diameter is 0.3
micron.
Example 2
Example 1 is repeated except that the proportion of baking soda is increased to 41 v,) the
proportion of glycerol is correspondingly reduced to 32.5% and a smaller particle size baking soda is
used.
The baking soda powder is U.S.P. grade having the following particle size distribution (in which
percentages represent the cumulative percent retained on the named sieve, and sieve sizes are U.S.
Standard); No. 45 sieve (sieve opening 350 microns), trace; No. 100 sieve (sieve opening 149
microns), 0.53$;
No. 170 sieve (sieve opening 88 microns), 200.,; No. 200 sieve (sieve opening 74 microns), 353"';
No. 325 sieve (sieve opening 44 microns), 70; No. 400 sieve, 80%
Example 3
Example 1 is repeated except that the proportion of chalk is increased to 103$ and the proportion of
baking soda is lowered to 35 ei.
Example 4
Example 1 is repeated except that the proportion of glycerol is increased to 37.5 sO the proportion
of water is reduced to 10.4 у and the amount of baking soda is 41C .
Example 5
Example 1 is repeated except that the proportion of glycerol is increased to 43.49, the proportion of
water is reduced to 10.4 , and the amount of baking soda is 35%.
The baking soda used in the Examples is a product made by precipitation from solution
(as by treating a sodium carbonate solution with carbon dioxide to precipitate the bicarbonate)
followed by drying, curing with carbon dioxide gas and screening to the desired particle size
(generally without substantial crushing or pulverizing).
These particles are generally monoclinic crystals or tablets or conglomerates thereof
94/1651
(e.g. twinned crystals) some having projecting spike-like portions of generally rhombohedral shape
with many re-entrant angles. See
Figure 1 of the accompanying illustrations which is a photomicrograph of the crystals used in
Example 1, and Figure 2 which is a vietw of the crystals in a scanning electron microscope. Figure 3
is a photomicrograph of the crystals used in Example 2.
The toothpastes of the foregoing Examples are non-effervescent. Thus when diluted with water they
do not actively evolve bubbles of carbon dioxide.
The toothpastes of this invention have an alkaline pH, generally in the range from 8.5 to 9.5, usually
below 9.1.
The dentin abrasion of the toothpastes may be determined by the procedure based on a radioactive
technique described by Grabenstetter et al in the "Journal of Dental Research, Volume 37. P. 1060
(1958) as modified by the description by Stookey et al in the "Journal of Dental Research", Volume 47,
page 524 (July-August 1968).
In the preparation of the toothpastes of this invention the abrasive particles are blended with all or
part of the vehicle and then subjected to subatmospheric pressure (e.g. a vacuum of from 26 to 30
inches of mercury, corresponding to an absolute pressure of up to about 100 mm Hg) to remove
dispersed gas. The vacuum treatment is, however, discontinued, despite continued formation of gas
bubbles under vacuum, before the pH (i.e.
the pH of the vacuum treated mixture minus the pH of the mixture without vacuum treatment) reaches
one pH unit and preferably less, e.g. 1/2 unit; this avoids decomposition of sodium bicarbonate and
production of sodium carbonate during degassing.
WHAT WE CLAIM IS:1. Toothpaste containing from 20 to 60% of abrasive particles3 predominantly sodium bicarbonate,
in a water-glycerol vehicle, the water: glycerol ratio being in the range from 0.4:1 to 0.7:1; and from
0.5 to 1.5% of an essential oil flavouring agent.
2. Toothpaste as claimed in Claim 1 containing at least 25% sodium bicarbonate.
3. Toothpaste as claimed in Claim 1 or
95/1651
Claim 2 containing sodium bicarbonate of particle diameter predominantly above 150 microns but
below 0.4 mm.
4. Toothpaste as claimed in any of the preceding Claims in which the amount of essential oil
flavouring agent present is in the range from 0.8 to 1.2%.
5. Toothpaste as claimed in any of the preceding Claims which also contains a polymeric gelling
agent.
6. Toothpaste as claimed in Claim 5 containing sodium carbosymethylcellulose as the gelling agent.
7. Toothpaste as claimed in any of the preceding Claims which also contains a compatible
surfactant.
8. Toothpaste as claimed in Claim 1 and substantially as described in any of the Examples.
**WARNING** end of DESC field may overlap start of CLMS **.
Claims:
**WARNING** start of CLMS field may overlap end of DESC **.
invention the abrasive particles are blended with all or part of the vehicle and then subjected to
subatmospheric pressure (e.g. a vacuum of from 26 to 30 inches of mercury, corresponding to an
absolute pressure of up to about 100 mm Hg) to remove dispersed gas. The vacuum treatment is,
however, discontinued, despite continued formation of gas bubbles under vacuum, before the pH
(i.e.
the pH of the vacuum treated mixture minus the pH of the mixture without vacuum treatment) reaches
one pH unit and preferably less, e.g. 1/2 unit; this avoids decomposition of sodium bicarbonate and
production of sodium carbonate during degassing.
96/1651
WHAT WE CLAIM IS:1. Toothpaste containing from 20 to 60% of abrasive particles3 predominantly sodium bicarbonate,
in a water-glycerol vehicle, the water: glycerol ratio being in the range from 0.4:1 to 0.7:1; and from
0.5 to 1.5% of an essential oil flavouring agent.
2. Toothpaste as claimed in Claim 1 containing at least 25% sodium bicarbonate.
3. Toothpaste as claimed in Claim 1 or
Claim 2 containing sodium bicarbonate of particle diameter predominantly above 150 microns but
below 0.4 mm.
4. Toothpaste as claimed in any of the preceding Claims in which the amount of essential oil
flavouring agent present is in the range from 0.8 to 1.2%.
5. Toothpaste as claimed in any of the preceding Claims which also contains a polymeric gelling
agent.
6. Toothpaste as claimed in Claim 5 containing sodium carbosymethylcellulose as the gelling agent.
7. Toothpaste as claimed in any of the preceding Claims which also contains a compatible
surfactant.
8. Toothpaste as claimed in Claim 1 and substantially as described in any of the Examples.
97/1651
25. CN1079247 - 25.11.1993
ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN1079247
Inventor(s):
EHRET CHARLES (FR); PETRZILKA MARTIN (FR)
Applicant(s):
GIVAUDAN ROURE INT (CH); EHRET CHARLES (FR); PETRZILKA MARTIN (FR)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
E Class: C11B9/02B
Application Number:
WO1993EP01195 (19930513)
Priority Number: EP19920108469 (19920520)
Family: WO9323509
Equivalent:
CN1044490; DE69307656; ES2097506; HU213864; HU66737; JP6511511
Cited Document(s):
EP0202647; US3415813; EP0468189
Abstract:
A PROCESS FOR THE PREPARATION OF HYPOALLERGENIC MOSS OILS, COMPRISING
REACTING THE STARTING MOSS OIL, A CONCRETE OR PREFERABLY AN ABSOLUTE THEREOF,
WITH AN ALDEHYDE REDUCING AGENT, IN AN ORGANIC SOLVENT MEDIUM.Description:
Essential Oil
98/1651
The present invention relates to the preparation of moss oils which are characterized by
hypoallergenicity, i.e. by a strongly reduced allergenic potential and excellent olfactive performance
in perfume compositions.
Moss oils are highly appreciated by perfumers for their typical woody notes and play an important
role in the creation of perfumes, e.g. of the so-called "Chypre" or "Fougre" type. They are obtained by
solvent extraction of lichens including, in particular Evernia prunastri L. for the Oakmoss oil and
Evernia furfuracea L. for
Treemoss oil. The total amount of lichens treated worldwide for perfumery use may be estimated to
6000 tons/year (P. Vigne, Parfums,
Cosmetiques, Aromas, (78), p 97-105, 1987) and represents an estimated annual turnover close to
$ 35 millions.
Moss extracts, e.g. moss absolutes or concretes, which are the most frequently used moss oil
products have been reported to cause contact sensitization on human skin, and several groups of
researchers have shown that some components of moss oils, particularly ethyl hematommate I, ethyl
chlorohematommate II, atranorin Ill and chloroatranorin IV as depicted on page 3 are involved in
these allergenic reactions.
European patent publication No. 202,647 (Shiseido Company Ltd.) describes a process for the
preparation of hypoallergenic moss oils by removing allergenic substances from moss oils by
chromatography, solvent extraction, countercurrent partition and membrane separation followed by
a catalytic hydrogenation and/or an alkaline treatment. The allergens removed in this way are
aldehydes which include the above mentioned ethyl hematommate I, ethyl chlorohematommate II,
atranorin III and chloroatranorin n.
The more recent European patent publication No. 468,189 (Roure
S.k) describes a process for the preparation of hypoallergenic moss oils by reacting, e.g. moss
absolutes or concretes in alcoholic solution with amino acid(s) under mono-phasic conditions
followed by removal of the insolubilized allergenic substances I-VI.
The concentrations of the allergens I-VI achieved in this way are clearly below the critical levels
(0.05 - 1%) established experimentally via alIergenicity tests.
99/1651
The goal of the present invention was to eliminate now substantially further the above-mentioned
aldehydes I-VI by using an economical process without affecting significantly the original color and
olfactive performance of the starting moss oil, thereby providing moss absolutes or concretes with a
strongly reduced allergenic potential. It was achieved by reacting moss extracts e.g. concretes or
absolutes with appropriate reducing agents, e.g. alkali metal borohydrides, which specifically and
exclusively reduce the allergenic aldehydes I-VI to the corresponding primary alcohols.
A further advantage of the novel process consists in the avoidance of concomitant formation of trace
amounts of colorants, which can cause inconveniences for some perfumery applications.
The present invention describes thus the reaction between moss extracts, e.g. oils, concretes or
absolutes, with appropriate aldehyde reducing agents, e.g. complex metal hydrides, and preferably
with alkali metal borohydrides, e.g. lithium or sodium borohydride, in organic solvent systems.
The starting moss extracts subjected to this treatment are suitably obtained by solvent extraction of
lichens and include in particular the Oakmoss concrete (Evernia prunastri L.) and the
Treemoss concrete (Evernia furfuracea L.) and, preferably, the absolutes thereof.
It is known from the literature rB.g. Reagents for Organic
Synthesis, L.F. Fieser and M. Fieser, p 599-603 and 1049-1055, Editor
John Wiley and Sons, Inc., 19671 that complex alkali metal hydrides, e.g. borohydrides or aluminium
hydrides are able to reduce aldehydes, ketones and even esters. The aldehydic allergens I-VI
contribute insignificantly to the total odour of moss extracts, but numerous esters, other aldehydes
and ketones are known to be olfactively important minor or major constituents of these extracts Et.
Ter Heide et al., Qualitative Analysis of the Odoriferous Fraction of
Oakmoss (Evernia prunastri (L.) Ach.), J. Agric. Food Chem., 23 (5) p 950-957(1975)].
It was therefore surprising to find, that the novel process allowed the selective reduction of allergens
I-VI without organoleptically deteriorating the moss oil, or in other words, none of the
abovementioned organoleptically active constituents, e.g. no organoleptically relevant esters appear
to have been removed from the original moss extract, as was demonstrated by GC data. In addition,
the concentration levels found for I-VI are far below the required limits (cf. Table 1). and those
achieved in earlier publications [EP publication No. 468,189 and C. Ehret, P. Maupetit, M. Petrzilka,
100/1651
G. Kiecak, Int. J. of Cosm. Science, 14, 121-130 (1992)].Finally, the colors of the resulting nonallergenic moss oils are very close to the original ones and are therefore suitable for most perfumery
applications.
Table
Concentration levels required
Aldehydes for moss absolute with reduced
allergenic potential (%)
Ethyl hematommate I S1
Ethyl chlorohematommate II 0.05
Atranorins m + IV 50.15
Atranol V < 0.2 Chloratranol VI S0.2
In the broadest context of the present invention, the allergenic moss oil is dissolved in an
appropriate organic solvent and treated with preferably an excess of an appropriate aldehyde
reducing reagent. The suitable reducing agents are those which are able to reduce exclusively, or at
least preferentially the aldehydes over the esters and belong to various types (cf. R.C.Larock,
Comprehensive
Organic Transfonnations, A Guide to Functional Group
Preparations, published by VCH Publishers, Inc., New-York, 527-535 [1989],) e.g.: - complex metal
or ammonium hydrides, such as sodium,
lithium, potassium, zinc, tetraethylammonium borohydrides,
etc., - substituted complex metal or ammonium hydrides, such as
sodium triacetoxyborohydride, potassium triacetoxyborohydride,
sodium cyanoborohydride or tetra-n-butylammonium
triacetoxyborohydride, - metal hydrides, such as diborane or an alkali or aluminium
hydride, etc.
The preferred reducing agents are lithium borohydride and sodium borohydride.
The reduction can be carried out according to know methods. It is usually carried out in an organic
medium, e.g. in solution using optionally halogenated, aliphatic or aromatic hydrocarbon solvents,
such as hexane, cyclohexane or toluene, etc., ester solvents such as ethyl acetate, isopropyl acetate
etc., or alcoholic solvents, such as methanol, ethanol etc. Alternatively ether solvents such as t-butyl
methyl ether, tetrahydrofuran etc., or halogenated solvents such as methylene chloride may also be
used. Another possibility consists in using mixtures of the above-mentioned solvents.
101/1651
The concentrations of moss extracts applied in the reaction may vary between Ca- 5-50%,
preferably between Ca- 5-15% (w/w).
Convenient amounts of reducing agents, e.g. alkali metal borohydrides, are Ca- 0.02-0.1g,
preferably Ca- 0.03-0.07g per g of moss extract. This amount represents a ca. 2 to 5 fold molar
excess, i.e. a ca. 8 to 20 fold reducing equivalent excess.
The reaction temperature is Ca- 20"-800C, preferably ca. 20"-30"C, if, e.g. lithium borohydride is
used, and preferably reflux temperature, e.g. that of an alcanol, e.g. ethanol, if sodium borohydride is
used.
The reaction is usually quenched after ca. 30 minutes to 3 hours, preferably after Ca- 30 to 60
minutes, if sodium borohydride is used, and after ca. 1-2 hours, if lithium borohydride is used.
If water insoluble solvents are used for the reaction, such as hydrocarbons, esters, halogenated and
aliphatic ether solvents, work up consists in extensively washing the reaction mixture with water or
aqueous acids (e.g. 1-10%, preferably 1-3% aq. HCl solution) followed by water until neutral. Finally
the organic solvent is distilled off at reduced pressure without exceeding a temperature of ca. 850C.
Alternatively, if water soluble solvents are used, e.g. an alcohol or a cyclic ether, such as
tetrahydrofuran, the solvent is first removed by distillation at reduced pressure. The remaining
residue is then redissolved in a water insoluble solvent, e.g. the solvents mentioned above, and
worked up as in the previous case.
Examples 1) Allereenicitv
The strongly reduced allergenic potential in the product was in each case determined by
conventional, filly established skin sensitization and skin response methods, i.e. in concreto the socalled * Modified BUEHLER method using guinea pigs, and the * RIPT (Repeated Insult Patch Test)
using human subjects.
2) Analvsis
Content of aldehvdes I. II. V and v'
The contents of products I, II, V and VI are suitably determined by GC analysis, using an internal
standard and working under the following conditions: * Column: 50m x 0.32mm inner diameter,
102/1651
fused silica * Stationary phase: CP Sil 5CB (a silicone) * Detector : Fm (flame ionisation detector) *
Vector gas : Helium, 2ml/1nn * Temperature program: 100-2400C, 20C/min.
* Internal standard : methyl 2,4-dihydroxy-3,6-dimethyl-benzoate Content of aldehydes III and IV
The contents of aldehydes III and IV are suitably determined by
HPLC, using an externaI standard and working under the following conditions * Column: 250mm
length, 4.6mm i.d.
* Stationary phase : RP 18 (reverse phase, particle size: 7 m) * Detector : UV at 260nm * Mobile
phase A: H2O acidified to pH 2.8 with conc. H3P04
B : acetronitrile * Gradient: Time(mln.) %A QoB Flow (milmin.)
0 80 20 1
30 5 95 1
40 5 95 1
This gradient allows the effective separation of the above nonvolative aldehydes III and IV.
Example 1
Production of Oakmoss absolute with strongly reduced allergenic potential using lithium borohvdride
A 500ml three-necked flask equipped with a mechanical stirrer, a condenser and a dropping funnel
was charged with 15g of a commercially available melted Oakmoss absolute (Givaudan-Roure, mp
about 700C), which then was dissolved in 200ml of cyclohexane/isopropyI acetate 3:1 at room
temperature and under N2. To this homogeneous solution was then added dropwise a suspension of
480mg (22 mmol) of lithium borohydride in 100ml of cyclohexane/isopropyl acetate 3:1 during ca. 30
minutes. Immediately after addition a precipitation occurred and a slight increase of the temperature of the reaction mixture (ca. 6 C) was observed.After stirring the reaction mixture for an
additional 2 hours at room temperature, it was carefully quenched with 150ml of 0.5% (w/w) aqueous
HCl and extracted with cyclohexaneisopropylacetate 3:1 (3 x 300ml). The organic layers were
washed with water (1 x 150ml), combined and concentrated at reduced pressure (20 mbars) on a
water bath without exceeding a temperature of ca. 850C. An Oakmoss absolute (12.78g, 85.2% yield)
was obtained in this way, which according to GC- and
HPLC- analysis contained extremely small amounts of aldehydes I-VI (cf. Table 2).
Table 2
Starting Resulting
Aldehyde Oakmoss Oakmoss
103/1651
absolute (%) absolute (%)
Ethyl hematommate I 2.40 < 0.01
Ethyl chlorohematommate II 1.44 < 0.01
Atranorins III + Iv 0.58 0.05
Atranol V 424 0.06 Chloratranol VI 2.28 < 0.01 Examnie2
Production of Oakmoss absolute with strongly reduced allergenic potential using sodium
borohydride
A 250ml three-necked flask equipped with a mechanical stirrer, a condenser and a dropping funnel
was charged with 14.9g of a commercially available melted Oakmoss absolute (Givaudan-Roure, mp
about 700 C), which then was dissolved in 90ml of ethanol 96% at room temperature and under
N2.To this solution was then added dropwise a suspension of 1g (26.4 mmol) of sodium borohydride
in 60ml of ethanol 96% during ca. 5 minutes. During the addition a slight increase of the temperature
(ca. 120C) was observed. After stirring the reaction mixture at reflux temperature during 45 minutes,
the ethanol was distilled off at reduced pressure (20 mbars) and the residue was taken up in 300ml
of t-butyl methyl ether (TBME). The reaction mixture was then carefully quenched with 150ml of water
and extracted with TBME (3 x 300ml). The organic layers were washed with water (1 x 150ml),
combined and concentrated at reduced pressure (20 mbars) on a water bath without exceeding a
temperature of ca. 65"C.An Oakmoss absolute (12.78g, 85.2% yield) was obtained in this way, which
according to GC- and HPLC- analysis contained extremely small amounts of aldehydes I-VI (cf.
Table 3).
Table 3
Starting Resulting
Aldehyde Oakmoss Oakmoss
absolute (%) absolute (%)
Ethyl hematommate I 3.78 0.11
Ethyl chlorohematommate II 1.46 0.02
Atranorins Ill + IV L16 0.01
Atranol V 3.30 < 0.01
Chloratranol Vl 1.92 0.03 Exampie3
Production of Oakmoss absolute with strongly reduced allermc potential using sodium borohydride
(acidic work un)
A 250ml three-necked flask equipped with a mechanical stirrer, a condenser and a dropping funnel
was charged with 15g of a commercially available (Givaudan-Roure), melted Oakmoss absolute (mp
about 70 C), which then was dissolved in 100ml of ethanol 96% at room temperature and under N2.
104/1651
To this solution was then added dropwise a suspension of ig (26.4 mmol) of sodium borohydride in
60ml of EtOH 96% during ca. 5 minutes. During the addition a slight increase of the temperature (ca.
15 C) was observed. After stirring the reaction mixture at reflux temperature during 45 minutes
ethanol was distilled off at reduced pressure (20 mbars) and the residue was taken up in 300ml of tbutyl methyl ether. The reaction mixture was then carefully quenched with 100ml of water and
acidified to pH = 1.5 with ca. 15ml of 6% aqueous HCl. The organic layer was washed with water (1
x 150ml) and concentrated at reduced pressure (20mbars) on a water bath without exceeding a
temperature of ca. 65 C. An
Oakmoss absolute (14.42g, 96.1% yield) was obtained in this way, which according to GC- and
HPLC- analysis contained extremely small amounts of aldehydes I-VI (cf. Table 4).
Table 4
Starting Resulting
Aldehyde Oakmoss Oakmoss
absolute (%) absolute (%)
Ethyl hematommate I 3.78 0.05
Ethyl chlorohematommate II 1.46 0.02
Atranorins III + IV 1.16 0.05
Atranol V 3.30 < 0.01
Chloratranol VI 1.92 < 0.01 Claims:
Claims
1. A process for the preparation of hypoallergenic moss oils, comprising reacting the starting moss
oil, a concrete or preferably an absolute thereof, with an aldehyde reducing agent, in an organic
solvent medium.
2. A process according to claim 1, wherein the reagent is an alkali metal hydride, an optionally
substituted complex metal or ammonium hydride, preferably an alkali metal borohydride, e.g.
preferably lithium or sodium borohydride.
105/1651
3. A process according to claim lor 2, wherein the solvent used is an optionally halogenated,
aliphatic or aromatic hydrocarbon, an ester, an alcohol, an ether or a mixture of such solvents.
4. A process according to any one of the claims 1 to 3, wherein the solvent used is substantially
water insoluble, e.g. a mixture of a aliphatic hydrocarbon, preferably hexane or cyclohexane, with a
alkane carboxylic acid ester, preferably ethyl acetate or isopropyl acetate or an aliphatic ether,
preferably t-butyl methyl ether.
5. A process according to any one of the claims 1 to 3, wherein the solvent used is water soluble,
preferably an alkanol, e.g. ethanol or a cyclic ether, e.g. tetrahydroftran.
6. A process according to clam 5, wherein the work up is carried out in a water insoluble solvent,
preferably a solvent of claim 4.
7. A process according to any one of claims 1 to 6, wherein the reaction is carried out within a
temperature range of ca. 200-80"C, preferably at ca. 20 -30 C if lithium borohydride is used and
preferably at ca. 60"-80"C if sodium borohydride is used.
8. Hypoallergenic moss oils, whenever prepared according to a process as claimed in any one of
claims 1 to 7 or by an obvious chemical equivalent thereof.
106/1651
26. CN1229114 - 22.09.1999
MAKING AND APPLICATION OF FPS WATERPROOF AND ANTICORROSIVE ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN1229114
Inventor(s):
LI GUANGHAI (CN); ZHOU JIAOYANG (CN); CHEN JINQUAN (CN)
Applicant(s):
CHEN JINQUAN (CN)
IP Class 4 Digits: C09D
IP Class:
C09D125/06; C09D5/08
Application Number:
CN19980112383 (19980314)
Priority Number: CN19980112383 (19980314)
Family: CN1229114
Abstract:
A WATER-PROOF AND ANTICORROSION REFINED FPS OIL USED AS BOTH THE
ANTICORROSION, WATER-PROOFING AND LEAKAGE-STOPPING AGENT AND THE DECORATIVE
PAINT OF METAL OR FERNITURE IS PREPARED FROM WASTE POLYSTYRENE, BUTYL ACETATE
AS SOLVENT, ETHYL ACETATE AS ADDITIVE, METHYL ETHYL KETONE PEROXIDE AS
PLASTICIZER, AROMATIC SOLIDIFYING AGENT AND COLOURING AGENT.
107/1651
27. CN1265597 - 06.09.2000
COMPOSITION COMPRISING PROPOLIS AND AT LEAST AN ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN1265597
Inventor(s):
MORICE ANDR PIERRE (FR)
Applicant(s):
ANDR PIERRE MORICE (FR)
IP Class 4 Digits: A61K
IP Class:
A61K35/78
Application Number:
CN19980807944T (19980804)
Priority Number: FR19970010414 (19970811); FR19980002027 (19980219)
Family: CN1288370
108/1651
28. CN1333326 - 30.01.2002
ROSEMARY ESSENTIAL OIL, ANTIOXIDANT AND PREPARATION PROCESS THEREOF
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN1333326
Inventor(s):
SONG GUANGWEI (CN); SUN GUIBIN (CN); YU ZHENTAO (CN)
Applicant(s):
HAINAN WANHENG BIOLOG ENGINEER (CN)
IP Class 4 Digits: C11B
IP Class:
C11B1/10
Application Number:
CN20010130930 (20010827)
Priority Number: CN20010130930 (20010827)
Family: CN1333326
Abstract:
THE PREPARATION METHOD OF ANTIOXIDANT AND ESSENTIAL OIL OR ROSEMARY INCLUDES
THE FOLLOWING STEPS: DRYING FRESH YOUNG TWIG OF ROSEMARY IN THE SHADE,
PULVERIZING, PLACING THE PULVERIZED MATERIAL IN THEEXTRACTION STILL OF CO2
SUPERCRITICAL EXTRACTION EQUIPMENT, EXTRACTION PRESSURE IS 10-5 MPA, AND
EXTRACTION TEMP. IS 20-80 DEG.C AND EXTRACTION TIME IS 2-4 HR., THEN ADOPTING
THREE-STAGE SEPARATOR TOSEPARATE EXTRACT SO AS TO OBTAIN ESSENTIAL OIL OF
ROSEMARY, THEM FREEZE-DRYING SO AS TO OBTAIN FAINT YELLOW POWDER, I.E. ROSEMARY
ANTIOXIDANT.
109/1651
29. CN1376539 - 19.09.2002
A SIMPLE PORTABLE MINI DISTILLATION APPARATUS FOR THE PRODUCTION OF ESSENTIAL
OILS AND HYDROSOLS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN1376539
Inventor(s):
SINGH VIRENDRA (IN); AHUJA PARAMVIR SINGH (IN); KAUL VIJAY KUMAR (IN);
BABU GARIKAPATI D KIRAN (IN)
Applicant(s): COUNCIL SCIENT IND RES (IN); SINGH VIRENDRA (IN); AHUJA PARAMVIR
SINGH (IN); KAUL VIJAY KUMAR (IN); BABU GARIKAPATI D KIRAN (IN)
IP Class 4 Digits: C11B; B01D
IP Class:
C11B9/02; B01D3/38; B01D11/02
E Class: C11B9/02H; B01D3/10; B01D5/00H10B; B01D11/02M2
Application Number:
WO2001IN00035 (20010313)
Priority Number: WO2001IN00035 (20010313); CN20010109963 (20010326)
Family: CN1376539
Cited Document(s):
FR516003; FR752093; US5478443; DE19804010; FR2435521
Abstract:
THIS INVENTION RELATES TO A SIMPLE, CONVENIENT, PORTABLE MINI-DISTILLATION
APPARATUS FOR THE PRODUCTION OF ESSENTIAL OILS AND HYDROSOLS, SAID APPARATUS
IS USEFUL TO DISTIL ESSENTIAL OILS AND HYDROSOLS SUCH AS ROSE WATER, AJOWAIN
WATER FROM FRESH AND DRIED PLANT MATERIAL LIKE LEAVES, FLOWERS, ROOTS AND
RHIZOMES BY WATER DISTILLATION, WATER AND STEAM DISTILLATIONS AND AS AN
OPTIONAL, STEAM DISTILLATION CAN ALSO BE PERFORMED AT ATMOSPHERIC PRESSURE AS
WELL AS SLIGHTLY HIGHER AND LOWER THAN ATMOSPHERIC PRESSURE, SAID APPARATUS
110/1651
CAN BE HEATED ON BRICK-CLAY FURNACE WITH SMALL AGRO-WASTE, LPG COOKING GAS,
ELECTRICALLY HEATED STOVE OR KEROSENE/DIESEL BURNER ETC. AND REQUIRES MINIMUM
ATTENTION DURING HANDLING; SINCE THE APPARATUS IS MADE OF STAINLESS STEEL AND
GLASS, THE ESSENTIAL OIL DISTILLED IS OF BETTER QUALITY.Description:
A SIMPLE PORTABLE MINI DISTILLATION APPARATUS FOR THE
PRODUCTION OF ESSENTIAL OILS AND HYDROSOLS
Technical Field
The present invention relates to a simple, convenient, portable mini-distillation apparatus for the
production of essential oils and hydrosols.
This apparatus is useful to distil essential oils and hydrosols such as rose water, ajowain water from
fresh and dried plant material like leaves, flowers, roots and rhizomes by water distillation, water and
steam distillations and as an optional, steam distillation can also be performed at atmospheric
pressure as well as slightly higher and lower than atmospheric pressure. This unit can be heated on
brick-clay furnace with small agro-waste, LPG cooking gas, electrically heated stove or
kerosene/diesel bumer etc. and requires minimum attention during handling. Since the apparatus is
made of stainless steel and glass, the essential oil distilled is of better quality than the oil distilled by
glass Clevenger type apparatus used in the laboratory.
Background Art
Laboratory equipment used for distillation of essential oils is called Clevenger type apparatus as
shown in Fig. 1 of the drawings accompanying this specification. Reference may be made to
Clevenger type, J. F., Apparatus for the determihatioyl of volatile oil. J.
Amer. Pharm. Assoc., 17, pp. 346 (1928), wherein the apparatus (1) is attached to the spherical
glass vessel (a) having charged with the plant material along with water in 1 : 2 ratio through opening
(b) which is also used for discharging the mixture after process is complete. The whole system is put
on a heating mantle (c), which has an energy regulator (d) for controlling the temperature. After few
minutes, the material inside starts boiling.
The vapours so formed are passed through a vertical condenser (e) through a long vertical glass
tube (f). The cold water around the condenser tube is circulated through inlet (g) and outlet (h). The
condensed distillate gets collected in a measuring tube (i) connected to the outlet of the condenser
111/1651
where an air outlet (j) open to atmosphere is placed. The volatile oil separates as an upper layer,
from the distillate because of its density difference, as the oil is lighter than the water. A return tube
(k), for recycling of aqueous part of the distillate, connects the bottom of the measuring tube (i) and
vertical tube (f). The oil is collected at the outlet by opening the stop-cock valve (1).
The major drawback of the apparatus is that it was designed to distillate the plant material by water
distillation at normal atmospheric pressure only. There are some aromatic plant materials exclusively
distilled by steam distillation method rather than water distillation, reason being that some of volatile
constituents get hydrolysed due to the presence of excessive water in the vessel. The apparatus
works neither on the principle of steam distillation nor on water and steam distillation technique.
Clevenger type apparatus is generally restricted to laboratories for the essential oil estimation but
cannot be used to produce the essential oil in higher quantities. Since the system is heated up with
the help of electric mantle (c) only, with very small batch capacity of material charging vessel (a),
long vertical glass tube (f) and condenser (e) are made up of glass which requires careful handling
and can not be heated without electricity which is difficult for a marginal farmer with small land
holdings in remote areas. The recovery and quality of the essential oil distilled in this glass Clevenger
type apparatus is of inferior quality. The colour of the oil is generally lighter than the commercially
distilled oil, which is not recommended in the market. Pure distillation is not possible since the oil is
obtained with other materials/contaminants.
There are distillation units, which are operated by Water and Steam distillation method.
Water and Steam distillation method involves a distillation tank with a false bottom and with or without
Calendria at the bottom. Cohobation column at the top which is connected to the condenser and a
distillate receiver. The plant material is charged from the charging hole and closed tightly. Prior to
charging of plant material some fresh water is added to the tank and the precautions are to be taken
to control the water level which should not touch the false bottom. The water level is maintained by
recycling the distillate collected in the receiver to the tank or continuous or batch-wise fresh water is
supplied to the tank. The tank is heated by direct firing of the agro-waste from the hearth, bellow. The
purpose of this method is to reduce the effect of hydrolysis of essential oil which are get hydrolysed
when they came in to continuous contact with excess water. After few minutes the water vapours
starts forming and extracts the essential oil from the plant material and carries it over to condenser
where they are condensed to liquid distillate. The distillate is collected in a receiver where it is
separated in to two fractions; one as an essential oil and other as saturated water layer. The essential
oil is separated, cleaned and then stored as per the recommended methods.
112/1651
The major drawbacks of the unit are that it can not distil the plant material by Steam distillation. Some
parts of the aromatic herbs such as cedar wood, sandalwood are preferably distilled by Steam
distillation method to obtain better recoveries and quality.
Also these units can not distil the plant material neither at reduced pressure nor at higher pressure
since the system is opened to the atmospheric pressure and can not operated as a closed system.
Being an industrial size, these units can not be a portable systems and thus difficult to take them to
the fields where the plant material is available in remote areas and distilling the fresh raw material is
not possible in such a system which is one of the major parameter in affecting the quality of an
essential oil. Being commercial scale units they requires more man power, operational costs etc.,
and the marginal farmers can not afford to purchase these industrial scale distillation units.
The widely used hydro distillation method in the essential oil industry is Steam distillation
The units used to perform the Steam distillation method merely consists of a distillation tank with a
false bottom fixed at a certain height from the bottom of the tank. A spurger is provided below the
false bottom, which is connected to the industrial size boilers. The plant material is placed above the
false bottom and then the lid is closed tightly by nutbolts. Steam generated from the boiler is fed to
the tank through the fixed steam spurger to commence the distillation. After few minutes the vapours
starts forming which are taken to the vapour inlet of a shell and tube condenser, which is connected
to the vapour out, let of the distillation tank at the top. The condensed liquid is collected in a receiver
where the essential oil and distillate are separated.
The major drawbacks of the unit are that it cannot distil the plant material neithel by Water distillation
nor by Water and Steam distillation. Some parts of the aromatic herbs are preferably distilled by
Water distillation method to obtain better recoveries and quality.
Also these units can not distil the plant material neither at reduced pressure nor at higher pressure
since the system is opened to the atmospheric pressure and can not operated as a closed system.
Being an industrial size these units cannot be a portable, and thus difficult to take them to the fields
where the plant material is available in remote areas and distilling the fresh raw material is not
possible in such a system which is one of the major parameter in affecting the consistency in the
quality of an essential oil. Being commercial scale units they require more man power, operational
costs etc., and the marginal farmer cannot afford to purchase these industrial scale distillation units.
113/1651
Thus, apparatus, industrial scale units and the process mentioned above has one or the other major
drawbacks like inferior oil quality, low oil recovery, low batch capacity, lack of water distillation,
steam distillation and water and steam distillation facility, restricted mode of heating, unable to distil
the plant material under vacuum and at higher pressures, difficulty in charging and discharging of
plant materials because of narrow mouth and requires more attention during processing, more
capital investment, operational cost.
Objects of the Invention
The main object of the present invention is to provide a simple, convenient, portable mini distillation
apparatus for the production of essential oils and hydrosols, which obviates the drawbacks as
detailed above.
Another object of the present invention is to provide an apparatus for the distillation of essential oils
having capacity little higher than the laboratory scale apparatus to meet the needs of marginal
farmers.
Still another object of the present invention is to provide an apparatus for the distillation of essential
oils, if required, slightly at higher and lower pressures than atmospheric pressure.
Yet another object of the present invention is to provide an apparatus for the distillation of essential
oil by water distillation, water and steam distillation and steam distillation on small scale.
Yet another object of the present invention is to provide an apparatus for the production of perfumed
water from aromatic plant materials at small scale.
Yet another object of the present invention is to provide an apparatus for the production of distilled
water from the tap water or natural sources for lab use or for other purpose.
Yet another object of the present invention is to provide portable and convenient apparatus for
effecting distillation even in the fields or remote farming areas.
Yet another object of the present invention is to provide an apparatus for the production of quality
grade essential oils at household scale as a cottage industry to suit the marginal
farmers/entrepreneurs who can not afford to install bigger capacity units.
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Brief description of the accompanying drawings
Figure 1 shows the conventional distillation apparatus.
Figure 2 shows the schematic diagram of the present invention.
Summary of the invention
Accordingly the present invention provides a simple, convenient and portable minidistillation
apparatus, essentially consists of main parts such as a distillation vessel (I) ; a cohobation column.
(8), condenser (11) and oil retention column (13) with recycle line (16) connected to the cohobation
column (8).
Detailed Description of the invention
Accordingly, the present invention provides a simple, convenient, portable mini-distillation apparatus
as shown in fig 2 of the accompanying drawings, for the production of essential oils and hydrosols,
which comprises one or more vessel (s) (1) capable of being heated either internally/externally or
both, the inside bottom of the said vessel (s) being provided with a threaded rod (6) fixed
concentrically in such a manner so as to allow vertical movement of a sieved false bottom (5), one or
more steam spurger (s) (24) being provided between the vessel bottom (2) and the said movable
false bottom (5, 7), the said vessel (s) being provided with lids (s) (3) having one or more safety
valve (s) (21), said lid (s) being attached with the vessel by means of removable fixing means, the lid
(s) are also provided with parameter gauges (20) such as pressure, vacuum, temperature gauges
and a vapor outlet (s) (9), the said vapor outlet (s) being connected by known means to the inlet of
one or more vertical cohobation column (s) (8), the outlet (s) of the said cohabitation column (s)
being fixed by known means to the inlet (10) of a condenser (11) provided with closeable vent (15),
the outlet (12) of the said condenser being detachably connected by one or more connecting means
(14) to a vertical receiver-cum-separator column (13) having a valve (18) at its lower end, which
controls an outlet (23), the bottom and middle of the said receiver-cum-separator column being
provided with a plurality of valves (17,19) which control flow of fluids in one or more recycling means
(16) connected to the upper portion of the said cohobation column (s).
In one embodiment of the present invention, the false bottom (5) in the vessel (1) is used to hold the
plant material to be distilled by adjusting at a suitable height to accommodate the material.
In another embodiment of the invention, when the apparatus used in water distillation method, the
false bottom (5) is removed completely from the vessel (1) or kept at the lowest possible height from
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the base and then the plant material is charged along with water for processing and the plant
material is immersed in water.
In still another embodiment of the invention, when the apparatus is used in water and steam
distillation method, the level of the water charged in the vessel (1) is kept below the false bottom (5)
and the plant material is charged over the false bottom (5) which is adjusted by revolving clockwise
or anti-clockwise as the case may be on the threaded rod (6), the false bottom (5) here is used to
separate the plant material and water.
In still another embodiment of the invention, the false bottom (5) is so adjusted to accommodate the
plant material which is very less to distil in a given capacity of distillation unit preferably atleast one
fifth of the holding capacity of the unit to minimise or no essential oil.
In yet another embodiment of the present invention, the apparatus comprising steam spurger (24)
having holes is provided below the false bottom (5) in the vessel (1) and when steam is injected into
the vessel through the steam spurger for distilling the plant material which is kept on the false bottom
by steam distillation method.
In yet another embodiment of the present invention, the vessel is heated internally by means of
known heating system preferably electrical system and externally by any conventional/nonconventional heating means/sources selected from fire woods, coal, oil, gas burners, boilers etc.
In yet another embodiment of the present invention, the vessel has a height to diameter ratio in the
range of 0.5 to 1.5.
In yet another embodiment of the present invention, the vessel, cohobation column, condenser and
recycling pipes are made up of metals selected from stainless steel, copper, tin.
In yet another embodiment of the present invention, the receiver-cum-separator is made up of glass,
coated with transparent plastic or covered with an aluminium casing.
In yet another embodiment of the present invention, the vertical receiver-cum-separator column is
graduated.
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In yet another embodiment of the present invention, the closeable vent (15) of the condenser is
optionally connected through a valve to a vacuum pump.
In yet another embodiment of the present invention, the cohobation column is connected to the
vessel, condenser by means of clamps with or without gaskets, o-rings, and threaded arrangements
with or without gaskets.
In yet another embodiment of the present invention, the condensing means is any conventional
means such as water or air cooling condenser.
In yet another embodiment of the present invention, the vessel is provided with handles.
In yet another embodiment of the present invention, the steam spurger (24) is connected to one or
more external steam sources such as boilers.
In yet another embodiment of the present invention, the fluids escaping from the condenser may be
recirculated to the vessel (1) or collected in separate containers using known means.
In fig. 2 of the drawings accompanying this specification, a schematic diagram of an embodiment of
the apparatus of the present invention is shown. The present invention essentially consists of main
parts such as a distillation vessel (I) ; a cohobation column. (8), condenser (11) and oil retention
column (13) with recycle line (16) connected to the cohobation column (8).
One of the embodiment of the invention the present portable mini distillation unit provides a simple,
convenient, portable apparatus for the distillation of essential oils which comprises charging of
aromatic plant material along with water in the ratio in the range of 1: 0 to 1: 2 in the vessel (1)
through the charging hole, as described above and depicted in
Fig. 2, depending upon the type of the distillation process to be used. Place the gasket properly
above the flange of the still, tighten the lid by quick fit joint (4) and attach the cohobation column (8),
condenser (11) and glass tube (13) with the lid by tightening the union (9) after ensuring the proper
setting of the gasket, place the whole system above the direct fired furnace/LPG burner/Kerosene or
Diesel stove for heating the vessel (1). Fill the shell side of the condenser with water and the optimum
water flow rate, for the total condensation, was maintained. Fill the oil retention glass tube (13) with
water through air vent (15) at rear end of the condenser (11) until water starts flowing in to the
cohobation column (8) through recycling line (16). The air vent (15) on the condenser (11) is opened
117/1651
throughout the process, if the plant material is to be distilled at atmospheric pressure and remain
closed if the plant material is to be extracted under pressure. The valve (19) on the recycle line is
kept opened throughout the process if essential oil only is to be distilled and remain closed if only
perfumed distillate required. Now start heating the vessel (1) with any heating means mentioned
above. Vapours start forming few minutes later and enter to the condenser (11) through cohobation
column (8) where they are condensed and collected in the glass tube. The essential oil in the
distillate settles as an upper layer over the lower layer of water as the case may be. The aqueous
part of the distillate is recycled, to the cohobation column (8) through the recycling line (16) if the
essential oil is lighter than the water otherwise, it is recycled through the other pipe line shown in the
Figure 2 as a dotted line. In order to recover the dissolved oil, the process is continued for 3 to 5
hours depending upon the type of plant material and distillation performed. After the completion of
process, the essential oil is collected from the outlet (23) of glass tube (13) by opening the valve (18).
The collected oil is measured and dried over anhydrous Na2S04 filtered and then can be stored in
aluminium bottles.
The constructional features of an embodiment of the apparatus of the present invention are given
below:
A stainless steel (SS)-304 vessel (1) having internal diameter (ID) = 325 mm, height = 325 mm with
slightly curved bottom (2) and wide mouth ID = 325 mm for easier charging and discharging plant
material is to be distilled, above which a conical lid (3) with base diameter = 325 mm, vertical height
= 150 mm, slant height = 210 mm to which a flange ID = 325 mm, outer diameter (OD) = 350 mm, is
welded. The lid is attached to the vessel by a quick-fit joint (4). The material of construction (MOC) of
lid (3) is stainless steel (SS)304. A false bottom (5), 320 , 2 mm thiclmess (thk.), with 2 holes in
triangle pitch and 10 hole in the centre to fit in the threaded SS rod (6) with 10 for adjusting up and
down according to the plant material charged. A circular strip (7) ID = 315 mm, OD = 325 mm
welded to the vessel at a height of 35 mm from the bottom end to hold the false bottom. At the top of
conical lid (3), a stainless steel cohobation column (8) is fixed with the help of union (9). The
cohobation column (8) ID = 50 mm up to at a height of 780 mm which is reduced to ID = 40 mm up
to a length of 215 mm and slant height of the reducer is 40 mm.
The outlet of the column, ID = 40 mm, is welded to a bend (10) having same ID. The bend is again
welded to a stainless steel horizontal shell and tube I-I heat exchanger (condenser) (11) with ten
number of SS seamless tubes ID = 8 mm, length (L) = 250 mm and shell ID = 80 mm, L= 330 mm
including both the bonnets with an inclination of 120 with horizontal plane. The outlet (12) ID = 25
mm, L= 60 mm, of the distillate welded at the rear end of the condenser, is connected to graduated
118/1651
glass (13) tube by 1/4"diameter nuts and bolts on flanges ID = 25 mm, OD = 110 mm for collecting
the distillate and the essential oil. A silicon gasket (14) ID = 25 mm, OD = 75 mm, thickness (thk.) = 2
mm is placed in between the flanges. An air vent (15) ID = 5 mm on the condenser rear end is
welded to distill the plant material at required pressures. A stainless steel recycling pipe (16) with ID
= 6 mm, L = 540 mm is welded to the cohobation column at a height of 745 mm from the base of the
glass column to recover the dissolved essential oil if the oil is lighter than the water. In case of oil
being heavier than water, the recycle line is shown in dotted lines. The other end of the pipe is
connected to the bottom of the glass tube ill = 10 mm by means of flexible silicon tube (17). The
glass tube for collecting the distillate is reduced from ID = 20 mm, for a distance of L = 80 mm at the
outlet flange of the condenser, to ID = 10 mm. The bottom of the glass tube (13) is again reduced to
ID = 1 mm (23) with a valve (18) in between for discharging the distillate and essential oil. The
flexible silicon tube has a clip (19) to isolate the SS recycling pipe from the base of the glass tube.
Length of the glass tube from its flange to recycle connection is 650 mm and length of the glass tube
portion from recycle connection to oil drain out valve is 40 mm.
Length of the glass tube from valve to the end of the capillary is 70 mm. A pressure gauge (20) and a
safety valve (21) were fixed above the lid.
The novelty of the apparatus of the present invention is that the said apparatus is capable of
providing water distillation, steam distillation, water and steam distillation at atmosphere pressure, as
also above and below atmospheric pressure. Further, the apparatus is capable of distilling the
heavier and lighter essential oils and also producing hydrosols (perfumed water) such as rose water,
ajowain water, camphor water.
The inventive steps of the constructional features of the apparatus of the present invention apart from
other modifications, preferably lies in incorporating (a) one or more steam spurgers between the
vessel bottom and moveable sieved false bottom, (b) air vent capable of being connected through a
valve to a vacuum pump and (c) a plurality of valve operated recycling lines.
The following examples are given by way of illustration of the device and the process of the present
invention for the distillation of essential oils and should not be construed to limit the scope of the
present invention.
Example 1
In the beginning, 6 lit of fresh water were charged into the sterilised/rinsed vessel (1).
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Then, 3 kg of fresh Geranium leaves were placed above the false bottom. The false bottom was
adjusted so that the distance between false bottom and water level was 80 mm (minimum). The
vessel was placed above the furnace. The furnace was so constructed that the 3/4 of the vessel
when immersed into the furnace can get maximum heat in-put to distill the plant material. Before
placing the vessel above the furnace, mud was coated outside of the vessel to reduce the soot
formation on the walls of the vessel. The lid and cohobation columns were fitted above the flange of
the vessel. It was ensured that the gasket on flange of the vessel and'0'ring between the outlet of the
lid to cohobation column was properly placed so that no leakage of vapour and liquid appeared. The
flange of the graduated glass tube was also fixed with the flange of the condenser outlet. A silicon
tube was also fixed to connect the recycling line to the oil receiving graduated glass tube.
The furnace was fired with agro-waste to heat the mixture in the vessel. After a few minutes, the water
below the false bottom started boiling and formed steam, which then passes through the Geranium
leaves and extracts essential oil present in it. The steam comes out with the oil and reaches the
condenser through cohobation column, the steam was enriched with oil in cohobation column, and
condensed in the condenser. The condensate was collected in the graduated glass tube. The oil as
its density was lower than the water, settled as an upper layer and the oil saturated water, as a lower
layer. The oilsaturated water was recycled through recycling line, connected at the bottom of oil
receiver to the cohobation column, to recover oil present in it. The process was continued for 3 hr. by
maintaining the flow rate of the distillate around 1.5 ml/min. The range of shell side fluid flow rate in
the condenser was maintained in such a way that the temperature of the condensate was around 20
C. At the end of the process the fire in the hearth was stopped.
There after the flow rate of distillate from condenser was also stopped followed by stoppage of water
connection to the condenser. The oil collected in the graduated glass receiver was measured to 6.9
ml with a recovery of 0.23 %. Two kg of same sample of
Geranium leaves was also distilled simultaneously, in a glass Clevenger type apparatus as
discussed in prior art and the oil yield was recorded to be 3.4 ml with a recovery of 0.17%.
The quality analysis was done by gas chromatographic analysis and the results are given below in
Table No 1.
Table 1
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Constituents Present invention (%) (Mini Prior art (%)
distillationapparatus (Clevenger apparatus)
Cis-rose oxide 0.09 0.09
Trans-roseoxide 0. 02 0. 02
Isomenthone 5.3 5.2
Citronellyl formate 5. 7 (18% extra) 4. 8
Geranyl formate 6. 0 (Double) 3. 0
Citronellol 23. 3 (8% extra) 21. 4
Geraniol. 28.6 (29% extra) 22. 1
Epi-y-eudesmol 5.4 5.3
Geranyl tiglate 1.7 1. 6
Thus, quality and quantity of the oil distilled in this apparatus was found to be better than
Clevenger type apparatus.
Example 2
The false bottom (5) was adjusted by rotating to fix at a height above the water level before placing
the still (1) above the LPG burner. The still was charged with 3 kg of fresh
Tagetes minuta (whole herb) along with 4 lit of fresh water, the whole mat-rial was processed by
water and hydro-distillation. The gasket (22) was placed properly above the flange of the still and
tightened the flange by quick fit clamp (4). The whole system was attached with the lid by tightening
the union (9) after ensuring the proper setting of the gasket The water connection was given from tap
to the condenser through rubber tube to fill the shell side of the condenser with water. Support was
given to the whole system by fixing with the stand so that it can withstand the impulses. The oil
retention glass tube (13) was filled with water through air vent (15) welded at the rear end of the
condenser till water starts flowing into the cohobation tower (8) through recycling line (16) The valve
(19) was remained open on the recycle line, throughout the process, main vessel (1) was started
heating by lightening the LPG gas burner. After a few minutes vapour started forming, if proper heat
is provided, the vapours formed were condensed in a condenser (11) and collected in a oil retention
glass tube (13). The essential oil part of the distillate was settled as an upper layer and oil saturated
water as a lower layer. The batch process was continued for 3 hr to recover the total oil. Heating was
stopped after completion of process. The oil settled in the graduated glass column forming upper
layer, was measured to 16 ml with a recovery of 0.53 and collected, by opening a valve (18~ and
121/1651
draining out the oil saturated water first then collecting the oil through the outlet (23) in a separate
container. The water droplets in the oil are dried with anhydrous sodium sulphate.
Simultaneously, 2 kg of same plant material Tagetes minuta was charged into the
Clevenger type apparatus and distilled for 3 hr. After completion of the process the oil yielded was
recorded as 6 ml with a recovery of 0.3 %. Thus, the efficiency of the present invention was 1.5 times
the Clevenger type apparatus. The quality analysis was done by gas chromatographic analysis and
the results are given below in Table No 2.
Table 2
Constituents Present invention (%) Prior art (%)
(Mini distillation (Clevenger apparatus)
apparatus)
Ocimene 38.13 36.41
Dihydrotagetone 28. 65 13. 95
E-Tagetone0. 98 0. 9
Z-Tagetone 9. 88 9. 53
E-Ocimenone 10.9 7.3
Z-Ocimenone 11.2 6.2
The oil distilled by apparatus of the present invention was of improved quality as compared to oil
distilled using Clevenger apparatus, as can be seen from the results with respect to constituents as
given in Table 2 above.
Dihydrotagetone was found 28.6% in mini distillation unit and less (13.9%) in Clevenger oil. Similarly,
E and Z ocimenones are found in higher percentage (10.9% and 11.2%) as compared to Clevenger
oil distilled which was in low percentage. In the case of tagetones, the marginal variations was found
in E-tagetone which is also one of the quality determining constituents.
The overall quality of oil distilled from mini distillation unit was found better than distilled from
Clevenger apparatus.
122/1651
The main advantages of the present invention are: 1. The unit is useful for the distillation of essential
oils and perfumed water from a number of aromatic herbs available in applicants surroundings such
as Basil, Kari patta, Ajowain, Eucalyptus, Mints. Citrus peels, Muskbala, Bachh, Wild Marigold and
cultivated aromatic crops like Damask rose. Lavender. Marigold and
Chamomile.
2. The plant material can be distilled at atmospheric pressure and also at higher or lower pressures
than atmospheric pressure, with all the three-hydro distillation methods.
3. The unit is portable and can be used in the fields where water and power sources are available.
4. Water distillation. Steam distillation and Water and Steam distillation can be done.
5. Household cottage industry for marginal farmers and housewives.
6. Can be used for demonstration, training and education purpose in R & D-and
Educational institutes.
7. Employment and income generation for economically backward classes.
8. This apparatus has been designed to meet the needs of small growers and entrepreneurs who
wish to start at a small scale and to learn the art, skill and science of essential oil production at an
affordable price.
9. The qualitative and quantitative yields are better than the Clevenger type apparatus.
10. The unit being quite inexpensive and sturdy, even small farmers can in, tall their individual
units.Claims:
Claims 1. A simple, convenient, portable mini-distillation apparatus for the production of essential oils
and hydrosols, which comprises one or more vessel (s) (1) capable of being heated either
intemally/externally or both, the inside bottom of the said vessel (s) being provided with a threaded
rod (6) fixed concentrically in such a manner so as to allow vertical movement of a sieved false
bottom (5), one or more steam spurger (s) (24) being provided between the vessel bottom (2) and
123/1651
the said movable false bottom (5,7), the said vessel (s) being provided with lids (s) (3) having one or
more safety valve (s) (21), said lid (s) being attached with the vessel by means of removable fixing
means, the lid (s) are also provided with parameter gauges (20) such as pressure, vacuum,
temperature gauges and a vapor outlet (s) (9), the said vapor outlet (s) being connected by known
means to the inlet of one or more vertical cohobation column (s) (8), the outlet (s) of the said
cohobatiion column (s) being fixed by known means to the inlet (10) of a condenser (11) provided
with closeable vent (15), the outlet (12) of the said condenser being detachably connected by one or
more connecting means (14) to a vertical receiver cum-separator column (13) having a valve (18) at
its lower end, which controls an outlet (23), the bottom and middle of the said receiver-cum-separator
column being provided with a plurality of valves (17,19) which control flow of fluids in one or more
recycling means (16) connected to the upper portion of the said cohobation column (s).
2. An apparatus as claimed in claim 1 wherein the false bottom (5) in the vessel (1) is used to hold
the plant material to be distilled by adjusting at a suitable height to accommodate the material.
3. An apparatus as claimed in claim 1 wherein, when the apparatus used in water distillation method,
the false bottom (5) is removed completely from the vessel (1) or kept at the lowest possible height
from the base and then the plant material is charged along with water for processing and the plant
material is immersed in water.
4. An apparatus as claimed in claim 1 wherein, when the apparatus is used in water and steam
distillation method, the level of the water charged in the vessel (1) is kept below the false bottom (5)
and the plant material is charged over the false bottom (5) which is adjusted by revolving clockwise
or anti-clockwise as the case may be on the threaded rod (6), the false bottom (5) here is used to
separate the plant material and water.
5. An apparatus as claimed in claim 4 wherein, the false bottom (5) is so adjusted to accommodate
the plant material which is very less to distil in a given capacity of distillation unit preferably atleast
one fifth of the holding capacity of the unit to minimise or no less of essential oil.
6. An apparatus as claimed in claim 1 comprising steam spurger (24) having holes is provided below
the false bottom (5) in the vessel (1) and when steam is injected into the vessel through the steam
spurger for distilling the plant material which is kept on the false bottom by steam distillation method.
124/1651
7. An apparatus as claimed in claim 1 wherein the vessel is heated internally by means of known
heating system preferably electrical system and externally by any conventional/non-conventional
heating means/sources selected from fire woods, coal, oil, gas burners, boilers etc.
8. An apparatus as claimed in claim 1, wherein the vessel has a height to diameter ratio in the range
of 0.5 to 1.5.
9. An apparatus as claimed in claim 1, wherein the vessel, cohobation column, condenser and
recycling pipes are made up of metals selected from stainless steel, copper, tin.
10. An apparatus as claimed in claim 1, wherein the receiver-cum-separator is made up of glass,
coated with transparent plastic or covered with an aluminium casing.
11. An apparatus as claimed in claim 1 wherein, the vertical receiver-cum-separator column is
graduated.
12. An apparatus as claimed in claim 1, wherein the closeable vent (15) of the condenser is
optionally connected through a valve to a vacuum pump.
13. An apparatus as claimed in claim 1 wherein, the cohobation column is connected to the vessel,
condenser by means of clamps with or without gaskets, O-rings, threaded arrangements with or
without gaskets.
14. An apparatus as claimed in claim 1 wherein, the condensing means is any conventional means
such as water or air cooling condenser.
15. An apparatus as claimed in claim 1, wherein the vessel is provided with handles.
16. An apparatus as claimed in claim 1, wherein the steam spurger (24) is connected to one or more
external steam sources such as boilers.
17. An apparatus as claimed in claim 1 wherein, the fluids a escaping from the condenser may be
recirculated to the vessel (1) or collected in separate containers using known means.
125/1651
30. CN1410522 - 16.04.2003
METHOD OF EXTRACTING ESSENTIAL OIL AND NATURAL BENZALDEHYDE FROM FRUIT SKIN
AND FRUIT PULP OF GARLIC FRUIT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN1410522
Inventor(s):
LI PIAOYING (CN); LI WEIGUANG (CN); LIU XIONGMIN (CN)
Applicant(s):
UNIV GUANGXI (CN)
IP Class 4 Digits: C11B
IP Class:
C11B1/16
Application Number:
CN20020139271 (20021109)
Priority Number: CN20020139271 (20021109)
Family: CN1410522
Abstract:
A PROCESS FOR EXTRACTING REFINED OIL AND NATURAL BENZALDEHYDE FROM THE PEEL
AND PULP FOR OILY MALANIA INCLUDES SUCH STEPS AS STEAM-DISTILLING TO EXTRACT
REFINED OIL OF OILY MALANIA, AND REFRICTING, SEPARATING AND PURIFYING THE SAID
REFINED OIL TO OBTAIN NATURAL BENZALDEHYDE. ITS ADVANTAGES ARE ABUNDANT RAW
MATERIAL SOURCE, HIGH OUTPUT RATE, AND LOW COST.
126/1651
31. CN1467274 - 14.01.2004
ANTIBIOTIC PLANT ESSENTIAL OIL, PERFUME AND SCENTED TEA
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN1467274
Inventor(s):
HAO JIANPING (CN)
Applicant(s):
HAO JIANPING (CN)
IP Class 4 Digits: C11B; A01N
IP Class:
C11B9/00; A01N65/00; A01N25/18
Application Number:
CN20030140542 (20030528)
Priority Number: CN20030140542 (20030528)
Family: CN1467274
Abstract:
AN ANTIBACTERIAL VEGETABLE ESSENCE IN THE FORM OF OIL, LIQUID, OR FLAKE FOR
KILLING THE HARMFUL BACTERIA IN AIR AND PREVENTING INFECTIOUS DISEASES IS
PREPARED FROM THE ACTIVE COMPONENTS EXTRACTED FROM PLANTS. ITS ADVANTAGES
ARE HIGH EFFECT, GREABLE AND REFRESHING SMELL, AND NO TOXIC BY-EFFECT.
127/1651
32. CN1488290 - 14.04.2004
GINGER ESSENTIAL OIL AND/OR OILY RESIN MICROCAPSULE AND PREPARING PROCES
THEREOF
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN1488290
Inventor(s):
WU SULING (CN); JIN JINGHONG (CN); SUN XIAOMING (CN)
Applicant(s):
NANJING WILD PLANT COMPREHENSI (CN)
IP Class 4 Digits: A23L
IP Class:
A23L1/221
Application Number:
CN20030132345 (20030815)
Priority Number: CN20030132345 (20030815)
Family: CN1488290
128/1651
33. CN2210191 - 18.10.1995
HIGH EFFICIENCY DISTILLATION MEANS FOR ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN2210191
Inventor(s):
ZHICHAO LIU (CN)
Applicant(s):
YIBIN PREFECTURE FOREST SCIENC (CN)
IP Class 4 Digits: C11B
IP Class:
C11B9/02; C11B1/16
Application Number:
CN19940230087U (19941222)
Priority Number: CN19940230087U (19941222)
Family: CN2210191
129/1651
34. CN85102662 - 24.09.1986
METHOD FOR OBTAINING PECTINE FROM PEELS OF ORANGES AND TANGERINES AND
PRODUCING WINE, ESSENTIAL OIL, JAM, PIGMENT AND PEEL GLUCOSIDE SIMULTANEOUSLY
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CN85102662
Inventor(s):
- (--)
Applicant(s):
- (--)
IP Class 4 Digits: A23L
IP Class:
A23L1/222; A23L1/04; A23L1/064
Application Number:
CN19850102662 (19850401)
Priority Number: CN19850102662 (19850401)
Family: CN85102662
Equivalent:
CN1003208
130/1651
35. CZ287992 - 14.03.2001
PROCESS FOR PREPARING CHAMOMILE ESSENTIAL OIL WITH TOTAL CONTENT OF NATURAL
CIS- AND TRANS-SPIROETHERS OF AT LEAST 1 PERCENT BY WEIGHT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=CZ287992
Inventor(s):
CARLE REINHOLD DR (DE); ISAAC OTTO DR (DE)
Applicant(s):
ASTA MEDICA AG (DE)
IP Class 4 Digits: A61K; C11B
IP Class:
A61K35/78; C11B9/02
Application Number:
CZ19880000867 (19880211)
Priority Number: CZ19880000867 (19880211)
Family: CZ287992
Equivalent:
CZ8800867
Abstract:
CAMOMILE OIL WITH A CONTENT OF NATURAL CIS- AND TRANS SPIRO ETHERS OF, IN TOTAL,
AT LEAST 1 WT.%, IS NEW. THE CAMOMILE OIL CAN BE PREPD. BY STEAM DISTN. OR DISTN.
WITH WATER OF FRESH CAMOMILE OR EXTN. RESIDUES FROM CAMOMILE EXTN. WATER DISTN.
IS PREF. CARRIED OUT AT PH 4-8, OPT. IN THE PRESENCE OF REDUCTANTS. THE EXTRACTS
PREF. CONTAIN CIS AND TRANS SPIRO ETHERS IN A TOTAL AMT. OF AT LEAST 1.0 MG/100G
EXTRACT, ESP. AT LEAST 0.5MG CIS AND 0.3MG TRANS SPIRO ETHER PER 100G EXTRACT. THE
RESULTING CAMOMILE OIL PREF. CONTAINS AT LEAST 1 WT.% CIS AND 0.5 WT.% TRANS
SPIRO ETHER, AND CAN BE ADDED TO ANY PHYSIOLOGICALLY ACCEPTABLE SOLVENT TO
GIVE MORE CAMOMILE EXTRACT.
131/1651
36. DE10011344 - 20.09.2001
PRESSURIZED GAS FOAM SPRAY CONTAINING ESSENTIAL OIL, USEFUL MEDICINALLY OR
COSMETICALLY FOR TREATING SKIN DISEASES, IS STABLE, EASILY APPLIED AND
HYPOALLERGENIC
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE10011344
Inventor(s):
MARSCHALL GERHARD VON (DE)
Applicant(s):
KRUEGER GMBH and CO KG (DE)
IP Class 4 Digits: A61K
IP Class:
A61K7/48; A61K9/12
E Class: A61K8/92C; A61Q19/00; A01N65/00+M; A61K9/12B; A61K8/04F
Application Number:
DE20001011344 (20000310)
Priority Number: DE20001011344 (20000310)
Family: DE10011344
Abstract:
A PRESSURIZED GAS FOAM SPRAY (A) FOR MEDICINAL OR COSMETIC USE CONTAINS AN
ESSENTIAL OIL (I) AS ACTIVE AGENT, TOGETHER WITH CONVENTIONAL PROPELLANTS AND
BASE COMPONENTS FOR FOAM SPRAYS. AN INDEPENDENT CLAIM IS INCLUDED FOR THE USE
OF (I) FOR THE PREPARATION OF A PRESSURIZED GAS FOAM SPRAY FOR TOPICALLY USE ON
THE HUMAN SKIN.Description:
Die Erfindung betrifft pharmazeutische oder kosmetische Prдparate in Form eines DruckgasSchaumsprays mit einem Gehalt an дtherischen Цlen.
132/1651
Дtherische Цle werden hдufig als Wirkstoffe in Arzneimitteln zur дusserlichen Anwendung, vor
allem bei Erkдltungskrankheiten, verwendet. Die Applikation der Цle erfolgt dabei entweder direkt in
Form des reinen Цls oder in Form flьssiger (Lцsungen) oder halbfester (Salben, Cremes)
Darreichungsformen.
Sprays werden im Arzneimittelbereich ьberwiegend zum Versprьhen von Lцsungen oder
Feststoffen verwendet. Bekannt ist vor allem die Zerstдubung von festen oder flьssigen
Arzneistoffen zur pulmonalen Applikation bzw. Inhalation (Asthmasprays).
Дtherische Цle sind stark lipophile, sehr dьnnflьssige, pflanzliche Wirkstoffe. Aufgrund ihrer
niedrigen Viskositдt sind sie in reiner Form sehr schlecht dosier- und applizierbar. Dies trifft auch auf
Verdьnnungen von дtherischen Цlen in fetten Цlen, wie Erdnussцl, zu, die ebenfalls noch sehr
niedrigviskos sind und gleichermassen nur ungenьgend eine punktuelle Applikation ermцglichen.
Дtherische Цle kцnnen prinzipiell in Salben eingearbeitet werden. Um ausreichende
Wirkkonzentrationen erzielen zu kцnnen, mьssen jedoch stark lipophile Grundlagen verwendet
werden. Solche Grundlagen haben jedoch auf geschдdigte Haut, insbesondere bei offenen Wunden,
einen unerwьnschten Okklusionseffekt. Zudem wird eine Salbe bei der Entnahme sehr leicht
mikrobiell kontaminiert, was den Einsatz ausreichender Mengen an Konservierungsstoffen erfordert,
die wiederum das Nebenwirkungs- und Allergiepotential von solchen Salben erhцhen.
Zudem erfolgt bei jeder Entnahme ein Zutritt von Sauerstoff, und es entstehen oxidationsbedingte
Abbauprodukte, welche die Qualitдt und Unbedenklichkeit der Zubereitung gefдhrden kцnnen.
Die gдngigen, pharmazeutischen Darreichungsformen fьr eine Applikation auf der Haut sind oft
schlecht handhabbar, erfordern zumindest zum Цffnen - bei Lцsungen auch zur Applikation - beide
Hдnde, und die verwendeten Packmittel sind oft nicht ausreichend stabil fьr einen mobilen Einsatz,
der bei einem derartigen Produkt wьnschenswert ist.
Es ist bekannt, dass дtherische Цle antimikrobielle Eigenschaften haben. Sie finden dennoch heute
nur begrenzt Einsatz als antiseptische oder antibiotische Wirkstoffe in Dermatika. Dies beruht im
wesentlichen auf zwei Faktoren:
133/1651
a) Bis vor wenigen Jahren standen in rascher Folge immer potentere, synthetische Antibiotika zur
Verfьgung, die praktisch alle therapeutischen Anwendungen abdeckten.
b) Einigen дtherischen Цlen wird ein allergenes Potential zugeschrieben.
In beiden Punkten sind jedoch in den letzten Jahren deutliche Verдnderungen eingetreten:
Zu a)
In zunehmendem Mass traten in den letzten Jahren Erregerstдmme auf, die gegen einen Grossteil
der zur Verfьgung stehenden, spezifisch wirkenden Antibiotika resistent sind. Weltweit besteht daher
ein ausserordentlich grosses Interesse an therapeutischen Alternativen, die auf anderen
Wirkmechanismen beruhen. Дtherische Цle nehmen hier als potentielle Alternativen einen hohen
Stellenwert ein.
Zu b)
Neuere Untersuchungen belegen fьr einige дtherische Цle, dass nicht die nativen Цle an sich ein
allergenes Potential besitzen, sondern dass dieses auf bei unsachgemдsser Lagerung bzw.
ungeeigneter, galenischer Formulierung entstehenden Oxidationsprodukten beruht (vergl. z. B. M.
Harkenthal et al., "Pharmazie PZ", Bd. 143 (Nr. 47 (1988), S. 4092-4096).
Aufgabe der Erfindung ist es, eine sichere und patientenfreundliche Dosierung und Applikation von
дtherischen Цlen in einem weiten Konzentrationsbereich von wenigen Zehntel% bis ьber 25% zu
ermцglichen. Dabei soll ein Schutz der enthaltenen, дtherischen Цle vor Sauerstoffeinwirkung
mцglichst weitgehend gewдhrleistet werden, eine mikrobielle Kontamination des Inhalts vermieden
werden und damit ein Zusatz von Konservierungsmitteln und Antioxidantien unterbleiben.
Gegenstand der Erfindung sind Prдparate fьr medizinische oder kosmetische Zwecke in Form eines
Druckgas-Schaumsprays, das mindestens ein дtherisches Цl als Wirkstoff sowie ьbliche Treibgase
und Grundstoffe fьr Schaumsprays enthдlt.
134/1651
Die Verarbeitung eines дtherischen Цls zu einem Druckgas-Schaumspray vereint dabei in idealer
Weise die Erfordernisse einer sicheren und anwenderfreundlichen Dosier- und Applizierbarkeit mit
der Gewдhrleistung eines grцsstmцglichen Schutzes des Produkts vor mikrobieller Kontamination
und Oxidation.
Insbesondere bieten die erfindungsgemдssen Prдparate folgende Vorteile:
- Das Verpackungsmaterial gewдhrleistet einen dauerhaften Lichtschutz, und zwar auch dann
noch, wenn die Packung bereits angebrochen ist.
- Sauerstoff wird aus der mit Fьllgut beaufschlagten Dose vor Zugabe des Treibgases und vor dem
Verschliessen der Dose verdrдngt.
- Ein erneuter Zutritt von Sauerstoff wird durch das Prinzip der Spraydose dauerhaft verhindert.
- Die Applikation als Schaum gewдhrleistet erhebliche Vorteile, wie gute Verteilbarkeit bei geringer,
mechanischer Belastung, geringe galenische Stabilitдtsprobleme trotz hohen Wirkstoffanteils, gute
Haftung des Produktes am Applikationsort und dergl.
- Eine mikrobielle Kontamination wird durch den Ьberdruck verhindert. Dadurch lдsst sich der
Einsatz von Konservierungsmitteln weitgehend vermeiden.
- Дtherische Цle werden fьr die Behandlung von Wunden und infizierten Hautprozessen
verfьgbar gemacht.
Insbesondere hat es sich herausgestellt, dass Teebaumцl, ein дtherisches Цl aus den Blдttern des
australischen Цlbaums (Melaeuca alternifolia L.), als Wirkstoff fьr die erfindungsgemдssen
Prдparate geeignet ist. Jedoch kommen auch beliebige andere, дtherische Цle, fьr die die
vorgenannten Kriterien gelten, in Frage. Beispiele hierfьr sind:
Pfefferminzцle
Eukalyptusцl
Thymianцl
Lavendelцl
Rosmarinцl
Coniferenцle
Melissenцl
Zitronellenцle
135/1651
Zitronenцl
Erfindungsgemдss wird insbesondere der Vorteil erzielt, dass das noch weitgehend ungenutzte
Potential bestimmter дtherischer Цle, insbesondere von Teebaumцl, zur Behandlung von
Hauterkrankungen in einer standardisierten, sicheren, gut vertrдglichen und
verbraucherfreundlichen, damit compliance-fцrdernden Form zugдnglich gemacht wird.
Die erfindungsgemдsse Darreichungsform eignet sich somit insbesondere auch:
- fьr andere oxidations- und lichtempfindliche Arzneistoffe,
- zur Herstellung hypoallergener Arzneimittel und Kosmetika und
- fьr Arzneimittel (und Kosmetika), bei denen eine besonders niedrige mikrobielle Belastung bei
gleichzeitiger Vermeidung von Konservierungsmitteln erforderlich ist, insbesondere solche zur
Anwendung auf geschдdigter Haut.
Es liegen bereits positive Erfahrungsberichte von Versuchspersonen vor, die das
erfindungsgemдsse Produkt des nachstehenden Beispiels 1 erprobt haben. Es wird als wirksam und
sehr gut vertrдglich beschrieben.
Eine erfindungsgemдsse Rezeptur kann beispielsweise folgende Bestandteile in geeigneten
Mengen enthalten:
Wasser
Polyoxyethylen-Fettalkoholether
Polyoxyethylen-Fettsдureester
Polyoxyethylensorbitanfettsдureester
Sorbitanfettsдureester
Glyzerolfettsдureester
Sterole
Zuckertenside, z. B. Saccharosefettsдureester
Lecithine
Betaine
Polyethylenglykolfettsдureester
Polyethylenglykolfettalkoholether
136/1651
Cetylalkohol
Cetylstearylalkohol
emulgierender Cetylstearylalkohol
Macrogole (Polyethylenglykole)
Natriumhydroxid
Acrylamid-Copolymere (z. B. Carbomere)
Propan
Butan
CO2
Stickstoff
1,2-Propylenglykol
Paraffin
Glycerylhydroxylstearat
Der Anteil des дtherischen Цls in den Prдparaten kann innerhalb weiter Grenzen variieren und
beispielsweise 0,5 bis 25% und insbesondere 5 bis 15% betragen.
Nachstehend werden beispielhafte Rezepturen aufgefьhrt.
Beispiel 1
Zur Herstellung eines Prдparats wird das Wasser auf 80 DEG C erwдrmt. Die Emulgatoren (Pos. 2 +
3) und der Gelbildner (Pos. 4) werden auf 85 DEG C erwдrmt und mit dem Wasser vermischt. Das
Gemisch wird homogenisiert, auf 50 DEG C abgekьhlt und sodann mit dem Teebaumцl und der
Natronlauge versetzt. Nach erneutem Homogenisieren lдsst man das Gemisch auf 30 DEG C
abkьhlen.
Die erhaltene Mischung wird unter Verwendung eines Gemisches aus Propan und Butan (Verhдltnis
3 : 5) unter Ьberdruck in Spraybehдltnisse aus innenbeschichtetem Aluminium oder anderen
geeigneten Materialien mit Ьberkopfsprayaufsatz gefьllt.
Beispiel 2
137/1651
Die Bestandteile 8, 9 und 10 werden bei 80 DEG C zusammengeschmolzen. Etwa 85% des
Bestandteils 1 werden bei 80 DEG C zugegeben. Anschliessend wird langsam unter Rьhren der
Bestandteil 4 zugesetzt. Sodann wird homogenisiert und gleichzeitig der Bestandteil 2 eingesaugt.
Hierauf lдsst man das Gemisch unter Bildung einer Voremulsion auf 35-45 DEG C abkьhlen.
In einem anderen Behдlter werden die Bestandteile 5, 6 und 7 und die Restmenge Wasser bei 45
DEG C vermischt und homogenisiert. Das Gemisch wird anschliessend in die Voremulsion
eingerьhrt. Nach Homogenisieren unter Vakuum wird mit dem Bestandteil 3 ein pH-Wert von 6
eingestellt.
Die erhaltene Mischung wird unter Verwendung eines Gemisches aus Propan und Butan (Verhдltnis
3 : 5) unter Ьberdruck in Spraybehдltnisse aus innenbeschichtetem Aluminium oder anderen
geeigneten Materialien mit Ьberkopfsprayaufsatz gefьllt.Claims:
1. Druckgas-Schaumspray fьr medizinische oder kosmetische Zwecke, enthaltend ein дtherisches
Цl als Wirkstoff sowie ьbliche Treibgase und Grundbestandteile fьr Schaumsprays.
2. Druckgas-Schaumspray nach Anspruch 1, dadurch gekennzeichnet, dass der Anteil des
дtherischen Цls 0,5-25% (m/m) betrдgt.
3. Druckgas-Schaumspray nach einem der Ansprьche 1 oder 2, dadurch gekennzeichnet, dass es
als дtherisches Цl Teebaumцl enthдlt.
4. Verwendung von дtherischen Цlen zu Herstellung von Druckgas- Schaumsprays zur topischen
Anwendung auf die menschliche Haut.
138/1651
37. DE10042710 - 28.03.2002
BUTTER-BASED DERMATOLOGICAL OR COSMETIC PREPARATION E.G. MILKING GREASE,
CONTAINS ESSENTIAL OIL TO PROVIDE BACTERIOSTATIC AND/OR BACTERICIDAL ACTIVITY
AND PLEASANT ODOR
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE10042710
Inventor(s):
KELLER PETER (DE)
Applicant(s):
KELLER PETER (DE)
IP Class 4 Digits: A61K
IP Class:
A61K7/48; A61K35/12
E Class: A61K8/92C; A61Q19/00; A61K35/20; A61K8/33; A61K8/49H2; A61K8/98C8; A61Q1/04;
A61Q17/04
Application Number:
DE20001042710 (20000831)
Priority Number: DE20001042710 (20000831)
Family: DE10042710
Abstract:
DERMATOLOGICAL OR COSMETIC PREPARATION (A), BASED ON MAMMALIAN BUTTER,
CONTAINS ESSENTIAL OIL(S) (I) HAVING BACTERIOSTATIC AND/OR BACTERICIDAL ACTIVITY
AND A CHARACTERISTIC PLEASANT ODOR (OR COMPONENT(S) OF THE OILS).Description:
Die vorliegende Erfindung betrifft eine neue dermatologische oder kosmetische Zubereitung auf der
Basis von Sдugetierbutter. Ausserdem betrifft die vorliegende Erfindung die Herstellung der neuen
dermatologischen oder kosmetischen Zubereitung. Des weiteren betrifft die vorliegende Erfindung
die Verwendung der neuen dermatologischen oder kosmetischen Zubereitung.
139/1651
Die Verwendung von Butterfett fьr die Herstellung dermatologischer und kosmetischer
Zubereitungen ist bekannt. Den Zubereitungen mьssen Stabilisatoren wie 1,2- Propylenglykol
zugesetzt werden, um sie vor dem chemischen oder dem bakteriellen Abbau zu bewahren. Indes
weisen die bekannten Stabilisatoren Nachteile auf, wie beispielsweise eine Hautunvertrдglichkeit, ein
hohes allergisches Potential und/oder eine vergleichsweise hohe Toxizitдt.
Die Verwendung von Butter in Melkfett ist aus dem deutschen Gebrauchsmuster 298 03 691.6
bekannt. Die darin beschriebenen Zubereitungen enthalten Butter, Wasser sowie ьbliche und
bekannte Zusatzstoffe wie Antioxidantien, Konservierungsmittel und Emulgatoren, insbesondere
Ascorbinsдure, Nipagin, Teebaumцl, Benzoesдure, Cetylalkohol, Lecithin und/oder Bienenwachs.
Dieses bekannte Melkfett weist gegenьber Melkfetten mit hohen Anteil an Mineralцlen den Vorteil
auf, dass auf den Kuheutern keine Schichten unlцslicher und/oder nicht biologisch abbaubarer
Schichten zurьckbleiben, die den Austritt von Schweiss verhindern und so zu einer Erkrankung der
Tiere fьhren kцnnen.
Nachteilig ist jedoch, dass dieses bekannte Melkfett in seiner bakteriostatischen und/oder
bakteriziden Wirkung und der Einstellung angenehmer Duftnoten zu wьnschen ьbrig lдsst, was
seiner breiten Anwendung in der Dermatologie und der Kosmetik entgegensteht.
Zwar liesse sich die bakteriostatische und/oder bakterizide Wirkung und der Duft ьber synthetische
Zusatzstoffe einstellen, indes ginge dann ein ganz wertvoller Vorteil des bekannten Melkfetts verloren,
dass es nдmlich ьberwiegend, wenn nicht sogar ausschliesslich, aus natьrlichen, nachwachsenden
Rohstoffen hergestellt werden kann.
Aufgabe der vorliegenden Erfindung ist es, eine neue dermatologische oder kosmetische
Zubereitung zu finden, die die Nachteile des Standes der Technik nicht mehr lдnger aufweist,
sondern die stabil gegenьber dem bakteriellen Abbau ist, eine sehr gute bakteriostatische und/oder
bakterizide Wirkung hat, eine angenehme charakteristische Duftnote aufweist, auf den Gebieten der
Dermatologie und der Kosmetik breit angewandt werden kann und ьberwiegend, wenn nicht gar
ausschliesslich, aus natьrlichen, nachwachsenden Rohstoffen hergestellt werden kann.
Demgemдss wurde die neue dermatologische oder kosmetische Zubereitung gefunden, die
mindestens ein bakteriostatisch und/oder bakterizid wirkendes, charakteristisch angenehm
140/1651
duftendes etherisches Цl und/oder mindestens einen Bestandteil hiervon enthдlt und die im
folgenden als "erfindungsgemдsse Zubereitung" bezeichnet wird.
Die erfindungsgemдsse Zubereitung wird auf der Basis von Sдugetierbutter hergestellt. Hierbei
kann die Sдugetierbutter, so wie sie bei ihrer Herstellung anfдllt, ohne vorhergehende
Entwдsserung oder einer chemischen Vorbehandlung direkt zur Herstellung der
erfindungsgemдssen Zubereitung verwendet werden, was ein weiterer besonderer Vorteil der
erfindungsgemдsse Zubereitung ist. Vorzugsweise wird die Sдugetierbutter zur Herstellung der
erfindungsgemдssen Zubereitung auf 70 bis 80 DEG C erhitzt.
Im Rahmen der vorliegenden Erfindung ist unter Sдugetierbutter die Butter zu verstehen, die aus der
Milch von Sдugetieren in ьblicher und bekannter Weise gewonnen wird. Vorzugsweise wird Kuh-,
Stuten-, Schafs- oder Ziegenmilch oder Gemische hiervon, besonders bevorzugt Kuhmilch, fьr die
Herstellung der Sдugetierbutter verwendet.
Der Gehalt der erfindungsgemдsse Zubereitung an Butter kann sehr breit variieren. Er richtet sich
vor allem danach, wieviel dermatologisch gut vertrдgliches Fett und Цl fьr die jeweilige Anwendung
oder Indikation notwendig sind. Vorzugsweise liegt der Gehalt bei 1 bis 60, bevorzugt 2 bis 55,
besonders bevorzugt 3 bis 50, ganz besonders bevorzugt 4 bis 45 und insbesondere 5 bis 40 Gew.%, jeweils bezogen auf die erfindungsgemдsse Zubereitung.
Der erfindungswesentliche Bestandteil der erfindungsgemдssen Zubereitung ist mindestens ein
bakteriostatisch und/oder bakterizid wirkendes, charakteristisch duftendes etherisches Цl und/oder
mindestens ein Bestandteil hiervon. Hierbei werden insbesondere die Bestandteile der etherischen
Цle verwendet, die deren Eigenschaftsprofil prдgen.
Unter etherischen Цlen werden Цle verstanden, die vorzugsweise aus nachwachsenden Rohstoffen,
insbesondere Pflanzen, hergestellt werden. Vorzugsweise werden die etherischen Цle aus
Gewьrzpflanzen hergestellt.
Die erfindungsgemдss zu verwendenden etherischen Цle weisen einen charakteristischen Duft auf.
Vorzugsweise haben sie einen angenehmen charakteristischen Duft, der die Handhabung und
Anwendung, insbesondere die Langezeitanwendung, ermцglicht. Ausserdem dient der angenehme
charakteristische Duft bzw. die Duftnote gewissermassen der Kennzeichnung der betreffenden
erfindungsgemдsse Zubereitung.
141/1651
Darьber hinaus haben die erfindungsgemдss zu verwendenden etherischen Цle eine
bakteriostatische Wirkung. Hierunter ist die konzentrationsabhдngige Fдhigkeit einer Substanz zu
verstehen, die Vermehrung von Keimen zu verhindern, ohne diese abzutцten; die geschдdigten
Keime kцnnen sich nach Einbringen in frische Nдhrmedien wieder vermehren (vgl. Pschyrembel,
Klinisches Wцrterbuch, 258. neubearbeitete Auflage, Walter de Gruyter, Berlin, New York,
1998, >>Bakteriostase<>Bakterizidie< 1.000 nm vorliegen, oder um eine Miniemulsion oder
Mikroemulsion handeln kann. Mikro- und Miniemulsionen sind Dispersionen aus Wasser, einer
Цlphase und einer oder mehreren oberflдchenaktiven Substanzen, die eine Trцpfchengrцssen von
5 bis 50 nm (Mikroemulsion) oder von 50 bis 500 nm (Miniemulsion) aufweisen (vgl. Emulsion
Polymerization and Emulsion Polymers, Editoren. P. A. Lovell und Mohamed S. El-Aasser, John Wiley
and Sons, Chichester, New York, Weinheim, 1997, Seiten 700 und folgende; Mohamed S. El-Aasser,
Advances in Emulsion Polymerization and Latex Technology, 30 Annual Short Course, Volume 3,
June 7-11, 1999, Emulsion Polymers Institute, Lehigh University, Bethlehem, Pennsylvania, U.S.A.).
Dabei kann die erfindungsgemдsse Zubereitung die Konsistenz einer mehr oder weniger viskosen
Creme oder Salbe oder einer leicht- bis zдhflьssigen Flьssigkeit haben.
Aufgrund ihrer besonderen vorteilhaften Eigenschaften, insbesondere ihrer vorzьglichen
Hautvertrдglichkeit und Langzeitsstabilitдt gegenьber dem bakteriellen Abbau, kann die
erfindungsgemдsse Zubereitung in der Kosmetik und Kцrperpflege angewandt werden.
Insbesondere dient sie der Pflege der menschlichen und tierischen Haut oder der Pflege
menschlicher und tierischer Nдgel, als Sonnenschutzcreme, Lippenbalsam oder als Gleitcreme,
vorzugsweise als Lippenbalsam und Melkfett, insbesondere als Melkfett.
Ausserdem kann die erfindungsgemдsse Zubereitung fьr die Herstellung von Mitteln zur
Behandlung und Prophylaxe von menschlichen und tierischen Krankheiten verwendet werden.
Insbesondere kann sie zur Herstellung von Mitteln zur Behandlung von Wunden, Narben und
Hautkrankheiten sowie von Mitteln zur prophylaktischen Behandlung der menschlichen und
tierischen Haut eingesetzt werden.
Beispiel
142/1651
Die Herstellung eines erfindungsgemдssen Melkfetts
Es wurde ein Melkfett auf der Basis von Kuhbutter aus den folgenden Bestandteilen durch
Vermischen und Homogenisieren hergestellt:
25 Gew.-% Butter,
62,6 Gew.-% deionisiertes Wasser,
2 Gew.-% Cetylalkohol,
2 Gew.-% Bienenwachs, rein,
8 Gew.-% Fluidlecithin CM,
0,1 Gew.-% Ascorbinsдure,
0,1 Gew.-% Benzoesдure und
0,2 Gew.-% Vanillin aus Vanilleschoten.
Das resultierende Melkfett war eine cremeartige, weisse Emulsion mit einem angenehmen leichten
Vanillinegeruch. Das Melkfett neigte auch nach mehrwцchiger Lagerung bei hцheren Temperaturen
nicht zur Entmischung seiner Bestandteile. Es war aufgrund seiner bakteriostatischen Wirkung
ausgesprochen stabil gegenьber dem bakteriellen Abbau. Die Bakteriostase wirkte sich aus
ausgesprochen positiv auf die Haut der Kuheuter und die exponierte Haut der Melker aus. Auch
nach mehrmonatiger Lagerung an der Luft wurde das erfindungsgemдsse Melkfett nicht
ranzig.Claims:
1. Dermatologische oder kosmetische Zubereitung auf der Basis von Sдugetierbutter, enthaltend
mindestens ein bakteriostatisch und/oder bakterizid wirkendes, charakteristisch angenehm
duftendes etherisches Цl und/oder mindestens einen Bestandteil hiervon.
2. Zubereitung nach Anspruch 1, dadurch gekennzeichnet, dass es sich bei der Sдugetierbutter um
Butter auf der Basis von Kuh-, Stuten-, Schafs- und/oder Ziegenmilch handelt.
3. Zubereitung nach Anspruch 2, dadurch gekennzeichnet, dass es sich bei der Sдugetierbutter um
Butter auf der Basis von Kuhmilch handelt.
143/1651
4. Zubereitung nach einem der Ansprьche 1 bis 3, dadurch gekennzeichnet, dass man als
bakteriostatisch und/oder bakterizid wirkende, charakteristisch angenehm duftende etherische Цle
Цle auf der Basis von Vanille, Heliotrop, Nelken, Rosmarin, Lavendel, Salbei, Rainfarn, Andorn,
Wacholder, Baldrian, Kalmus, Pfefferminze, Krauseminze, Wermut, Melisse, Johanniskraut, Thymian,
Origanum, Verbena, Chinesischem Zimt, Eukalyptus, Geranium, Bittermandel, Vetifer, Gaultheria,
Indischem Geranium, Spiraea, Sternanis, Iris, Serpyllum, Ceylonzimt, Anis, Betula, Senfцl, Cumium,
Neroli, Ylang, Fenchel, Reseda, Zitrone, Kajepul, Sassafras, Cedron, Petersilie, Veilchen und/oder
Angelica und/oder deren Bestandteile verwendet.
5. Zubereitung nach Anspruch 4, dadurch gekennzeichnet, dass man Цle verwendet, die einen
geringen Gehalt an Campher aufweisen oder campherfrei sind.
6. Zubereitung nach Anspruch 5, dadurch gekennzeichnet, dass man Цle auf der Basis von Melisse,
Johanniskraut und/oder Vanille verwendet.
7. Zubereitung nach einem der Ansprьche 4 bis 6, dadurch gekennzeichnet, dass man
Phenoletheraldehyde enthaltende Цle verwendet.
8. Zubereitung nach Anspruch 7, dadurch gekennzeichnet, dass es sich bei den
Phenoletheraldehyden um Anisaldehyd, Vanillin und/oder Piperonal (Heliotropin) handelt.
9. Zubereitung nach Anspruch 7 oder 8, dadurch gekennzeichnet, dass man Vanillin verwendet.
10. Zubereitung nach Anspruch 9, dadurch gekennzeichnet, dass aus Vanilleschoten hergestelltes
Vanillin verwendet wird.
11. Zubereitung nach einem der Ansprьche 1 bis 10, dadurch gekennzeichnet, dass sie noch
mindestens einen Zusatzstoff enthдlt, wie er in dermatologischen und/oder kosmetischen
Zubereitung ьblicherweise verwendet wird.
12. Verwendung der Zubereitung gemдss einem der Ansprьche 1 bis 11 in der Kosmetik und der
Kцrperpflege.
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13. Verwendung nach Anspruch 12, dadurch gekennzeichnet, dass sie die Pflege der menschlichen
und tierischen Haut oder die Pflege menschlicher und tierischer Nдgel sowie die Verwendung als
Sonnenschutzcreme, Lippenbalsam oder als Gleitcreme, insbesondere als Melkfett, umfasst.
14. Verwendung nach Anspruch 13, dadurch gekennzeichnet, dass die Zubereitung als
Lippenbalsam und als Melkfett verwendet wird.
15. Verwendung der Zubereitung gemдss einem der Ansprьche 1 bis 11 fьr die Herstellung von
Mitteln zur Behandlung und Prophylaxe von menschlichen und tierischen Krankheiten.
16. Verwendung nach Anspruch 14, dadurch gekennzeichnet, dass sie die Herstellung von Mitteln
zur Behandlung von Wunden, Narben und Hautkrankheiten bei Mensch und Tier sowie von Mitteln
zur prophylaktischen Behandlung der menschlichen und tierischen Haut umfasst.
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38. DE10162058 - 24.07.2003
AQUEOUS CLEANING AND DISINFECTING PREPARATION, USEFUL FOR ALLEVIATION OF
HEMORRHOIDS, INTERTRIGO, DECUBITUS AND RELATED DISORDERS, COMPRISES ESSENTIAL
OIL AND COOLING COMPONENTS OF VEGETABLE OR SYNTHETIC ORIGIN
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE10162058
Inventor(s):
POPP CLAUDIA (DE); LEMMERMANN MICHAEL (DE)
Applicant(s):
COSPHARCON GMBH (DE)
IP Class 4 Digits: A61K
IP Class:
A61K35/78; A61K38/05
E Class: A61K35/78
Application Number:
DE20011062058 (20011217)
Priority Number: DE20011062058 (20011217)
Family: DE10162058
Abstract:
AN AQUEOUS PREPARATION (A), FOR CLEANING, MILD DISINFECTION AND SIMULTANEOUS
ALLEVIATION OF ADVERSE SYMPTOMS ASSOCIATED WITH HEMORRHOIDS, ANAL FISSURES,
INFLAMMATION AND POST-OPERATIVE PROBLEMS IN THE ANAL REGION, OR FOR
PROPHYLAXIS OF INTERTRIGO AND DECUBITUS, CONTAINS ESSENTIAL OIL AND COOLING
COMPONENTS (I) OF VEGETABLE OR SYNTHETIC ORIGIN (OR THEIR DERIVATIVES).
146/1651
39. DE10246377 - 15.04.2004
PRODUCTION OF PLASTER USEFUL FOR PROLONGED RELEASE OF ACTIVE AGENT,
ESPECIALLY ESSENTIAL OIL, COMPRISING COATING ONE SIDE OF ABSORBENT CARRIER WITH
ADHESIVE THEN CHARGING OPPOSITE SIDE WITH ACTIVE AGENT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE10246377
Inventor(s):
KLEINHORST ANGELA (DE); SINNEN MARIKE (DE); MOELLER THOMAS (DE)
Applicant(s):
BEIERSDORF AG (DE)
IP Class 4 Digits: A61L
IP Class:
A61L15/44
E Class: A61K9/70E; A61L15/58M+C08L53/02; A61K9/00M20; A61K31/60+M
Application Number:
DE20021046377 (20021004)
Priority Number: DE20021046377 (20021004)
Family: DE10246377
Abstract:
A PLASTER (A) CONTAINING AN ACTIVE AGENT (I) IS PRODUCED BY (A) COATING ONE SIDE OF
AN ABSORBENT CARRIER (II) WITH PRESSURE-SENSITIVE ADHESIVE (III), (B) CHARGING THE
OPPOSITE SIDE OF (II) WITH (I) (OPTIONALLY IN SOLUTION) SO THAT (II) TAKES UP (I), (C)
COVERING THE WHOLE WIDTH OF THE (III)-COATED SIDE OF (II) WITH A (III)-REPELLENT
COATING MATERIAL, AND (D) SEALING THE WHOLE PLASTER IN AIR-TIGHT PACKAGING. AN
INDEPENDENT CLAIM IS ALSO INCLUDED FOR PLASTERS (A) OBTAINED BY THE ABOVE
PROCESS.Description:
[0001] Die vorliegende Erfindung betrifft ein Verfahren zur Herstellung wirkstoffhaltiger Pflaster und
das so hergestellte Pflaster. Das Verfahren umfasst die Beschichtung eines saugfдhigen
Trдgermaterials auf einer Seite mit einer Selbstklebemasse und auf der gegenьberliegenden Seite
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mit einem Wirkstoff oder einer wirkstofthaltigen Lцsung. Das saugfдhige Trдgermaterial nimmt den
Wirkstoff auf und wirkt somit als Wirkstoffreservoir. Die mit Klebmasse beschichtete Seite des
Trдgermaterials wird ьber seine ganze Breite mit einem klebstoffabweisenden Trдgermaterial
abgedeckt und das gesamte Pflaster anschliessend luftdicht eingesiegelt.
Stand der Technik
[0002] Wirkstofthaltige Pflaster zдhlen zu den Drug Delivery Systemen. Es handelt sich um
pflasterartige Arzneiformen, die den Wirkstoff in Form eines Reservoirs enthalten, aus dem die
Wirkstofffreisetzung ьber einen lдngeren Zeitraum nach 0. Ordnung erfolgen kann. Aufgrund dieser
Eigenschaften sind die Drug Delivery Systeme in der Lage, den Organismus unabhдngig von der
Wirkstoftkonzentration im Reservoir ьber einen langen Zeitraum mit konstanten Mengen Wirkstoff pro
Zeiteinheit zu versorgen und werden daher der Gruppe von Retardarzneimitteln zugeordnet.
[0003] Drug Delivery Systeme werden in die Gruppen Topical und Transdermal Delivery eingeteilt.
Die topicalen Formulierungen enthalten Wirkstoffe, deren Freisetzung und Wirkung auf den Bereich
direkt unterhalb und der Umgebung des Orts der Applikation begrenzt ist. Die transdermalen
Formulierungen hingegen enthalten Wirkstoffe, die durch die Haut appliziert werden, um durch das
Eindringen in das Gefдsssystem im gesamten Organismus einen wirksamen Wirkstoffspiegel zu
erzeugen.
[0004] Die fьr Drug Delivery Systeme verwendeten Wirkstoffe sind in der Regel feste oder flьssige
Verbindungen, die ьber die Haut des Organismus oder die Atemluft aufgenommen werden. Zu den
Wirkstoffen, die im Bereich der Kцrpertemperatur in den gasfцrmigen Zustand ьbergehen und
deren Applikation in erster Linie mit der Atemluft erfolgt, zдhlen die дtherischen Цle. Дtherische
Цle und ihre Bestandteile gehen bereits in einem niedrigen Temperaturbereich vom flьssigen in den
gasfцrmigen Zustand ьber, so dass die durchschnittliche Kцrpertemperatur ausreichend ist, um ein
schnelles Verdunsten der дtherischen Цle herbeizufьhren.
[0005] Bei Drug Delivery Systemen (DDS) stellt sich die Aufgabe aufgrund des Wirkstoffreservoirs
eine kontrollierte Freisetzung der дtherischen Цle ьber eine langfristige Applikationszeit zu
erreichen. Bei einer cutanen Applikation von дtherischen Цlen durch flьssige oder halbfeste
Arzneiformen hingegen kann durch Inhalieren und/oder transdermale Effekte lediglich ein
kurzzeitiger therapeutischer Effekt erzielt werden, der eine hдufige Wiederholung der Applikation zur
Folge hat. Zudem besteht bei der Applikation im Bereich der Nase die Gefahr einer starken Reizung
der Schleimhдute.
Aufgabenstellung
148/1651
[0006] Aufgabe der vorliegenden Erfindung ist es, ein Verfahren zur Verfьgung zu stellen, mit dem
sich wirkstoffhaltige Pflaster herstellen lassen, die eine Aufnahme und spдtere Abgabe des
Wirkstoffes gewдhrleisten ohne das die Klebemasse bearbeitet wird und in ihren Eigenschaften
beeintrдchtigt wird.
[0007] Weiterhin besteht die Aufgabe ein Verfahren zur Verfьgung zu stellen, dass es ermцglicht
relativ schnell, einfach und kostengьnstig wirkstoffhaltige Pflaster in einem inline Prozess
herzustellen.
[0008] Gelцst wird die Aufgabe mit einem Verfahren entsprechend dem Hauptanspruch.
Gegenstand der Unteransprьche sind vorteilhafte Ausfьhrungsformen des erfindungsgemдssen
Verfahrens.
[0009] Es war ьberraschend und fьr den Fachmann nicht vorauszusehen, dass ein Verfahren zur
Herstellung eines wirkstoffhaltigen Pflasters indem ein saugfдhiges Trдgermaterial auf einer Seite
mit einer Selbstklebemasse beschichtet wird, auf der gegenьberliegenden Seite mit einem Wirkstoff
oder einer wirkstoffhaltigen Lцsung beaufschlagt wird, so dass das Trдgermaterial eine Menge des
Wirkstoffes oder der wirkstoffhaltigen Lцsung aufnimmt, die mit Klebmasse beschichtete Seite des
Trдgermaterials ьber seine ganze Breite mit einem klebstoffabweisenden Trдgermaterial abgedeckt
wird und das gesamte Pflaster luftdicht eingesiegelt wird, den Nachteilen des Standes der Technik
abhilft.
[0010] Das Verfahren ist zudem ьberraschenderweise einfach und ohne spezielle Maschinen
durchfьhrbar.
[0011] Der Wirkstoff wird entgegen den bekannten ьblichen Verfahrensschritten nicht in die
Selbstklebemasse eingebracht sondern direkt auf das Trдgermaterial aufgebracht. Das
Trдgermaterial kann mit dem Wirkstoff oder dessen Lцsung beaufschlagt, insbesondere besprьht
oder getrдnkt werden. Durch das Beaufschlagen des saugfдhigen Trдgermaterials mit dem
Wirkstoff oder der wirkstoffhaltigen Lцsung lagert sich der Wirkstoff im Trдgermaterial an. Es bildet
sich ein Wirkstoffreservoir im Trдgermaterial, dessen Umfang von der Saugfдhigkeit des
Trдgermaterials, der Aufnahmekapazitдt der Klebemasse, der beaufschlagten Wirkstoffmenge und
den Abmessungen, insbesondere der Dicke, des Trдgermaterials abhдngt.
[0012] Das Trдgermaterial wird entsprechend bekannten Verfahren, beispielsweise ьber
Walzensystemen, gefьhrt und bevorzugt ьber seine gesamte Breite mit dem Wirkstoff oder einer
wirkstoffhaltigen Lцsung besprьht. Dadurch nimmt das Trдgermaterial eine von Auftragmenge,
Durchlaufgeschwindigkeit der Walzensysteme und Saugfдhigkeit des Trдgermaterials
entsprechende Menge an Wirkstoff auf. Ebenso ist die Auftragmenge von der Wirkstoffkonzentration
in der Wirkstofflцsung abhдngig.
149/1651
[0013] Der Wirkstoff kann ferner wдhrend der weiteren Herstellung und Lagerung des Pflasters
gegebenenfalls in die Selbstklebemasse eindringen. Durch die Reservoirwirkung erfolgt ein
stдndiger Transport des Wirkstoffes vom Trдgermaterial durch die Selbstklebemasse hin zur
дusseren Klebeschicht, die bei der Anwendung auf der Haut aufgebracht wird. Somit ist die Abgabe
des Wirkstoffes sowohl an die Haut und ьber das Trдgermaterial an die Umgebungsluft mцglich.
[0014] Das bahnfцrmige mit Klebemasse beschichtete Trдgermaterial erhдlt somit auf der
gegenьberliegenden Seite eine Beaufschlagung mit dem Wirkstoff oder der wirkstoffhaltigen
Lцsung.
[0015] Zur Beschichtung der zunдchst bahnfцrmigen Trдgermaterialien mit einer
Selbstklebemasse eignen sich verschiedene Verfahren, die aus dem Stand der Technik bekannt sind.
Lцsungsmittelfreie Selbstklebemassen lassen sich beispielsweise mittels einer dem
Doppelschneckenextruder nachgeschalteten Extrusionsdьse beschichten. Zum Druckaufbau fьr die
Dьsenbeschichtung werden Einschneckenextruder und/oder Schmelzepumpen besonders
bevorzugt, so dass die Beschichtung der bahnfцrmigen Trдgermaterialien mit Masseauftrдgen sehr
geringer Schwankungsbreite erfolgen kann.
[0016] Eine weitere Mцglichkeit zur Beschichtung von bahnfцrmigen Trдgermaterialien mit der
nach erfindungsgemдssen Verfahren hergestellten wirkstoffhaltigen Pflaster ist die Verwendung von
Walzenbeschichtungsauftragswerken oder Mehrwalzen-Beschichtungskalandern, die vorzugsweise
aus mindestens zwei Beschichtungswalzen bestehen, wobei die Selbstklebemasse bei Durchgang
durch einen oder mehrere Walzenspalte vor Ьbergabe auf das bahnfцrmige Material auf die
gewьnschte Dicke geformt wird. Dieses Beschichtungsverfahren wird besonders dann bevorzugt,
wenn eine Beschichtung mit Extrusionsdьsen allein nicht mehr die erforderte Genauigkeit im
Masseauftrag liefert. Je nach Art des zu beschichtenden bahnfцrmigen Trдgermaterials kann die
Beschichtung im Gleichlauf- oder Gegenlaufverfahren erfolgen.
[0017] Als bevorzugte Klebemasse werden Heissschmelzselbstklebemassen aus
- phasenseparierenden Styrolblockcopolymeren,
- klebrigmachenden Harzen,
- Tackifiern,
- Weichmachern,
- Fьllstoffen und/oder Additiven verwendet.
[0018] Als Styrolblockcopolymere kommen bevorzugt A-B- und/oder A-B-A- Blockcopolymere oder
deren Mischungen in Frage. Die harte domдnenbildende Phase A besteht vornehmlich aus
Polystyrol oder dessen Derivaten. Die weiche Phase wird vornehmlich aus Polyisopren und
Polybutadien oder deren Mischungen gebildet. Die phasenseparierende Struktur der
150/1651
Styrolblockcopolymere verhilft den Polymeren zu einem thermoplastischen Verhalten, welches sich
von Polymeren mit statistisch verteilten Monomeren unterscheidet und eine mastikationsfreie
Verarbeitung gewдhrleistet. Aufgrund der Unvertrдglichkeit der A- und B-Blцcke besitzen die
Blockcopolymere zwei Glasьbergangstemperaturen: Durch die B-Blцcke eine niedrige unterhalb
der Raumtemperatur und durch die Styrolblцcke eine hohe oberhalb Raumtemperatur. Im
Temperaturbereich zwischen den beiden Glasьbergangstemperaturen zeigen die Blockcopolymere
einerseits elastisches Verhalten aufgrund der B-Blцcke, andererseits aber bleibt der Kautschuk
durch die harten Styroldomдnen, die durch Nebenvalenzkrдfte der Styrolblцcke entstehen, kohдsiv.
[0019] Ebenso kцnnen Kautschukmassen, die lцsungsmittel-basiert sind, beispielsweise n-Hexan
oder auch Benzin, eingesetzt werden.
[0020] Die genannten Eigenschaften der Klebmatrix legen insbesondere die Venroendung fьr
medizinische Produkte, insbesondere Pflaster, medizinische Fixierungen, Wundabdeckungen,
orthopдdische oder phlebologische Bandagen und Binden nahe.
[0021] Schliesslich wird die Matrix mit einem klebstoffabweisenden Trдgermaterial, wie
silikonisiertem Papier, eingedeckt oder mit einer Wundauflage oder einer Polsterung versehen. Auf
seiner selbstklebend ausgerьsteten, spдter der Haut zugewandten Seite ist das
erfindungsgemдsse Pflaster ьber seine ganze Breite bis zum Gebrauch mit einem
klebstoffabweisenden Trдgermaterial abgedeckt. Dieses schьtzt die Selbstklebeschicht aus der gut
hautvertrдglichen Klebemasse der Matrix, die vorzugsweise im Transferverfahren aufgebracht
worden ist, und stabilisiert zusдtzlich das ganze Produkt. Die Abdeckung kann in bekannter Weise
einstьckig oder vorzugsweise zweiteilig ausgebildet sein.
[0022] Abschliessend werden entsprechend den gewьnschten Grцssen und Formen, die Pflaster
aus den Bahnen zugeschnitten und umgehend luftdicht versiegelt. Die Versiegelung dient dazu,
dass der Wirkstoff im System verbleibt und nicht entweichen kann.
[0023] Fьr das erfindungsgemдsse Herstellungsverfahren kommen als Trдgermaterial nur
saugfдhige, d.h. den Wirkstoff oder die wirkstoffhaltige Lцsung aufnehmende Materialien in Frage.
Es kцnnen daher bevorzugt alle bekannten textilen Trдger wie Gewebe, Gewirke oder Vliese
verwendet werden, wobei unter "Vlies" zumindest textile Flдchengebilde gemдss EN 29092 (1988)
sowie Nдhwirkvliese und дhnliche Systeme zu verstehen sind.
[0024] Ebenfalls kцnnen Abstandsgewebe und -gewirke mit Kaschierung verwendet werden.
Derartige Abstandsgewebe werden in der EP 0 071 212 B1 offenbart. Abstandsgewebe sind
mattenfцrmige Schichtkцrper mit einer Deckschicht aus einem Faser- oder Filamentvlies, einer
Unterlagsschicht und zwischen diesen Schichten vorhandene einzelne oder Bьschel von
Haltefasern, die ьber die Flдche des Schichtkцrpers verteilt durch die Partikelschicht
hindurchgenadelt sind und die Deckschicht und die Unterlagsschicht untereinander verbinden. Als
151/1651
zusдtzliches, aber nicht erforderliches Merkmal sind gemдss EP 0 071 212 B1 in den Haltefasern
Partikel aus inerten Gesteinspartikeln, wie zum Beispiel Sand, Kies oder dergleichen, vorhanden.
[0025] Die durch die Partikelschicht hindurchgenadelten Haltefasern halten die Deckschicht und
die Unterlagsschicht in einem Abstand voneinander und sie sind mit der Deckschicht und der
Unterlagsschicht verbunden.
[0026] Abstandsgewebe oder -gewirke sind u. a. in zwei Artikeln beschrieben, und zwar einem
Artikel aus der Fachzeitschrift "kettenwirk-praxis 3/93", 1993, Seiten 59 bis 63 "Raschelgewirkte
Abstandsgewirke" und einem Artikel aus der Fachzeitschrift "kettenwirk-praxis 1/94", 1994, Seiten 73
bis 76 "Raschelgewirkte Abstandsgewirke" auf deren Inhalt hiermit Bezug genommen wird und deren
Inhalt Teil dieser Offenbarung und Erfindung wird.
[0027] Als Vliesstoffe kommen besonders verfestigte Stapelfaservliese, jedoch auch Filament-,
Meltblown- sowie Spinnvliese in Frage, die meist zusдtzlich zu verfestigen sind. Als mцgliche
Verfestigungsmethoden sind fьr Vliese die mechanische, die thermische sowie die chemische
Verfestigung bekannt. Werden bei mechanischen Verfestigungen die Fasern meist durch
Verwirbelung der Einzelfasern, durch Vermaschung von Faserbьndeln oder durch Einnдhen von
zusдtzlichen Fдden rein mechanisch zusammengehalten, so lassen sich durch thermische als auch
durch chemische Verfahren adhдsive (mit Bindemittel) oder kohдsive (bindemittelfrei) Faser-FaserBindungen erzielen. Diese lassen sich bei geeigneter Rezeptierung und Prozessfьhrung
ausschliesslich oder zumindest ьberwiegend auf Faserknotenpunkte beschrдnken, so dass unter
Erhalt der lockeren, offenen Struktur im Vlies trotzdem ein stabiles, dreidimensionales Netzwerk
gebildet wird.
[0028] Besonders vorteilhaft haben sich Vliese erwiesen, die insbesondere durch ein Ьbernдhen
mit separaten Fдden oder durch ein Vermaschen verfestigt sind.
[0029] Derartige verfestigte Vliese werden beispielsweise auf Nдhwirkmaschinen des Typs
"Malivlies" der Firma Karl Meyer, ehemals Malimo, hergestellt und sind unter anderem bei den Firmen
Naue Fasertechnik und Techtex GmbH beziehbar. Ein Malivlies ist dadurch gekennzeichnet, dass
ein Querfaservlies durch die Bildung von Maschen aus Fasern des Vlieses verfestigt wird.
[0030] Als Trдger kann weiterhin ein Vlies vom Typ Kunitvlies oder Multiknitvlies verwendet werden.
Ein Kunitvlies ist dadurch gekennzeichnet, dass es aus der Verarbeitung eines lдngsorientierten
Faservlieses zu einem Flдchengebilde hervorgeht, das auf einer Seite Maschen und auf der anderen
Maschenstege oder Polfaser-Falten aufweist, aber weder Fдden noch vorgefertigte Flдchengebilde
besitzt. Auch ein derartiges Vlies wird beispielsweise auf Nдhwirkmaschinen des Typs "Kunitvlies"
der Firma Karl Mayer schon seit lдngerer Zeit hergestellt. Ein weiteres kennzeichnendes Merkmal
dieses Vlieses besteht darin, dass es als Lдngsfaservlies in Lдngsrichtung hohe Zugkrдfte
aufnehmen kann. Ein Multiknitvlies ist gegenьber dem Kunitvlies dadurch gekennzeichnet, dass das
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Vlies durch das beidseitige Durchstechen mit Nadeln sowohl auf der Ober- als auch auf der
Unterseite eine Verfestigung erfдhrt.
[0031] Schliesslich sind auch Nдhvliese als Vorprodukt geeignet, ein erfindungsgemдsses
Klebeband zu bilden. Ein Nдhvlies wird aus einem Vliesmaterial mit einer Vielzahl parallel
zueinander verlaufender Nдhte gebildet. Diese Nдhte entstehen durch das Einnдhen oder
Nдhwirken von durchgehenden textilen Fдden. Fьr diesen Typ Vlies sind Nдhwirkmaschinen des
Typs "Maliwatt" der Firma Karl Mayer, ehemals Malimo, bekannt.
[0032] Weiterhin besonders vorteilhaft ist ein Stapelfaservlies, das im ersten Schritt durch
mechanische Bearbeitung vorverfestigt wird oder das ein Nassvlies ist, das hydrodynamisch gelegt
wurde, wobei zwischen 2% und 50% der Fasern des Vlieses Schmelzfasern sind, insbesondere
zwischen 5% und 40% der Fasern des Vlieses.
[0033] Ein derartiges Vlies ist dadurch gekennzeichnet, dass die Fasern nass gelegt werden oder
zum Beispiel ein Stapelfaservlies durch die Bildung von Maschen aus Fasern des Vlieses oder durch
Nadelung, Vernдhung beziehungsweise Luft- und/oder Wasserstrahlbearbeitung vorverfestigt wird.
[0034] In einem zweiten Schritt erfolgt die Thermofixierung, wobei die Festigkeit des Vlieses durch
das Auf- oder Anschmelzen der Schmelzfasern nochmals erhцht wird.
[0035] Die Verfestigung des Vliestrдgers lдsst sich auch ohne Bindemittel beispielsweise durch
Heissprдgen mit strukturierten Walzen erreichen, wobei ьber Druck, Temperatur, Verweilzeit und die
Prдgegeometrie Eigenschaften wie Festigkeit, Dicke, Dichte, Flexibilitдt u.д. gesteuert werden
kцnnen.
[0036] Fьr die erfindungsgemдsse Nutzung von Vliesen ist besonders die adhдsive Verfestigung
von mechanisch vorverfestigten oder nassgelegten Vliesen von Interesse, wobei diese ьber Zugabe
von Bindemittel in fester, flьssiger, geschдumter oder pastцser Form erfolgen kann. Prinzipielle
Darreichungsformen sind vielfдltig mцglich, zum Beispiel feste Bindemittel als Pulver zum Einrieseln,
als Folie oder als Gitternetz oder in Form von Bindefasern. Flьssige Bindemittel sind gelцst in
Wasser oder organischen Lцsemittel oder als Dispersion applizierbar. Ьberwiegend werden zur
adhдsiven Verfestigung Bindedispersionen gewдhlt: Duroplasten in Form von Phenol- oder
Melaminharzdispersionen, Elastomere als Dispersionen natьrlicher oder synthetischer Kautschuke
oder meist Dispersionen von Thermoplasten wie Acrylate, Vinylacetate, Polyurethane, StyrolButadien-Systeme, PVC u.д. sowie deren Copolymere. Im Normalfall handelt es dabei um
anionische oder nicht-ionogen stabilisierte Dispersionen, in besonderen Fдllen kцnnen aber auch
kationische Dispersionen von Vorteil sein.
[0037] Die Art des Bindemittelauftrages kann gemдss dem Stand der Technik erfolgen und ist
beispielsweise in Standardwerken der Beschichtung oder der Vliestechnik wie "Vliesstoffe" (Georg
153/1651
Thieme Verlag, Stuttgart, 1982) oder "Textiltechnik-Vliesstofferzeugung" (Arbeitgeberkreis
Gesamttextil, Eschborn, 1996) nachzulesen.
[0038] Fьr mechanisch vorverfestigte Vliese, die bereits eine ausreichende Verbundfestigkeit
aufweisen, bietet sich der einseitige Sprьhauftrag eines Bindemittels an, um
Oberflдcheneigenschaften gezielt zu verдndern.
[0039] Neben dem sparsamen Umgang mit dem Bindemittel wird bei derartiger Arbeitsweise auch
der Energiebedarf zur Trocknung deutlich reduziert. Da keine Abquetschwalzen benцtigt werden
und die Dispersionen vorwiegend in dem oberen Bereich des Vliesstoffes verbleibt, kann eine
unerwьnschte Verhдrtung und Versteifung des Vlieses weitgehend verhindert werden.
[0040] Fьr eine ausreichende adhдsive Verfestigung des Vliestrдgers ist im allgemeinen
Bindemittel in der Grцssenordnung von 1 % bis 50 %, insbesondere 3 % bis 20 %, bezogen auf das
Gewicht des Faservlieses, zuzugeben.
[0041] Die Zugabe des Bindemittels kann bereits bei der Vliesherstellung, bei der mechanischen
Vorverfestigung oder aber in einem gesonderten Prozessschritt erfolgen, wobei dieser in-line oder
off-line durchgefьhrt werden kann. Nach der Bindemittelzugabe muss temporдr fьr das Bindemittel
ein Zustand erzeugt werden, in dem dieses klebend wird und adhдsiv die Fasern verbindet - dies
kann wдhrend der Trocknung zum Beispiel von Dispersionen, aber auch durch Erwдrmung erreicht
werden, wobei ьber flдchige oder partielle Druckanwendung weitere Variationsmцglichkeiten
gegeben sind. Die Aktivierung des Bindemittels kann in bekannten Trockenkanдlen, bei geeigneter
Bindemittelauswahl aber auch mittels Infrarotstrahlung, UV-Strahlung, Ultraschall,
Hochfrequenzstrahlung oder dergleichen erfolgen. Fьr die spдtere Endanwendung ist es sinnvoll,
aber nicht zwingend notwendig, dass das Bindemittel nach Ende des Vlies-Herstellprozesses seine
Klebrigkeit verloren hat.
[0042] Eine weitere Sonderform der adhдsiven Verfestigung besteht darin, dass die Aktivierung
des Bindemittels durch Anlцsen oder Anquellen erfolgt. Prinzipiell kцnnen hierbei auch die Fasern
selbst oder zugemischte Spezialfasern die Funktion des Bindemittels ьbernehmen. Da fьr die
meisten polymeren Fasern derartige Lцsemittel jedoch aus Umweltgesichtspunkten bedenklich
beziehungsweise problematisch in ihrer Handhabung sind, wird dieses Verfahren eher selten
angewandt.
[0043] Als Ausgangsmaterialien fьr den textilen Trдger sind insbesondere Polyester-,
Polypropylen-, Viskose- oder Baumwollfasern vorgesehen. Die vorliegende Erfindung ist aber nicht
auf die genannten Materialien beschrдnkt, sondern es kцnnen, fьr den Fachmann erkenntlich ohne
erfinderisch tдtig werden zu mьssen, eine Vielzahl weiterer Fasern zur Herstellung des
Trдgermaterials, des Vlieses, eingesetzt werden.
154/1651
[0044] Weiterhin sind auch Maschenwaren hervorragend geeignet. Maschenwaren sind textile
Flдchengebilde hergestellt aus einem oder mehreren Fдden oder Fadensystemen durch
Maschenbildung (Fadenschleifen), im Unterschied zu Webwaren (Geweben), bei der die Flдche
durch Verkreuzen von zwei Fadensystemen (Kett- und Schussfдden) hergestellt wird und den
Vliesen (Faserverbundstoffen), bei denen ein loser Faserflor durch Wдrme, Nadelung, Nдhen oder
durch Wasserstrahlen verfestigt wird.
[0045] Maschenwaren lassen sich in Gestricke, bei denen die Fдden in Querrichtung durch das
Textil laufen, und in Gewirke einteilen, bei denen die Fдden lдngs durch das Textil laufen.
Maschenwaren sind durch ihre Maschenstruktur prinzipiell nachgiebige, anschmiegsame Textilien,
weil sich die Maschen in Lдnge und Breite dehnen kцnnen und das Bestreben haben, in ihre
Ausgangslage zurьckzukehren. Sie sind bei hochwertigem Material sehr strapazierfдhig.
[0046] Zusammenfassend kann festgehalten werden, dass als Trдgermaterialien sich alle starren
und elastischen Flдchengebilde aus synthetischen und natьrlichen Rohstoffen eignen. Bevorzugt
sind Trдgermaterialien, die so eingesetzt werden kцnnen, dass sie Eigenschaften eines
funktionsgerechten Verbandes erfьllen. Beispielhaft sind Textilien wie Gewebe, Gewirke, Gelege,
Vliese, Laminate, Netze, Folien, Schдume und Papiere aufgefьhrt. Weiter kцnnen diese Materialien
vor- beziehungsweise nachbehandelt werden. Gдngige Vorbehandlungen sind Corona und
Hydrophobieren; gelдufige Nachbehandlungen sind Kalandern, Tempern, Kaschieren, Stanzen und
Eindecken.
[0047] Besonders vorteilhaft ist, wenn das Trдgermaterial sterilisierbar, bevorzugt [gamma](gamma) sterilisierbar, ist.
[0048] Als erfindungsgemдsse Wirkstoffe werden Substanzen verstanden, die in menschlichen
oder tierischen Organismen zur Verhьtung, Heilung, Linderung oder Erkennung von Krankheiten
dienen oder einfach nur dem Wohlbefinden des Menschen oder zur kosmetischen Vebesserung
dienen. Die eingesetzten Wirkstoffe kцnnen sowohl systemisch als auch lokal wirksam sein.
[0049] Typische, erfindungsgemдss eingesetzte Wirkstoffe sind hierbei: Aceclidin, Amfetaminil,
Amfetamin, Amylnitrit, Apophedrin, Atebrin, Alpostadil, Azulen, Arecolin, Anethol, Amylenhydrat,
Acetylcholin, Acridin, Adenosintriphosphorsдure, Дpfelsдure, Alimemazin, Allithiamin,
Aminoethanol, Apyzin, Apiol, Azatadin, Alprenolol, Дthinazon, Bisabolol, Bisnorephedrin,
Butacetoluid, Benactyzin, Campher, Colecalciferol, Chloralhydrat, Clemastin, Chlorobutanol,
Capsaicin, Cyclopentamin, Clobutinol, Chamazulen, Dimethocain, Codein, Chloropromazin, Chinin,
Chlorthymol, Cyclophosphamid, Cinchocain, Chlorambuzil, Chlorphenesin, Dexchlorpheniramin,
Dinoproston, Dixyrazin, Ephedrin, Ethosuximid, Enallylpropymal, Emylcamat, Erytroltetranitrat, Emetin,
Eucalyptol, Etofenamat, Ethylmorphin, Fentanyl, Fluanison, Guajazulen, Hyoscyamin, Histamin,
Fencarbamid, Hydroxycain, Hexylresorcin, Isoaminilcitrat, Isosorbiddinitrat, Ibuprofen, Jod, Jodoform,
155/1651
Isoaminil, Lidocain, Lopirin, Levamisol, Methadon, Methyprylon, Methylphenidat, Mephenesin,
Methylephedrin, Meclastin, Methopromazin, Mesuximid, Menthol, Methylpentinol, Metixen,
Mesoprostol, Nicethamid, Norpseudoephedrin, Nonylsдurevanillyamid, Oxytetracain, Oxyprenolol,
Oxyphenbutazon, Oxychinolin, Pinen, Prolintan, Procyclidin, Piperazin, Pivazid, Phensuximid, Procain,
Phenindamin, Promethazin, Pentetrazol, Profenamin, Perazin, Phenol, Pethidin, Pilocarpin,
Prenylamin, Phenoxybenzamin, Resochin, Scopolamin, Salicylsдure, Spartein, Timolol, Trifluperazin,
Tetracain, Trimipramin, Tranylcypromin, Trimethadion, Tybamat, Thymol, Thioridazin, Valproinsдure,
Verapamil, sowie weitere, dem Fachmann gelдufige, ьber die Haut, eingeschlossen Schleimhдute,
aufnehmbare Wirkstoffe. Selbstverstдndlich ist diese Aufzдhlung nicht abschliessend.
[0050] Weitere, fьr die Wundheilung fцrderliche Wirkstoffe, wie Silbersulfadiazin, kцnnen ebenfalls
eingesetzt werden.
[0051] Besonders bevorzugt weden als Wirkstoffe дtherische Цle eingesetzt, die sowohl ьber die
Haut als auch ьber die Atemluft wirken kцnnen. Bevorzugt ist hierbei der Weg ьber die Atemluft.
[0052] Unter дtherischen Цlen sind aus Pflanzen gewonnene Konzentrate zu verstehen, die als
natьrliche Rohstoffe hauptsдchlich in der Parfьm- und Lebensmittelindustrie eingesetzt werden und
die mehr oder weniger aus flьchtigen Verbindungen bestehen. Als Beispiele fьr diese Verbindungen
kцnnen 1,8-Cineol, Limonen, Menthol, Borneol und Kampfer genannt werden. Oft wird der Begriff
дtherische Цle fьr die noch in den Pflanzen enthaltenen flьchtigen Inhaltsstoffe verwendet. Im
eigentlichen Sinn versteht man aber unter дtherischen Цlen Gemische aus flьchtigen Komponenten,
die durch Wasserdampfdestillation aus pflanzlichen Rohstoffen hergestellt werden.
[0053] Дtherische Цle bestehen ausschliesslich aus flьchtigen Komponenten, deren Siedepunkte
in der Regel zwischen 150 und 300[deg.]C liegen. Sie enthalten ьberwiegend Kohlenwasserstoffe
oder monofunktionelle Verbindungen wie Aldehyde, Alkohole, Ester, Ether und Ketone.
Stammverbindungen sind Mono- und Sesquiterpene, PhenylpropanDerivate und lдngerkettige
aliphatische Verbindungen.
[0054] Bei manchen дtherischen Цle dominiert ein Inhaltsstoff (zum Beispiel Eugenol in Nelkenцl
mit mehr als 85%), andere дtherische Цle stellen hingegen komplex zusammengesetzte
Mischungen der einzelnen Bestandteile dar. Oft werden die Organoleptische Eigenschaften nicht
von den Hauptkomponenten, sondern von Nebenoder Spurenbestandteilen geprдgt, wie zum
Beispiel von den 1,3,5-Undecatrienen und Pyrazinen im Galbanum-Цl. Bei vielen der kommerziell
bedeutenden дtherischen Цle geht die Zahl der identifizierten Komponenten in die Hunderte. Sehr
viele Inhaltsstoffe sind chiral, wobei sehr oft ein Enantiomer ьberwiegt oder ausschliesslich
vorhanden ist, wie zum Beispiel (-)-Menthol im Pfefferminzцl oder (-)-Linalylacetat im Lavendelцl.
[0055] Als bevorzugte дtherische Цle, die beispielsweise fьr die Indikation Bronchitis und Asthma
eingesetzt werden, kцnnen Oleum Eucalypti, Oleum Menthae piperitae, Oleum camphoratum,
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Oleum Rosmarini, Oleum Thymi, Oleum Pini sibricum und Oleum Pini silverstris sowie die Terpene
1,8-Cineol und Levomethanol genannt werden.
[0056] Als weitere дtherische Цle, mit denen eine Freisetzung aus Wirkstoffhaltigen Pflastern
mцglich ist, sind Oleum Abietis albae, Oleum Anisi, Oleum Aurantii Floris, Oleum Bergamottae,
Oleum Calendulae infusum, Oleum camphoratum, Oleum Caryophylli, Oleum Chamomillae, Oleum
Cinnamomi ceylanici, Oleum Citri, Oleum Citronellae, Oleum Cupressi, Oleum Cymbopogonis,
Oleum Jecoris, Oleum Lavendulae, Oleum Macidis, Oleum Majoranae, Oleum Melaleucae viridiflorae,
Oleum Melissae, Oleum Menthae arvensis, Oleum Menthae piperatae, Oleum Millefolium, Oleum
Myrrhae, Oleum Myrte, Oleum Oregani, Oleum Pini sibricum, Oleum Pinisilvestris, Oleum Salviae,
Oleum Santali, Oleum Terebinthinae rectificat., Oleum Thymi Oleum Valerianae, Oleum Zingiberis
und/oder Teebaumцl zu nennen.
[0057] Fьr die Applikation der дtherischen Цle in Wirkstoffhaltigen Pflastern werden neben
Bronchitis und Asthma die folgende Indikationen angegeben:
- Sedativum durch die beruhigende Wirkung des Oleum Melissae, Oleum Valerianae und Oleum
Lavendulae.
- Antiphlogistische Wirkung bei rheumatischen und anderen Erkrankungen durch Oleum
Chamomillae, Oleum Eucalypti, Oleum Pini sibricum, Oleum Pinisilvestris, Oleum Rosmarini, Oleum
Salviae, Oleum Terebinthinae rectificat und Oleum Thymi
- Die дtherischen Цle Oleum Bergamottae, Oleum Majoranae, Oleum Caryophylli und Oleum
Melaleucae viridiflorae werden aufgrund ihrer antiseptische Wirkung zur Behandlung von offenen
Wunden eingesetzt.
- Lokalanдsthetische und desinfizierende Wirkung des Oleum Caryophylli bei schmerzender und
entzьndeter Pulpa.
- Der ьberwiegende Teil der angegebenen дtherischen Цle wird in der Aromatherapie verwendet.
[0058] Die дtherischen Цle werden bevorzugt mit einem Anteil von 0,01 bis 25 Gew.%,
insbesondere 4 bis 5 Gew.%, bezogen auf die Gesamtmasse des Pflaster eingesetzt. Es hat sich als
vorteilhaft erwiesen, dass das erfindungsgemдsse Pflaster nicht nur ein дtherisch Цl enthalten kann
sondern dass es die spezifische Formulierung erlaubt mehrere, insbesondere bis zu 5, verschiedene
дtherische Цle in dem Trдgermaterial zu inkorporieren.
[0059] Als weiterer Vorteil von дtherischen Цlen in dem erfindungsgemдssen Pflaster kann
erwдhnt werden, dass die дtherischen Цle aufgrund ihrer Diffusionseigenschaften im Bereich der
Klebematrix ohne Probleme aus dem Pflaster freigesetzt werden, wobei der Einsatz von Enhencern
nicht zwingend notwendig ist. Bei einer kontrollierten Freisetzung aus dem System wird aus diesem
Grunde im Gegensatz zu festen Wirkstoffen auf einen erheblichen Ьberschuss des Wirkstoffs
157/1651
verzichtet. Ferner ermцglicht die gleichzeitige Applikation, per inhalationem und transdermal, den
aus den erfindungsgemдssen Systemen freigesetzten дtherischen Цlen einen pharmakologischen
Effekt durch die gleichzeitige Wirkung in mehreren Bereichen des Organismus. Ausserdem kцnnen
neben den дtherischen Цlen der Matrix weitere Stoffe zugesetzt werden, die kosmetische,
hautpflegende oder stabilisierende Eigenschaften aufweisen.
[0060] Die beschriebenen Wirkstoffe kцnnen gegebenenfalls auch in Lцsung auf das
Trдgermaterial aufgebracht werden. Geeignete Lцsungsmittel sind neben Wasser, Alkohol, Olivenцl,
Mineralцl, Glycerin und/oder Chloroform oder deren Mischungen.
[0061] Als besonders vorteilhaft hat sich als Lцsungsmittel eine Mischung aus Methylsalicylat (MS)
und Ethylenglycolmonosalicylat (EGMS) sowie in geringen Mengen Nelkenцl und Pfefferminzцl
herausgestellt, wobei diese Mischung selber als Wirkstoff fungieren kann.
[0062] Дtherische Цle hinterlassen auf Papier im Gegensatz zu den fetten Цlen keine Fettflecken,
so dass ein weiterer Vorteil darin liegt, dass auch kein fleckiges/fettiges Gewebe nach dem
erfindungsgemдssen Aufsprьhvorgang auf dem Pflaster verbleibt. Die Anwendungsakzeptanz ist
damit deutlich erhцht.
[0063] Beispielhaft ergibt sich folgende Zusammensetzung der Wirkstofflцsung:
Camphor:11,20 Gew.%
Menthol:33,59 Gew.%
MS:22,39 Gew.%
EGMS:22,39 Gew.%
Borneol:1,32 Gew.%
Nelkenцl:2,20 Gew.%
Thymol:1,32 Gew.%
Pfefferminzцl:5,60 Gew.%
[0064] Als aktive Wirkstoffe wirken dabei Camphor mit 2% +/- 20%, (d.h. 1,6% - 2,4%); Menthol mit
6% +/- 20%, (d.h. 4,8% - 7,2%); Methylsalicylate mit 4% +/- 20%, (d.h. 3,2% - 4,8%) und
Ethylenglycol monosalicylate mit 4% +/- 20%, d.h. (3,2% - 4,8%), bezogen auf die Gesamtmasse der
Wirkstofflцsung.
[0065] Die Wirkstofflцsung wird mittels Versprьhen auf das Trдgermaterial gleichmдssig
aufgetragen. Nach dem Zuschneiden, Eindecken mit klebstoffabweisenden Trдgermaterial werden
die Pflaster umgehend versiegelt.
[0066] Das erfindungsgemдss hergestellte Pflaster wird nun zur Anwendung aus der Versiegelung
entnommen und auf der Haut appliziert. Der Wirkstoff kann nun ьber die Luft und gegebenfalls ьber
die Klebemasse lokal an die Haut abgegeben werden und seine Wirkung entfalten.
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[0067] Aufgrund der Reservoirwirkung des Trдgermaterials und der luftdichten Versiegelung ist
ausreichend Wirkstoff im Pflastersystem enthalten, so dass eine langanhaltende Wirkstofffreisetzung
gewдhrleistet ist.Claims:
1. Verfahren zur Herstellung eines wirkstoffhaltigen Pflasters indem ein saugfдhiges Trдgermaterial
auf einer Seite mit einer Selbstklebemasse beschichtet wird, auf der gegenьberliegenden Seite mit
einem Wirkstoff oder einer wirkstoffhaltigen Lцsung beaufschlagt wird, so dass das Trдgermaterial
eine Menge des Wirkstoffes oder der wirkstoffhaltigen Lцsung aufnimmt, die mit Klebmasse
beschichtete Seite des Trдgermaterials ьber seine ganze Breite mit einem klebstoffabweisenden
Trдgermaterial abgedeckt wird und das gesamte Pflaster luftdicht eingesiegelt wird.
2. Verahren nach Anspruch 1, dadurch gekennzeichnet, dass das Trдgermaterial ьber seine
gesamte Breite mit dem Wirkstoff oder der wirkstoffhaltigen Lцsung besprьht wird.
3. Verfahren nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass als Trдgermaterialien Gewebe,
Gewirke, Gelege, Vliese, Laminate, Netze, Folien, Schдume und/oder Papiere gewдhlt werden.
4. Verfahren nach einem der vorstehenden Ansprьche, dadurch gekennzeichnet, dass als Wirkstoffe
дtherische Цle gewдhlt werden.
5. Verfahren nach Anspruch 4, dadurch gekennzeichnet, dass als Wirkstoffe дtherische Цle in einer
Mischung aus Methylsalicylat und Ethylenglycolmonosalicylat gewдhlt werden.
6. Verfahren nach Anspruch 5, dadurch gekennzeichnet, dass als Wirkstofflцsung eine Lцsung mit
1,6 Gew.% - 2,4 Gew.% Camphor, bevorzugt 2 Gew.%, 4,8 Gew.% - 7,2 Gew.% Menthol, bevorzugt
6 Gew.%, 3,2 Gew.% - 4,8 Gew.% Methylsalicylate, bevorzugt 4 Gew.%, und 3,2 Gew.% - 4,8
Gew.% Ethylenglycol monosalicylate, bevorzugt 4 Gew.%, bezogen auf die Gesamtmasse der
Wirkstofflцsung, gewдhlt wird.
7. Verfahren nach einem der vorstehenden Ansprьche, dadurch gekennzeichnet, dass vor der
Versiegelung entsprechend den gewьnschten Grцssen und Formen, die Pflaster aus den Bahnen
zugeschnitten werden.
8. Wirkstoffhaltiges Pflaster erhдltlich nach einem Verfahren gemдss einem der Ansprьche 1 bis 7.
Es folgt kein Blatt Zeichnungen
159/1651
40. DE19821106 - 18.11.1999
MITICIDAL CLEANING COMPOSITION COMPRISING ESSENTIAL OIL DISSOLVED IN EMULSIFIER,
USED FOR CLEANING DOMESTIC TEXTILES TO PREVENT ALLERGIC DISEASE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE19821106
Applicant(s):
GREWE HELMUT F (DE)
IP Class 4 Digits: A01N; C11D; D06L
IP Class:
A01N65/00; C11D3/48; D06L1/12
E Class: A01N65/00+M; C11D3/00B13; C11D3/18; C11D3/00B6
Application Number:
DE19981021106 (19980512)
Priority Number: DE19981021106 (19980512)
Family: DE19821106
Abstract:
A MITICIDAL CLEANER COMPRISES A SOLUTION OF A VEGETABLE OIL HAVING A HIGH
ESSENTIAL OIL CONTENT IN AN EMULSIFIER. THE SOLUTION IS USED TO FORM AN AQUEOUS
EMULSION FOR SOAKING OR WASHING TEXTILES OR CLEANING CARPETS OR CUSHIONS. A
NOVEL MITICIDAL CLEANING COMPOSITION FOR BED LINEN, DOMESTIC WASHING, CLOTHES,
CARPETS OR CUSHIONS IS OBTAINED BY DISSOLVING A VEGETABLE OIL WITH A HIGH
ESSENTIAL OIL CONTENT IN THE MINIMUM POSSIBLE AMOUNT OF EMULSIFIER (20-100%
BASED ON OIL), FOLLOWED BY USING THE OBTAINED OIL-EMULSIFIER SOLUTION TO FORM
AN AQUEOUS EMULSION FOR SOAKING OR WASHING TEXTILES IN A WASHING MACHINE OR
CLEANING OR SPRAY EXTRACTION OF CARPETS OR CUSHIONS. THE EMULSIFIER CONTAINS
10-30% OR MORE OF NONIONIC SURFACTANT AND UP TO 20% ANIONIC
SURFACTANT.Description:
160/1651
Zugrundeliegendes Problem und Stand der Technik
Es ist bekannt, dass viele atopische Erkrankungen auf Allergene aus dem Kцrper und den
Exkrementen von Hausstaubmilben und Vorratsmilben (domestic mites) zurьckzufьhren sind. Zu
diesen Erkrankungen gehцren:
- Atopisches Ekzem (Neurodermitis) mit ca. 2.5 Mio Betroffenen
- Allergisches Asthma mit ca. 1.5 Mio Betroffenen
- Ganzjдhrige allergische Rhinitis mit > 1 Mio Betroffenen in der BRD
Bei der Behandlung dieser Erkrankungen und zur Prдvention steht die Vermeidung eines Kontaktes
mit Allergenen von Milben besonders der Hausstaubmilbe ьber die Atemwege und ьber die Haut an
vorrangiger Stelle.
Es ist weiter bekannt, dass die Matratze, wegen der dort vorherrschen den gьnstigen
Lebensbedingungen (Feuchte, Wдrme und Hautschuppen), ein bevorzugter Aufenthaltsort fьr
Milben insbesondere Hausstaubmilben ist. Im klinisch therapeutischen Einsatz haben sich daher
Luft-/Allergen-dichte aber wasserdampfdurchlдssige Matratzenhьllen, sogenannte "encasings",
bewдhrt, ohne bei allen Betroffenen die durch Milbenallergene verursachten Beschwerden zu
lindern oder gдnzlich vermeiden zu kцnnen.
Es ist weniger bekannt, dass sich hohe Konzentrationen an Milben und Milbenallergenen auch in
Bettextilien, Wolldecken und Kleidungsstьcken (1., 2.) befinden kцnnen und von dort aus in direkten
Kontakt mit den Betroffenen kommen (ьber Haut und Atemwege). Die Milbenallergene aus deren
Kцrper und Exkrementen kцnnen aus den Textilien durch normale Wдsche in der Waschmaschine
bereits in nur warmem Wasser zu ьber 90% entfernt werden. Eine Vernichtung der Milben selbst
kann durch hygienische Wдsche erfolgen bei mind. 55 DEG C (3.). Eine solche Wдsche ist aber fьr
viele Textilien besonders Wolle nicht an wendbar (z. B. wegen Verfilzung) bzw. widerspricht dem
Trend nach energiesparenden Kalt-Waschmitteln. Beim Waschen mit Temperaturen unterhalb 55
DEG C und gдngigen Waschmitteln werden Milben aber nicht bzw. nur unzureichend abgetцtet.
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Es ist weiter bekannt, dass sich hohe Konzentrationen an Milben und Milbenallergenen auch in
Teppichen, Teppichbцden und Polstermцbeln befinden, besonders in Schlafzimmern und
kombinierten Zimmern wie Kinderzimmern (4., 5.), und von dort aus in direkten Kontakt mit den
Betroffenen kommen (ьber Haut und Atemwege).
Das Entfernen von Milben besonders aus mittel- und hochflorigen Teppichen ist nur unzureichend
mцglich, da sich lebende Milben in tieferen Schichten verhaken und verstecken, wo sie ausreichend
mit Hautschuppen versorgt sind und der Staub durch Kapillarwirkung fьr ausreichend Feuchtigkeit
sorgt.
Der mцgliche Einsatz von Benzylbenzoat, dem Benzylalkoholester der Benzoesдure, in
Waschmitteln und Teppich-/Polsterreinigungsmitteln hat eine milbentцtende (akarizide) Wirkung.
Toxikologisch sichere Erkenntnisse zum Benzylbenzoat in Bezug auf eine Unbedenklichkeit beim
Menschen liegen aber bisher nicht vor.
Da bei Benzylbenzoat die Wirksamkeit auf einem einzigen Wirkprinzip beruhen dьrfte, ist die Gefahr
einer langfristigen Resistenzbildung bei Milben, die besonders anpassungsfдhig sind, gross. Auch
der Geruch des Benzylbenzoats wird von vielen Menschen nicht akzeptiert. Das fьhrt bei
betroffenen Personen zu einer weitgehenden Ablehnung und dem Nichteinsatz entsprechender
Akarizide auf der Basis synthetischer Chemikalien, die oft auch grundsдtzlich abgelehnt werden.
Es ist bekannt, dass die Dдmpfe von дtherischen Pflanzenцlen insbesondere auch Baumцlen eine
milbentцtende Wirkung haben (6.). Дtherische Цle lassen sich durch geeignete Emulgatoren in
wдssrige Emulsionen ьberfьhren.
Literatur
1. Siebers, R. W. et al.; J ALLERGY CLIN IMMUNOL 1996; 97, 853-4
2. Tovey, E. R. et al.; J ALLERGY CLIN IMMUNOL 1995; 96, 999-1001
3. McDonald, L. G. et al.; J ALLERGY CLIN IMMUNOL 1992; 90, 599-608
4. Mumcuoglu, Y. K.; ALLERGOLOGY 1988; 6, 223-8
5. Jьrgens, H. W.; DER KINDERARZT 1992; 11, 1884-9
6. Watanabe. F. et al.; SHOYAKUGAKU ZASSHI 1998; 43, (2), 163-8.
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Beschreibung der Erfindung
Es war Ziel der vorliegenden Erfindung Wege zu finden, die Milben durch ein schonendes
Einweichen/Vorbehandeln (30 DEG C bzw. Raumtemperatur) der kontaminierten Textilien, Teppiche
und Polster vor dem normalen Waschgang/Reinigungsgang zu vernichten bei gleichzeitiger
Anpassung der Waschprogramme/Reinigungsprogramme moderner Waschmaschinen bzw.
Teppich-/Posterreinigungsgerдte an die notwendige Behandlung.
Dies ist schon bei ca. 20-30 DEG C mцglich durch emulgierte essentielle Pflanzenцle, besonders
auch Baumцle, in einer Konzentration von 0,2 bis 1,0% Цl bezogen auf Waschflotte (Textilwдsche)
bzw. 0,5 bis 2,0% Цl bezogen auf Reinigungsflotte (Teppich-/Polsterreinigung) nach einer
Kontaktzeit von ca. 30 bis 60 Minuten je nach Temperatur. Die niedrige Temperatur erfordert die
hцhere Kontaktzeit. Mehr als 90 bis zu 100% der Milben lassen sich so abtцten.
Geeignete Цl-Emulgatoren enthalten primдr Niotenside. Eine Begrenzung der Konzentration des
Emulgators nach oben ist notwendig, um den Kontakt der in Micellen gebundenen Цltrцpfchen mit
der Milbenoberflдche nicht zu sehr durch Abstossung zu reduzieren bzw. durch zu starke
Schaumbildung. Das Цl muss in ausreichendem Masse an den Milbenkцrper herangebracht
werden дhnlich der Wirkung von Badeцlen, bei denen das Цl an die Hautoberflдche gelangen soll.
Gleichzeitig ist der Einsatz anionischer Emulgatoren (in der Regel starke Detergentien mit
Salzcharakter) auch zu beschrдnken, um gegenьber der Milbe keine isotonische Lцsung
anzubieten, die eine Schutzfunktion ausьben kцnnte.
Die Behandlung lдsst sich vorteilhaft durch Einweichen/Vorbehandeln in/mit einer entsprechenden
Emulsion vor dem eigentlichen Waschgang/Reinigungsgang durchfьhren.
Das Waschprogramm fьr Textilien pumpt nach einer bewegungsarmen Einweichphase mit nur einer
Einspьlung die Einweichflotte ab und geht dann zur je nach Textilart geeigneten Hauptwдsche ьber.
Das Reinigungsprogramm fьr Teppiche und Polster erfolgt durch Sprьhextraktion in zwei Schritten.
Zuerst wird der Teppich (Polster) mit der Цl-haltigen Emulsion besprьht. Bedarf an Sprьhlцsung:
0,5-2 l/m je nach Teppichdicke. Nach der Einwirkzeit wird in einem zweiten Schritt eine gдngige
163/1651
Teppichreinigungslцsung in mцglichst konzentrierter Form zusдtzlich aufgesprьht und gleichzeitig
saugextrahiert.
Beispiel
Milben-tцtendes Reinigungsmittel als Einweichmittel
Bei Bettwдsche und Bekleidung ist eine Behandlung besonders gut realisierbar in neuen Front- und
Topladerwaschmaschinen mit spezifischem Einweichprogramm (teils zeitlich regelbar) bei geringer
Umwдlzung der Waschflotte also geringer mechanischer Belastung des Textils. Handeinweichen ist
ebenfalls mцglich. Danach kцnnen die ab gestorbenen Milben, deren Allergene und weitere
Schmutzpartikel und -substanzen in einem normalen, fьr das Textil geeigneten Waschgang entfernt
werden. Vor dem Hauptwaschgang muss allerdings die stark Цl-haltige Emulsion, Einweichflotte,
abgepumpt werden, um die Wirksamkeit der Hauptwдsche nicht zu gefдhrden. Da auch bei
modernen Waschmaschinen mit Einweichprogramm die Einweichflotte direkt fьr die Hauptwдsche
genutzt wird, bedeutet das ein Abschalten des Programms, das Einstellen von "Abpumpen" und
anschliessende Neustarten der Hauptwдsche.
Praktischer ist ein Waschprogramm mit zeitlich einstellbarer Einweichphase von 30-60 Minuten bei
Eingabe des Reinigungsmittels (Цl-Emulgatorlцsung) ьber das Eingabefach
"Vorwдsche/Einweichen" und nur einmaligem Einspьlen von Wasser, danach automatischem
Abpumpen der Einweichflotte und Ьbergang zur Hauptwдsche. Ein solches durchgehendes
Programm inklusive Einweichphase ist gerade auch fьr die Wollwдsche (stark kontaminiert)
notwendig, fьr die bisher kein Einweichen vorgesehen ist. Wдhrend der Einweichphase ist die
Bewegung der Waschtrommel zum Umwдlzen der Einweichflotte auf max. 10 pro Minute zu
reduzieren. Es erfolgt ein nur einmaliges Einspьlen.
Wichtig fьr den Erfolg ist die feine Verteilung des Pflanzenцls in der Waschflotte durch Zusatz eines
geeigneten Emulgators. Als Emulgator geeignet ist ein Gemisch verschiedener Tenside, wie es z. B.
in modernen flьssigen Hand-Geschirrspьlmittelkonzentraten mit besonderer Befдhigung zur Fett/Цl-Emulsion vorliegt:
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- hoher Anteil an Niotensiden (10 bis ьber 30%)
- kleiner Anteil an anionischen Tensiden (bis zu 5%)
- Wasser ad 100%.
Der Emulgator sollte in einer Menge von 20-35% bezogen auf Цl eingesetzt werden und zusammen
mit dem Цl eine klare Lцsung bilden (Цl-Emulgatorlцsung).
Die Stabilitдt der Emulsion lдsst sich daran erkennen, dass 20-30 ml Цl-Emulgatorlцsung vermischt
in 1 l Wasser eine opake Emulsion ergeben, die zumindest fьr 30 Min. stabil bleibt (keine
Abscheidung von Pflanzenцl).
Ausgehend von einer 0,4%igen Цlkonzentration in der Einweichflotte, z. B. Eukalyptusцl, einem
Emulgatorzusatz von 25% bezogen auf Цl und einem Volumen von 8 l Wasser (Bedarf fьr 1 kg Wolle
oder Feinwдsche) fьr das einmalige Einspьlen, werden ca. 40 ml Reinigungsmittel, ЦlEmulgatorlцsung, benцtigt, die sich aus 32 ml Цl und 8 ml Emulgator zusammensetzen.
Beispiel
Milben-tцtendes Reinigungsmittel als Hauptwaschmittel
Fehlt eine Einweichmцglichkeit, kann zur Not ein Hauptwaschmittel (fьr Vor- und Hauptwдsche)
eingesetzt werden, bei dem der Emulgator einen erhцhten Anteil an Niotensiden (15 bis ьber 30%)
und einen mittleren Anteil an anionischen Tensiden (5 bis 15%) hat. Der Emulgator sollte dann in
einer Menge von 30-50% bezogen auf Pflanzenцl eingesetzt werden und zusammen mit dem Цl
eine klare Lцsung bilden (Цl-Emulgatorlцsung).
Beispiel
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Milben-tцtendes Reinigungsmittel als Teppich-/Posterreinigungsmittel
Zur Reinigung von Teppichen und Polstern lдsst sich besonders gut die moderne Sprьhextraktion
einsetzen. Wichtig fьr den Erfolg ist die feine Verteilung des Pflanzenцls in der Sprьhlцsung durch
Einsatz eines geeigneten Emulgators. Als Emulgator geeignet ist ein Gemisch verschiedener Tenside,
wie es z. B. fьr flьssige Teppichreiniger eingesetzt wird.
- hoher Anteil an Niotensiden (20 bis ьber 30%)
- geringer bis mittlerer Anteil an anionischen Tensiden (bis zu 15%)
- Wasser ad 100%.
Der Emulgator sollte in einer Menge von 20-35% bezogen auf Цl eingesetzt werden und zusammen
mit dem Цl eine klare Lцsung bilden (Цl-Emulgatorlцsung).
Fьr die Reinigung von 10 mTeppich-/Polsterflдche werden ca. 10 l Sprьhlцsung benцtigt (1 l/m,
Spanne 0,5-2 l/m). Eine 1%ige Konzentration des Цls in der Sprьhlцsung entspricht dem Einsatz
von 100 ml Цl, zusдtzlich 25 ml Emulgator (Lцsung des Цls in 25% Emulgator bezogen auf Цl),
also insgesamt 125 ml Цl-Emulgatorlцsung. Das entspricht einer 80fachen Verdьnnung der ЦlEmulgatorlцsung.
Teppiche und Polstermцbel werden zuerst mit der mit Wasser verdьnnten Цl-Emulgatorlцsung
(Sprьhlцsung) besprьht. Einwirkzeit zum Abtцten der Milben: ca. 30-60 Minuten. Der
Emulgatoranteil bewirkt zusдtzlich die Loslцsung von abgetцteten Milben, Allergenen und weiteren
Schmutzpartikeln. Die Entfernung von toten Milben, deren Allergenen und weiterem Schmutz erfolgt
durch eine anschliessende Extraktion/Saugextraktion unter zusдtzlichem Einsatz eines geeigneten
Teppich-/Polsterreinigungsmittels in mцglichst konzentrierter Form.
Da wдhrend der Einwirkzeit und auch noch nach abschliessender Extraktion in geringem Masse
дtherische Цle im Teppich bzw. im Polster zur Wirkung kommen, empfiehlt sich der Einsatz einer
Kombination an дtherischen Цlen, bei der der Geruch vom Anwender akzeptiert wird. Claims:
166/1651
1. Milbentцtendes Reinigungsmittel, Цl-Emulgatorlцsung, fьr
Betttextilien/Haushaltswдsche/Kleidung, Teppiche und Polster auf der Basis дtherischer
Pflanzenцle zum Einsatz in Therapie und Prдvention atopischer Erkrankungen wie Neurodermitis,
Allergisches Asthma und Allergische Rhinokonjunktivitis, dadurch gekennzeichnet, dass ein
Pflanzenцl mit hohem Anteil an дtherischen Цlen in einer geringstmцglichen Menge Emulgator (20100% bezogen auf Цl) gelцst wird, Цl-Emulgatorlцsung, und die Lцsung zur Herstellung einer
wдssrigen Emulsion zum Einweichen oder Waschen von Textilien in der Waschmaschine bzw. zur
Reinigung/Sprьhextraktion von Teppichen und Polstern genutzt wird.
Anteil der Niotenside im Emulgator: 10 bis ьber 30% Anteil der anionischen Tenside im Emulgator:
bis 20%
2. Milbentцtendes Reinigungsmittel nach Anspruch 1 auf der Basis von Baumцlen wie Teebaumцl
vom Cyneol- und Terpinenoltyp, Eukalyptusцl, Zedernцl, Zypressenцl, Mandelbaumцl.
3. Milbentцtendes Reinigungsmittel nach Anspruch 1 auf der Basis von Pflanzenцlen wie Citronellцl,
Wintergrьnцl, Grьne-Minze-Цl, Kьmmel-Цl und Dill-Цl.
4. Milbentцtendes Reinigungsmittel nach Anspruch 1 auf Basis von essentiellen Hauptbestandtteilen
von Pflanzenцlen wie Cineol, Citronellal, Linalool, d-Carvon, l-Carvon, Salicylsдuremethylester,
Salicylsдureдthylester, Terpinen-4-ol und Menthon.
5. Milbentцtendes Reinigungsmittel nach Anspruch 1-4, dadurch gekennzeichnet, dass fьr das
Einweichen von Textilien das Цl in 20-40 Vol-% Emulgator bezogen auf Цl gelцst wird.
6. Milbentцtendes Reinigungsmittel nach Anspruch 1-4, dadurch gekennzeichnet, dass fьr die Vorund Hauptwдsche von Textilien das Цl in 30-50 Vol-% Emulgator bezogen auf Цl gelцst wird.
7. Milbentцtendes Reinigungsmittel nach Anspruch 1-4, dadurch gekennzeichnet, dass fьr die
Reinigung von Teppichen und Polstern das Цl in 20-40 Vol-% Emulgator bezogen auf Цl gelцst
wird.
167/1651
8. Milbentцtendes Reinigungsmittel nach Anspruch 1-7, dadurch gekennzeichnet, dass als
Emulgator ein Tensidgemisch eingesetzt wird mit dem Hauptbestandteil Niotenside (10-30%
bezogen auf Emulgator).
9. Milbentцtendes Reinigungsmittel nach Anspruch 1-8, dadurch gekennzeichnet, dass das
Pflanzenцl, besonders Eukalyptusцl, in Form von Badeцl eingesetzt wird mit (Цl-EmulgatorLцsung) mit 30-85 Vol-% Pflanzenцl bezogen auf Badeцl.
10. Milbentцtendes Reinigungsmittel nach Anspruch 1-5, 8, 9, dadurch gekennzeichnet, dass das
Цl fьr das Einweichen von Textilien in der Einweich-/Waschflotte in einer Konzentration von 0,2-0,6%
vorliegt.
11. Milbentцtendes Reinigungsmittel nach Anspruch 1-4, 6,8, 9 dadurch gekennzeichnet, dass das
Цl fьr die Vor- und Hauptwдsche von Textilien in der Waschflotte in einer Konzentration von 0,41,0% vorliegt.
12. Milbentцtendes Reinigungsmittel nach Anspruch 1-4, 7-9 dadurch gekennzeichnet, dass fьr die
Reinigung von Teppichen und Polstern das Цl in der Reinigungsflotte, Sprьhlцsung, in einer
Konzentration von 0,5-2,0% vorliegt.
13. Milbentцtendes Reinigungsmittel nach Anspruch 1-5, 8-10 dadurch gekennzeichnet, dass das
Volumen der Einweichemulsion zwecks geringem Gesamtwasserverbrauch wie in modernen
Waschmaschinen reduziert ist auf max. 10 l/kg Textil.
14. Milbentцtendes Reinigungsmittel nach Anspruch 1-5, 8-10, 13, dadurch gekennzeichnet, dass
es in einem durchgehenden Waschprogramm bei 30 DEG , max. 40 DEG C, verwendet wird mit 3060 minьtiger Einweichphase bei nur einer Einspьlung und geringer Umwдlzung (max. 10 x pro Min.),
anschliessendem Abpumpen der Einweichflotte und direktem Anschluss einer fьr die Textilart (auch
Wolle) geeigneten Hauptwдsche.
15. Milbentцtendes Reinigungsmittel nach Anspruch 1-4, 7-9, 12, dadurch gekennzeichnet, dass es
in einem Sprьhextraktionsverfahren, in zwei Schritten eingesetzt wird mit Aufsprьhen der
verdьnnten Цl-Emulgatorlцsung (40-160fache Verdьnnung in Wasser), einer Einweichphase von
30-90 Minuten und anschliessender kombinierter Sprьhextraktion mit einer geeigneten Teppich/Polsterreinigerlцsung.
168/1651
169/1651
41. DE19901408 - 20.07.2000
BALL-SHAPED CHRISTMAS TREE ORNAMENT, CONTAINING ESSENTIAL OIL WITH FIR TREE
SCENT, ESPECIALLY SUITABLE FOR DECORATION OF SCENTLESS CHRISTMAS TREE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE19901408
Applicant(s):
PRODUCTA HAMMER PRODUKTIONS MA (DE)
IP Class 4 Digits: A47G
IP Class:
A47G33/08
E Class: A61L9/12; A47G33/08
Application Number:
DE19991001408 (19990115)
Priority Number: DE19991001408 (19990115)
Family: DE19901408
Abstract:
THE ORNAMENT (1) IS MADE OF BLOWN GLASS, BALL-SHAPED WITH A SHORT TUBULAR TOP
(2), WHICH IS COVERED BY A METAL CAP (3) WITH AN ATTACHED HOLDING BOW (4) FOR THE
INSERTION OF A SHORT METAL STRING. THE ORNAMENT (1)IS FILLED WITH AN ABSORBENT
MATERIAL (5), SOAKED WITH AN ESSENTIAL OIL OR A PERFUME SMELLING OF FIR TREES. THE
SCENT IS EVAPORATED THROUGH THE GAPS BETWEEN THE TUBE-SHAPED TOP (2) AND THE
METAL CAP (3). THE DEVICE (1) CAN BE RE-FILLED BY USING A SMALL PIPETTE.Description:
Die Erfindung betrifft einen Weihnachtsschmuck-Hohlkцrper, insbesondere eine Christbaumkugel,
mit einem oberen, mit dem Inneren des Hohlkцrpers in Verbindung stehenden Stutzen, einer auf
dem Stutzen angeordneten Abdeckkappe und einem die Abdeckkappe sowie den Stutzen
durchsetzenden Halterungsbьgel.
170/1651
Weihnachtsschmuck-Hohlkцrper der genannten Art sind in der Praxis seit Jahren allgemein bekannt.
Das Innere des Hohlkцrpers ist regelmдssig leer.
In neuerer Zeit werden in der Weihnachtszeit zunehmend Nordmanntannen aufgestellt, die den
Nachteil haben, keinen Tannenduft zu verstrцmen. Hier will die Erfindung Abhilfe schaffen.
Der Erfindung liegt die Aufgabe zugrunde, einen Weihnachtsschmuck-Hohlkцrper der eingangs
genannten Art so auszubilden, dass er in einem Weihnachtsbaum hдngend weihnachtlichen Duft
verstrцmt.
Die erfindungsgemдsse Lцsung dieser Aufgabe besteht darin, dass das Innere des Hohlkцrpers
zumindest teilweise mit einem natьrlichen oder synthetischen Vliesmaterial oder einem porцsen
Trдgermaterial, das jeweils mit einem дtherischen Цl getrдnkt ist oder einem Duftgel gefьllt ist.
Bei dem erfindungsgemдssen Weihnachtsschmuck-Hohlkцrper wird das den Weihnachts- bzw.
Tannenduft verstrцmende Цl im Inneren des Hohlkцrpers allmдhlich verdampft. Es diffundiert dann
durch den Stutzen und die in der Abdeckkappe vorgesehene Цffnung fьr den Halterungsbьgel
sowie die unvermeidbaren Zwischenrдume zwischen dem Stutzen und der Abdeckkappe nach
draussen.
Im folgenden wird die Erfindung anhand einer ein Ausfьhrungsbeispiel darstellenden Zeichnung
nдher erlдutert.
Die einzige Figur der Zeichnung zeigt einen Weihnachtsschmuck-Hohlkцrper 1 in Form einer
Christbaumkugel mit einem oberen, mit dem Inneren des Hohlkцrpers 1 in Verbindung stehenden
Stutzen 2, der im Zuge des Blasens des Hohlkцrpers 1 entsteht. Auf den Stutzen 2 ist eine
Abdeckkappe 3 aufgesetzt. Diese sowie der Stutzen 2 werden von einem federnden
Halterungsbьgel 4 durchsetzt, mit dem der Weihnachtsschmuck-Hohlkцrper 1 gegebenenfalls unter
Zuhilfenahme eines kurzen Drahtstьckes an einem Christbaum befestigt werden kann.
Das Innere des Hohlkцrpers 1 ist zum ьberwiegenden Teil mit einem natьrlichen Vliesmaterial 5
gefьllt. Dieses Vliesmaterial 5 ist mit einem дtherischen Цl oder Parfьmцl getrдnkt, das Tannenbzw. Weihnachtsduft verstrцmt. Das verdampfende Цl diffundiert durch den Stutzen 2 und die
Abdeckkappe 3 nach draussen.
171/1651
Ist das Цl erschцpft, kann nach Anheben der Abdeckkappe 3 und des Halterungsbьgels 4 mit Hilfe
einer Pipette neues Цl nachgefьllt werden.Claims:
Weihnachtsschmuck-Hohlkцrper, insbesondere Christbaumkugel, mit einem oberen, mit dem
Inneren des Hohlkцrpers in Verbindung stehenden Stutzen, einer auf dem Stutzen angeordneten
Abdeckkappe und einem die Abdeckkappe sowie den Stutzen durchsetzenden Halterungsbьgel,
dadurch gekennzeichnet, dass das Innere des Hohlkцrpers (1) zumindest teilweise mit einem
natьrlichen oder synthetischen Vliesmaterial (5) oder einem porцsen Trдgermaterial, das jeweils mit
einem дtherischen Цl oder einem Parfьmцl getrдnkt ist, oder einem Duftgel gefьllt ist.
172/1651
42. DE19922193 - 16.11.2000
STABLE, SOLUBILIZER-FREE, WATER-DILUTABLE ESSENTIAL OIL CONCENTRATE
FORMULATION, USEFUL E.G. IN PHARMACEUTICAL, COSMETIC OR FOOD APPLICATIONS,
COMPRISING LIPOSOMES BASED ON HYDROGENATED LECITHIN
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE19922193
Inventor(s):
SONNENBERG FRANK (DE)
Applicant(s):
SONNENBERG FRANK (DE)
IP Class 4 Digits: A61K; A61L; A01N; A23L; C11D
IP Class:
A61K7/46; A61L9/01; A01N65/00; A61K7/16; A61K7/00; C11D3/50; A01N25/28;
C11D3/48; A61K9/50; A23L1/22; A23L1/03; A61L2/16; C11D9/44
E Class: A61L9/01; A01N65/00+M; C11D3/50; A23L1/22B2; A61K7/16P; A61K7/46P; A61K7/50;
A61K9/127; C11D17/00D
Application Number:
DE19991022193 (19990512)
Priority Number: DE19991022193 (19990512)
Family: DE19922193
Abstract:
A CONCENTRATE FORMULATION, WHICH CAN BE DILUTED HOMOGENEOUSLY WITH WATER,
COMPRISING AN ESSENTIAL OIL MICROENCAPSULATED IN AN AQUEOUS LIPOSOME SYSTEM,
COMPRISES (BY WEIGHT) 0.01-20.00 % HYDROGENATED LECITHIN, (0.10-50.00 % ESSENTIAL
OILS, AND 35.00-99.00% WATER, IS NEW. AN INDEPENDENT CLAIM IS ALSO INCLUDED FOR
THE PREPARATION OF (I), BY PREPARING AN EMPTY LIPOSOME SYSTEM ABOVE THE PHASE
TRANSITION TEMPERATURE THEN CHARGING WITH THE ESSENTIAL OILS.Description:
173/1651
Die vorliegende Erfindung betrifft ein wasserlцsliches Konzentrat, bestehend aus дtherischen Цlen
mikroverkapselt in einem Liposomensystem, ein Verfahren zu seiner Herstellung und die
Verwendung.
Дtherische Цle werden in den unterschiedlichsten Bereichen eingesetzt und ihr Gebrauch hat eine
lange Tradition. Verwendet werden дtherische Цle unter anderem als Aroma-, Duft-, Heil- und
Wirkstoffe (Monographien des BGA; Hagers Handbuch der Pharmazeutischen Praxis, Springer 1998).
In ihrer reinen Konzentration entfalten die meisten дtherischen Цle jedoch eine starke Reizwirkung
und wirken toxisch. Es ist aus diesem Grund notwendig дtherische Цle vor einer Anwendung durch
geeignete Verdьnnung in eine zweckmдssige Konzentration zu ьberfьhren. Die Verdьnnung fьr die
meisten Anwendungen sollte aufgrund der gewьnschten Neutralitдt des Lцsungsmittels mit Wasser
durchgefьhrt werden.
Дtherische Цle sind mit Wasser in der Regel nicht mischbar. Sie bestehen aus einem sehr
vielfдhigen und bisweilen aggressiven Stoffgemisch. Bei der Emulsion von дtherischen Цlen
werden die Emulgierleistungen der meisten ьblichen Emulgatoren ьberfordert. Ein wasserlцsliches
Konzentrat mit дtherischen Цlen erfordert deshalb den Einsatz eines oder mehrerer spezieller
Lцsungsvermittler.
Stand der Technik ist, Alkohole oder/und ethoxylierte Verbindungen als Lцsungsvermittler fьr
wasserlцsliche Konzentrate mit дtherischen Цlen einzusetzen. Diese Lцsungsvermittler haben
jedoch bei der Zubereitung von Konzentraten erhebliche Nachteile:
- Sie haben eine hohe toxische Komponente.
- Sie mьssen in grossen Mengen eingesetzt werden, um eine homogene Verteilung des
Konzentrats bei der Verdьnnung mit Wasser zu erzielen.
- ethoxylierte Verbindungen haben eine stark konsistenzerhцhende Wirkung auf das Produkt.
In verschiedenen Schriften wird die Mikroverkapselung in einem Liposomensystem als geeignetes
Verfahren zur Lцsung von in Wasser unlцslichen Stoffen genannt (WO 98/36735). Aus Lecithin
hergestellte Liposomensysteme eignen sich hervorragend dazu, stabile fettfreie Lцsungen mit einem
hohen Anteil дtherischer Цle durch Beladung herzustellen. Die liposomale Mikroverkapselung
schьtzt die дtherischen Цle gegen Oxidation, verbessert ihre Hautvertrдglichkeit und erzeugt einen
174/1651
lang anhaltenden Effekt, bei dem die verkapselten Wirkstoffe zeitlich gestaffelt abgegeben werden
(DE 41 22 744). Beladene Liposomensysteme aus ungesдttigtem Lecithin besitzen jedoch den
Nachteil, dass sie nicht ohne den Eintrag von Energie oder Zusatz von Co-Emulgatoren oder/und
Alkoholen als Hilfsstoffe bei der Verdьnnung mit Wasser homogen verteilen (DE 32 25 706, DE 40 21
083).
Der vorliegenden Erfindung liegt die Aufgabe zugrunde, ein sich bei der Verdьnnung mit Wasser
homogen verteilendes Konzentrat mit дtherischen Цlen herzustellen, das die Vorteile eines
Liposomensystems aufweist und keine weiteren Lцsungsvermittler enthдlt.
Diese Aufgabe wird erfindungsgemдss durch die im Patentanspruch 1 aufgefьhrten Merkmale der
Mikroverkapselung von дtherischen Цlen in einem Liposomensystem aus hydriertem Lecithin
gelцst.
Im Gegensatz zu Liposomensystemen aus ungesдttigtem Lecithin erfolgt nach der Verdьnnung
dieses Liposomensystems aus hydriertem Lecithin mit Wasser eine homogene Verteilung, ohne das
weitere Energie oder Lцsungsvermittler zugefьhrt werden mьssen. Ein weiterer Vorteil ist die
Stabilitдt dieses Liposomensystems aus hydriertem Lecithin gegenьber Liposomensystemen aus
ungesдttigtem Lecithin (M. Tagawa et al., Preprints XIVth IFSCC Congress, Barcelona 1986, Vol. 1,
L.2.10, 395; M. Schneider, Med-Report 14/13, 1-4, 1989). Auch nach einer Lagerung von mehreren
Jahren konnte keine Neigung zur Bodensatzbildung festgestellt werden.
Die Herstellung eines Konzentrats durch Mikroverkapselung von дtherischen Цlen in einem
wдssrigen Liposomensystem aus hydriertem Lecithin das sich bei der Verdьnnung mit Wasser
homogen verteilt, sollte unter folgenden Gesichtspunkten erfolgen:
- Das Verhдltnis von hydriertem Lecithin und дtherischen Цl sollte so gewдhlt werden, dass das
fertige Liposomensystem eine wдssrige Konsistenz aufweist und sich homogen mit Wasser
verdьnnen lдsst.
- Liposomensysteme zeichnen sich unter anderem durch eine hohe Penetrationsfдhigkeit der Haut
aus. Um die Einschleusung von toxischen Stoffen in die Haut so gering wie mцglich zu halten,
sollten der Anteil und die Zusammensetzung der дtherischen Цle so gewдhlt werden, dass auf eine
weitere Konservierung des Liposomensystems verzichtet werden kann.
175/1651
- Um oxidative Wirkungen auszuschliessen, sollte der Herstellungsprozess und das Abfьllen des
Liposomensystems unter Schutzgas erfolgen.
Дtherische Цle sind leichtflьchtig und dementsprechend sehr temperaturempfindlich. Ab einer
Verarbeitungstemperatur von 30 DEG C muss mit deutlichen Qualitдtseinbussen der дtherischen
Цle gerechnet werden. Um den Einsatz von hydriertem Lecithin als entscheidendem Kostenfaktor
bei der Herstellung eines Liposomensystems so gering wie mцglich zu haften ist es erforderlich, die
Liposomenbildung oberhalb der Phasenumwandlungstemperatur von hydriertem Lecithin
vorzunehmen. Abhдngig von der Zusammensetzung des hydrierten Lecithins liegt die
Phasenumwandlungstemperatur zwischen 40 DEG -60 DEG C. Die unterschiedlichen
Temperaturanforderungen von дtherischen Цlen und hydriertem Lecithin fbhren zu der
Notwendigkeit, zuerst ein Leerliposomensystem aus hydriertem Lecithin mittels eines hochtourigen
Mixers (Rotor-Stator, etc.) oberhalb der dafьr notwendigen Phasenьbergangstemperatur
herzustellen. Anschliessend wird dieses Leerliposomensystem nach einer Abkьhlungsphase auf
unter 30 DEG C unter permanenter Kьhlung mit дtherischen Цlen beladen und homogenisiert. Bei
Bedarf kann die Einstellung des optimalen osmotischen Druckes mit organischen oder
anorganischen Salzen durchgefьhrt werden. Die Einstellung eines gewьnschten pH-Wertes kann mit
Sдuren oder Laugen erfolgen. Um trьbe oder milchige Konzentrate herzustellen kann die
Homogenisierung ebenfalls mittels hochtourigem Mixer durchgefьhrt werden. Mit einer
nachfolgenden Hochdruckhomogenisation oder Ultraschallbehandlung ist jedoch auch die
Herstellung optisch transparenter Konzentrate mцglich.
Die so hergestellten Konzentrate kцnnen in den unterschiedlichsten Anwendungsbereichen
eingesetzt werden. Beispiele fьr den Einsatz dieser Konzentrate liegen in der Verwendung als
Mundwasser, Badezusatz, Saunaaufguss, Aromazusatz, Parfьm, Desinfektions- und
Reinigungsmittel. Ein weiterer Vorteil dieser Konzentrate ist ihre problemlose Einarbeitung in
hautfreundliche Gele, Salbengrundlagen, Hygieneartikel.
Entsprechend den gewьnschten Konzentrationen an дtherischen Цlen und dem
Verwendungszweck der Konzentrate kцnnen die Gehalte der einzelnen Komponenten in folgenden
Grenzen varieren:
Columns=2>
Wasser25,00-99,00 Gew.-%
176/1651
Die nachfolgenden Beispiele orientieren sich an den oben gemachten Herstellungsvorschriften.
Beispiel 1
Mundwasserkonzentrat
Columns=2>
02,00 Gew.-%
Menthol02,00 Gew.-%
Wintergrьnцl00,50 Gew.-%
Teebaumцl03,50 Gew.-%
Nelkenцl00,25 Gew.-%
Anisцl02,00 Gew.-%
Origanumцl00,75 Gew.-%
100,00 Gew.-%
Beispiel 2
Badezusatz
Columns=2>
10,00 Gew.-%
Eucalyptusцl05,00 Gew.-%
100,00 Gew.-%
Einstellung des pH-Werts auf 5,5 mit Milchsдure.
177/1651
Beispiel 3
Saunaaufgusskonzentrat
Columns=2>
04,00 Gew.-%
Latschenkiefernцl09,00 Gew.-%
Kamillenцl01,00 Gew.-%
Pfefferminzцl01,00 Gew.-%
100,00 Gew.-%
Beispiel 4
Aromakonzentrat fьr Erfrischungsgetrдnke
Columns=2>
11,00 Gew.-%
Zitronenцl06,20 Gew.-%
100,00 Gew.-%
Beispiel 5
Desinfektionsmittelkonzentrat
178/1651
Columns=2>
18,00 Gew.-%
Nelkenцl03,00 Gew.-%
Origanumцl03,00 Gew.-%
100,00 Gew.-%
Beispiel 6
Reinigungskonzentrat
Columns=2>
Claims:
1. Formulierung zur Zubereitung eines mit Wasser homogen verdьnnbaren Konzentrates, bestehend
aus дtherischen Цlen mikroverkapselt in einem wдssrigen Liposomensystem, dadurch
gekennzeichnet, dass sie
1. 0,01 Gew.-% bis 20,00 Gew.-% hydriertes Lecithin und
2. 0,10 Gew.-% bis 50,00 Gew.-% дtherische Цle und
3. 25,00 Gew.-% bis 99,00 Gew.-% Wasser enthдlt.
2. Formulierung nach Anspruch 1, dadurch gekennzeichnet, dass das hydrierte Lecithin zu 15 Gew.% bis 99 Gew.-% aus Phosphatidylcholin besteht.
3. Formulierung nach Anspruch 1 dadurch gekennzeichnet, dass sie keine weiteren
Lцsungsvermittler enthдlt.
179/1651
4. Formulierung nach Anspruch 1, dadurch gekennzeichnet, dass sie keine Alkohole und/oder
ethoxylierte Verbindungen enthдlt.
5. Formulierung nach Anspruch 1, dadurch gekennzeichnet, dass sie keine Konservierungsmittel
enthдlt.
6. Formulierung nach Anspruch 1, dadurch gekennzeichnet, dass im Bedarfsfall organische oder
anorganische Salze zur Einstellung des osmotischen Drucks, Sдuren oder Laugen zur Einstellung
des pH-Werts zugegeben werden.
7. Verfahren nach einem der Ansprьchen 1-6, dadurch gekennzeichnet, dass zur Herstellung eines
Konzentrates zuerst ein Leerliposomensystem oberhalb der dafьr notwendigen
Phasenьbergangstemperatur hergestellt wird, dass anschliessend bei einer Temperatur unter 30
DEG C mit дtherischen Цlen beladen wird.
8. Verwendung der Formulierung nach Ansprьche 1-6 als Pharmazeutikum, Kosmetikum, Lebens-,
Haushalts- oder Hygienemittel oder zur Zusammensetzung und Erzeugung dieser Mittel.
180/1651
43. DE19962426 - 26.07.2001
PERFUME COMPOSITION FOR VAPORIZATION INTO THE AIR OF A ROOM COMPRISES AN
ESSENTIAL OIL AND AN EMULSIFIER
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE19962426
Inventor(s):
MAUSE SILKE (DE)
Applicant(s):
MAUSE SILKE (DE)
IP Class 4 Digits: C11B; B01D; A61M
IP Class:
C11B9/00; A61M15/00; B01D1/00
E Class: A61L9/01; A61L9/013
Application Number:
DE19991062426 (19991222)
Priority Number: DE19991062426 (19991222)
Family: DE19962426
Abstract:
PERFUME COMPOSITION FOR VAPORIZATION INTO THE AIR OF A ROOM COMPRISES 70-95
VOL.% ESSENTIAL OIL AND 5-30 VOL.% EMULSIFIERDescription:
Die Erfindung betrifft ein Duftцl fьr die Verdunstung in Raumluft mit Hilfe eines Verdampfers,
Duftbrunnen oder dergleichen.
Zur Erzeugung einer behaglichen Atmosphдre in Rдumen von Gebдuden, die beispielsweise als
Wohnung oder Bьros genutzt werden, ist der Einsatz von Aromen durchaus ьblich. Als Trдger von
181/1651
Aromen dienen hierbei vor allem дtherische Цle, die auf natьrliche Weise gewonnen oder
synthetisch hergestellt sind.
Um eine mцglichst gute Verbreitung des Aromas in dem betreffenden Raum zu erreichen, werden
Hilfsmittel benutzt, die die Aufnahme der Aromastoffe von der Raumluft und deren Verbreitung im
Raum beschleunigen. Solche Hilfsmittel sind beispielsweise Brunnen oder Verdampfer, durch die
der Feuchtigkeitsgehalt der Luft begьnstigt wird. Dabei wird dem Wasser des Brunnens oder
Verdampfers ein дtherisches Цl als sogenanntes Duftцl zugesetzt. Die ьblicherweise im Handel
erhдltlichen Duftцle sind nicht bzw. nur ungenьgend fьr die Verwendung in Verdampfergerдten
oder Duftbrunnen geeignet. Dies ist darin begrьndet, dass das дtherische Цl (Duftцl) und Wasser
eine Emulsion bilden, das heisst, das Duftцl mischt sich nicht mit Wasser, sondern schwimmt als
Fettaugen an der Wasseroberflдche. Hierdurch ist auch die Verdampfung des дtherischen Цls
unzureichend, so dass Rьckstдnde in der Verdampfungseinrichtung bzw. dem Brunnen gebildet
werden, die regelmдssige Reinigungsarbeiten erforderlich machen.
Um diesem Problem zu begegnen, wurde bereits vorgeschlagen, eine Mischung aus дtherischem
Цl und mehreren Emulgatoren in Kombination sowie einem Lцsungsvermittler zu erzeugen, wofьr
jedoch ein erheblicher Aufwand fьr die Bemessung der jeweiligen Anteile der mehreren Emulgatoren
und des Lцsungsvermittlers und die entsprechende Vermischung aller Komponenten erforderlich ist.
Der vorliegenden Erfindung liegt daher die Aufgabe zugrunde, ein Duftцl fьr Verdampfer,
Duftbrunnen oder dergleichen zu schaffen, das einfacher und kostengьnstiger herstellbar ist.
Diese Aufgabe wird durch ein Duftцl mit den Merkmalen des Anspruchs 1 gelцst.
Durch die erfindungsgemдsse Mischung, aus der das Duftцl besteht, ist die erforderliche
Wasserlцslichkeit des дtherischen Цls gegeben und zwar durch Herabsetzen der
Grenzflдchenspannung zwischen den beiden Phasen der Emulsion. Da lediglich ein einziger
Emulgator benцtigt wird, ist die Herstellung des Duftцls дusserst einfach und kostengьnstig.
Wegen der ausserordentlich guten Lцslichkeit im Wasser erfolgt eine Verdampfung ohne
nennenswerte Rьckstдnde, so dass rьckstandsbedingte Reinigungsarbeiten nicht erforderlich sind.
Das Duftцl enthдlt ausschliesslich Stoffe, die nicht aggressiv gegen die in Duftbrunnen und
Verdampfern verwendeten Materialen sind, so dass beispielsweise Pumpen, Verdampferflдchen
oder dergleichen nicht angegriffen werden.
182/1651
Ein weiterer Vorteil des Duftцls wird darin gesehen, dass das in Wasser gelцste Duftцl nicht
schдumt. Als besonders zweckmдssig wird angesehen, dass die Mischung ausschliesslich aus
dem дtherischen Цl und dem einzigen Emulgator besteht, so dass keine weiteren Bestandteile
enthalten sind. Das Mischungsverhдltnis von дtherischem Цl zu Emulgator kann innerhalb der im
Anspruch 1 angegebenen Bandbreite durchaus variiert werden, wobei als besonders zweckmдssig
ein Mischungsverhдltnis von дtherischem Цl zu Emulsion von mindestens annдhernd 9 : 1
angesehen wird. Daneben wird aber auch bei einem Mischungsverhдltnis von 8 : 2 noch eine gute
Wasserlцslichkeit und gute Verdunstung ohne nennenswerte Rьckstдnde erreicht.
Der einzige Emulgator besteht vorzugsweise aus Alkohol, wobei hier insbesondere vergдllter Alkohol
Nr. 611 benutzt wird. Dabei hat Alkohol in der Duftцlmischung eine doppelte Funktion, nдmlich die
Wirkung als Emulgator und zusдtzlich die Wirkung als Trдgerstoff fьr Duftpigmente. Claims:
1. Duftцl fьr die Verdunstung in Raumluft mit Hilfe eines Verdampfers, Duftbrunnen oder dergleichen,
das im wesentlichen aus einem дtherischen Цl, dem ein Emulgator beigemischt ist, besteht, wobei
der Anteil des дtherischen Цls am Gesamtvolumen der Mischung mindestens 70% und maximal
95% betrдgt und das Restvolumen im wesentlichen aus einem einzigen Emulgator besteht.
2. Duftцl nach Anspruch 1, dadurch gekennzeichnet, dass das Restvolumen der Mischung
ausschliesslich aus dem einzigen Emulgator besteht.
3. Duftцl nach Anspruch 1 oder 2, dadurch gekennzeichnet, das das Mischungsverhдltnis von
дtherischem Цl zu Emulgator etwa 82 betrдgt.
4. Duftцl nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass das Mischungsverhдltnis von
дtherischem Цl zu Emulgator mindestens annдhernd 9 : 1 betrдgt.
5. Duftцl nach einem der Ansprьche 1 bis 4, dadurch gekennzeichnet, dass als einziger Emulgator
Alkohol vorgesehen ist.
183/1651
44. DE3540515 - 21.05.1987
USE OF A PLASTER RELEASING AN ESSENTIAL OIL AND THE PLASTER ITSELF
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=DE3540515
Inventor(s):
KASTELL WOLFGANG (DE)
Applicant(s):
KASTELL WOLFGANG (--)
IP Class 4 Digits: A61L; A61F
IP Class:
A61F13/02; A61L15/03
E Class: A61F5/56; A61F13/02; A61K9/70
Application Number:
DE19853540515 (19851115)
Priority Number: DE19853540515 (19851115)
Family: DE3540515
Abstract:
THE INVENTION RELATES TO A PLASTER FOR MEDICINAL PURPOSES AND THE USE THEREOF.
IN THE PRIOR ART THERE HAVE BEEN A WIDE VARIETY OF DIFFERENT ATTEMPTS TO PREVENT
INDIVIDUALS FROM SNORING. HOWEVER, THE SUCCESS OF SUCH MEANS AND DEVICES WAS
ALWAYS VERY LIMITED OR EVEN INVOLVED UNPLEASANTNESS. THE INVENTION PROVIDES A
REMEDY HERE AND ENVISAGES A SIMPLE PLASTER WHICH CAN BE FASTENED ON THE UPPER
LIP BEFORE RETIRING TO BED AND WHICH CAUSES A REDUCTION IN SWELLING OF THE
NASAL MUCOSA SLOWLY BY THE RELEASE OF ESSENTIAL OILS, SO THAT SNORING IS
PREVENTED. Description:
184/1651
Die vorliegende Erfindung betrifft die Verwendung eines дtherische Цle freisetzenden Pflasters
sowie das Pflaster selbst.
Herkцmmliche Pflaster werden in der Medizin in den unterschiedlichsten Formen und Grцssen zu
verschiedenen Anwendungszwecken eingesetzt. So ist z.B. das ABC-Pflaster zur Behandlung von
rheumatischen Erkrankungen oder auch das Gutaplast- Pflaster (beide Warenzeichen der Firma
Beiersdorf AG) bekannt.
Bisher hat man jedoch kein zuverlдssiges Mittel gegen Schnarchen gefunden. Schnarchen entsteht
dadurch, dass die wдhrend des Schlafens erschlafften Gaumensegel flattern und zwar infolge der
wechselnden Druckdifferenz zwischen Nasenrachenraum und Mund bzw. infolge Verkleinerung der
Rachenhцhle durch die im Schlaf zurьckgesunkene Zunge. Besonders gesundheitsgefдhrdend ist
dabei der sog. Schnarchkrampf (Rhenchospasmus), welcher bei Hysterie und dergl. auftreten kann.
Da viele Personen durch das Schnarchen betroffen sind und nach Abhilfe suchen, hat man auch
schon versucht, Nasensprays einzusetzen, die дtherische Цle als Bestandteil aufweisen. Das
direkte Auftragen solcher Substanzen auf die Nasenschleimhдute brachte jedoch gewisse Nachteile
bezьglich ihrer Konzentration und ihrer unzureichenden anhaltenden Wirkung mit sich.
Der vorliegenden Erfindung liegt deshalb die Aufgabe zugrunde, hier Abhilfe zu schaffen und der
schnarchenden Person ein Mittel zur Verfьgung zu stellen, das das Schnarchen mцglichst
anhaltend verhindert, ohne besondere Unannehmlichkeiten hervorzurufen.
Diese Aufgabe wird durch die Verwendung eines дtherische Цle freisetzenden Pflasters gemдss
Anspruch 1 bzw. durch das Pflaster gemдss Anspruch 2 gelцst.
Ьberraschenderweise hat sich also gezeigt, dass das erfindungsgemдsse Pflaster eine
Abschwellung der Nasenschleimhaut fьr lдngere Zeit bewirkt, da die дtherischen Цle aufgrund
ihres Dampfdrucks aus der Emulsion freigesetzt und durch das Atmen von den Nasengдngen
aufgenommen und zu den Schleimhдuten gefьhrt werden. Hierdurch wird erfindungsgemдss das
Schnarchen verhindert bzw. erheblich gemindert, da die Atemwege zu den Bronchien und den
Lungen selbst freigehalten werden.
Von besonderer erfindungsgemдsser und vorteilhafter Bedeutung ist die Tatsache, dass die
дtherischen Цle in Form einer emulgierten Creme vorliegen, so dass sie nicht ad hoc in die
185/1651
Umgebungsluft freigesetzt werden, sondern ihre Dдmpfe aus der Gaze und der Emulsion heraus
praktisch schubweise inhaliert werden.
Weitere Vorteile und Merkmale gehen aus den vorstehenden Unteransprьchen hervor.
Im folgenden wird ein bevorzugtes Ausfьhrungsbeispiel anhand der Zeichnung nдher erlдutert.
Es zeigt:
Fig. 1 eine schematische Draufsicht auf ein erfindungsgemдsses Pflaster; und
Fig. 2 eine schematische Querschnittsansicht des in Fig. 1 gezeigten erfindungsgemдssen Pflasters.
In den Fig. 1 und 2 ist das erfindungsgemдsse Pflaster allgemein mit 10 bezeichnet. Es weist eine
rechteckige Form auf und ist stark vergrцssert und vereinfacht dargestellt. Es dьrfte jedoch
einleuchten, dass Form und Grцsse des Pflasters sich in einem geeigneten Rahmen verдndern
lassen und nicht kritisch sind.
Das Pflaster 10 besteht aus dem eigentlichen Trдger 12, welcher beidseitig im wesentlichen
vollflдchig eine Klebeschicht (nicht dargestellt) aufweist. Vor Gebrauch kann die Unter- bzw.
Innenseite mit Schutzfolie(n) oder dergl. versehen sein, die dann zum Gebrauch abgenommen
werden, so dass das Pflaster 10 dann an der Oberlippe der normalerweise schnarchenden Person
vor dem Schlafengehen wieder lцsbar angeklebt werden kann. Die Ober- bzw. Aussenseite des
erfindungsgemдssen Pflasters 10 besitzt eine im wesentlichen vollflдchig ausgebildete Gaze- oder
Mullschicht 14. Es versteht sich, dass auch diese Gazeschicht 14 nicht unbedingt vollflдchig sein
muss, sondern sich ggf. auf einige Oberflдchenbereiche des Pflasters 12 beschrдnken lдsst. Auch
lдsst sich ebenso das Material dieser Schicht 14 im geeigneten Rahmen ersetzen, sofern
sichergestellt ist, dass die mit 16 angedeuteten дtherischen Цle bzw. diese in Form einer
emulgierten Creme von ihr sicher aufgenommen werden und eine langsame Freisetzung der
дtherischen Dдmpfe durch das Einatmen der schnarchenden Person gewдhrleistet ist. Claims:
186/1651
1. Verwendung eines дtherische Цle freisetzenden Pflasters auf der Oberlippe zur Abschwellung
der Nasenschleimhaut, insbesondere zur Verhinderung des Schnarchens.
2. Pflaster fьr Heilzwecke mit Klebe- und Gazeschicht sowie organischem Wirkstoff, dadurch
gekennzeichnet, dass die Gazeschicht im wesentlichen die Aussenseite des Pflasters vollstдndig
bedeckt und mit дtherischen Цlen und dergl. versehen ist, deren Freisetzung ein Abschwellen der
Nasenschleimhaut bewirkt.
3. Pflaster nach Anspruch 2, dadurch gekennzeichnet, dass die дtherischen Цle in Form einer
emulgierten Creme auf die Gazeschicht aufgetragen sind.
4. Pflaster nach Anspruch 2 und 3, dadurch gekennzeichnet, dass die дtherischen Цle
leichtflьchtig sind bzw. einen hohen Dampfdruck aufweisen.
5. Pflaster nach Anspruch 2 bis 4, gekennzeichnet durch eine rechteckige Form von insbesondere
2,5 cm Lдnge und 1,5 cm Breite.
6. Pflaster nach Anspruch 2, gekennzeichnet durch zwei Klebeseiten, von denen eine mit der
Gazeschicht im wesentlichen vollstдndig verbunden ist.
7. Pflaster nach Anspruch 2 bis 6, dadurch gekennzeichnet, dass folgende дtherische Цle
eingesetzt werden: Oleum Menthae pip., insbes. 1 Gew%
Oleum Eucalyptus
Oleum Pini
Salbengrundlage: Цl-Wasser- Emulsion.
187/1651
45. EG18156 - 30.01.1994
IMPROVED EXTRACTS AND ESSENTIAL OIL OBTAINED FROM THE NEW VARIETY CAMOMILE
MANZANA
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EG18156
Applicant(s):
PHARMA A G (--)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
EG19850000034 (19850121)
Priority Number: EG19850000034 (19850121)
Family: EG18156
188/1651
46. EP0130027 - 20.05.1986
GROWTH INHIBITOR FOR CARIOGENIC BACTERIA
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP0130027
Inventor(s):
SATO TOSHIYA (JP); YAMAGUCHI YUZO (JP)
Applicant(s):
TAKASAGO PERFUMERY CO LTD (JP)
IP Class 4 Digits: A61K
IP Class:
A61K31/045
E Class: A61K31/045; C11B9/00; A23G3/30+D4; A61K7/16D2
Application Number:
US19840622598 (19840620)
Priority Number: JP19830110113 (19830621)
Family: EP0130027
Equivalent:
DK299184; JP1599506; JP2025890; JP60004126
Abstract:
A GROWTH INHIBITOR FOR CARIOGENIC BACTERIA WHICH COMPRISES CONTAINING THEREIN
L- ALPHA -CADINOL AS AN ACTIVE INGREDIENT. IN PARTICULAR, THE EFFECT OF GROWTH
INHIBITION TO STREPTOCOCCUS MUTANS IPCR 1009 STRAIN CAN BE PRODUCED AT A
CONCENTRATION OF 1/50,000.Description:
FIELD OF THE INVENTION
The present invention relates to a growth inhibitor for cariogenic bacteria. More particularly, it relates
to a growth inhibitor for cariogenic bacteria which comprises containing therein l-.alpha.-cadinol as
an active ingredient.
189/1651
BACKGROUND OF THE INVENTION
The caries is generally referred to as a decayed tooth. It is caused by Streptococcus mutans and
other lactic acid bacteria indigenous to the oral cavity which form lactic acid in the bacterial plaque
resulting from sucrose etc. in the food. The lactic acid dissolves calcium in the tooth. (This is called
decalcification.)
Heretofore, several attempts have been made to prevent caries. They include use of antibiotics,
fungicides, an enzyme which dissolves cell walls and medicines having the antibacterial action to
prevent the growth of cariogenic bacteria. They also include use of polysaccharide hydrolase to
prevent the formation of bacterial plaque. However, those have a disadvantage of disturbing the
bacterial flora in the oral cavity and intestine and destroying the natural balance among bacteria. In
addition, the use of antibiotics tend to produce side effects. These disadvantages in practical use
have not been overcome yet.
In view of these circumstances, as a result of a series of investigations in search for a material having
a high antibacterial activity specifically for cariogenic bacteria, it has been found that some of natural
vegetable essential oils have such antibacterial activity, such a material is commonly contained in the
essential oils, such is l-.alpha.-cadionol, and this material has the properties to achieve the object of
this invention. The present invention has been attained on the basis of this finding.
SUMMARY OF THE INVENTION
Accordingly, an object of this invention is to provide a growth inhibitor for cariogenic bacteria which
comprises containing therein l-.alpha.-cadinol as an active ingredient.
DETAILED DESCRIPTION OF THE INVENTION
The l-.alpha.-cadinol used in this invention is the conventional compound represented by the
structural formula:
This compound is a colorless crystal having a melting point of 74 DEG to 74.5 DEG C. and an optical
rotation of [.alpha.]D@20 =-46 DEG (in ethanol). The compound is contained in cubeb oil, Java
citronella oil, juniper berry oil, and cade oil. The compound is also contained in the creeping pine
leave oil produced in Japan.
190/1651
l-.alpha.-Cadinol can be isolated from these essential oils by the conventional method such as
fractional distillation or silica gel column chromatography.
The cariogenic bacteria growth inhibitor containing l-.alpha.-cadinol according to this invention can
be used in the form of a solution by dissolving it in an organic solvent such as ethanol, propylene
glycol or glycerine, which casues no problem in the oral cavity, because l-.alpha.-cadinol is hardly
soluble in water but soluble in an organic solvent such as alcohols. The inhibitor can also be used in
the form of an emulsion by emulsifying it in water using a surfactant such as Span 20 (a product of
Atlas Powder Co.). Moreover, it is also possible to make such an emulsion into a waterdispersible
powder by adding dextrin thereto followed by spray drying. Thus, the growth inhibitor of this
invention can be used in various forms depending upon the purpose of use thereof. The inhibitor can,
of course, be used in combination with other medicines, if desired.
l-.alpha.-Cadinol performs bacteriostatic action on cariogenic bacteria, and its bactericidal action is
mild. Therefore, l-.alpha.-cadinol can be suitably added to chewing gum, candy, troche, wheat
gluten, and other foods which stay in the oral cavity for a long time, in the form of a propylene glycol
or glycerine solution. Further, l-.alpha.-cadinol can be suitably added to toothpaste and mouth wash
in the form of an emulsion and to tooth powder in the form of a powder.
The growth inhibitor of this invention can completely inhibit the growth of Streptococcus mutans
RIMD 3125001 strain which causes caries under the anaerobic condition in the medium, at a
concentration of 1/50,000 of l-.alpha.-cadinol. However, when used at the same concentration, the
inhibitor did not inhibit at all the growth of enteric bacteria such as Bacteroides microfusus IPCR
1009 strain and Escherichia coli ATCC 10789 strain (which are both aerobic) and Bifidobacterium
adolescentis (which is absolutely anaerobic). The inhibitor exhibited a slight antibacterial action
against gram-positive bacteria such as Bacillus subtilis, Pseudomonas aeruginosa, and
Staphylococuss aureus under the aerobic conditions; but did not exhibit any antibacterial action
against gram-negative bacteria and molds such as Aspergillus nigar, Candida albicans, and
Klebsiella pneumoniae.
The effectiveness of the growth inhibitor of this invention was not affected by a surfactant such as
sodium laurylsulfonate or "Span 20".
191/1651
Where the cariogenic bacteria growth inhibitor of this invention is incorporated into foods or dentifrice,
it is preferred that the concentration thereof be slightly higher than the effective concentration
(1/50,000), because the contact time of the food or dentifrice to cariogenic bacteria is comparatively
short.
Any essential oil containing l-.alpha.-cadinol may be used for the object of this invention. It is
however preferred that the essential oil be purified completely or to a certain extent so as not to give
off an unpleasant odor in the oral cavity due to other components.
The cariogenic bacteria growth inhibitor of this invention is specifically effective to Streptococcus
mutans and its effect of inhibiting the growth of bacteria is not affected by a surfactant. l-.alpha.Cadinol is highly safe because it is a component contained in the natural vegetable essential oil. In
addition, it tastes only a little and gives no unpleasant feeling when put in the mouth.
This invention is now described by reference to the following examples but is not limited thereto.
Unless otherwise indicated, all percents, parts, ratios and the like are by weight.
EXAMPLE 1
2.0 g of l-.alpha.-cadinol was dissolved in 98 g of official ethyl alcohol with stirring at room
temperature to give 100 g of a solution.
This solution was added to the heart infusion agar medium. Streptococcus mutans RIMD 3125001
(designated as A in Table) was transplanted by stabbing to this medium. Incubation was performed
at 37 DEG C. for 72 hours. No growth was observed in the medium containing the solution at a
concentration of 1/1,000 (or 1/50,000 calculated as l-.alpha.-cadinol). Growth was barely observed in
the medium containing the solution at a concentration of 1/1,600 (or 1/80,000 calculated as l-.alpha.cadinol).
Then, Bacteroides microfusus IPCR 1009 (designated as B in Table 1) and Escherichia coli ATCC
10789 (designated as C in Table 1) were transplanted to the abovementioned medium. Incubation
was performed under the aerobic condition at 37 DEG C. for 72 hours. Their growth was inhibited at
a concentration of 1/2,000 as l-.alpha.-cadinol.
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Bifidobacterium adolescentis ATCC 15705 (designated as D in Table 1) was transplanted to the
same medium as mentioned above, and incubation was performed under the anaerobic condition at
37 DEG C. for 72 hours. The growth was inhibited at a concentration of 1/7,500 as l-.alpha.-cadinol.
The same test as above was performed under the aerobic condition for Pseudomonas aeruginosa (E),
Bacillus subtilis (F), Staphylococuss aureus (G), Apergillus nigar (H), Candida alibicans (I), and
Klebiella pneumoniae (J). The results obtained are shown in Table 1 below.
TABLE 1
______________________________________
Concentration for
Designation growth inhibition
of bacteria (as l-.alpha.-cadinol)
______________________________________
A
1/50,000
B
1/2,000
C
1/2,000
D
1/7,500
E
1/500
F
1/5,000
G
1/5,000
H
1/1,000
I
1/2,000
J
1/1,000
______________________________________
EXAMPLE 2
2.0 g of l-.alpha.-cadinol was dissolved in 6 ml of official ethyl alcohol, and glycerine was then added
thereto to give 100 g of a solution.
This solution was added to two kinds of heart infusion agar media, one containing 1.0 g of sodium
laurylsulfonate and the other, 1.0% of "Span 20". Streptococcus mutans RIMD 3125001 was
transplanted to the media. Incubation was performed at 37 DEG C. for 72 hours. The concentration
for growth inhibition was 1/1,000 (or 1/50,000 calculated as l-.alpha.-cadinol) in both cases. This
indicates that the effectiveness of the growth inhibitor is not affected by the surfactant used.
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EXAMPLE 3
Creeping pine leave oil was purified by column chromatography so that the concentration of l.alpha.-cadinol was increased to 75%. 10 g of this purified essential oil was mixed with 1 g of "Span
20" and 1 g of "Span 40". To the resulting mixture was added 150 ml of water and 50 g of dextrin,
followed by homogenization. The mixture was spray-dried to give 53 g of a powder containing 14.2%
of l-.alpha.-cadinol.
The antibacterial action of this powder on Streptococcus mutans RIMD 3125001 was investigated
using the heart infusion agar medium. The concentration for growth inhibition was 1/7,000 as powder,
which is equivalent to 1/50,000 as l-.alpha.-cadinol.
While the invention has been described in detail and with reference to specific embodiments thereof,
it will be apparent to one skilled in the art that various changes and modifications can be made
therein without departing from the spirit and scope thereof.
Claims:
What is claimed is:
1. A composition for inhibiting growth of Streptococcus mutans, comprising an antibacterially
effective amount of l-.alpha.-cadinol and a pharmaceutically acceptable carrier.
2. A composition as claimed in claim 1, wherein l-.alpha.-cadinol is present in a concentration of at
least 1/50,000 parts by weight.
3. A composition as claimed in claim 1, wherein said pharmaceutically acceptable carrier is an
organic solvent.
4. A composition is claimed in claim 3, wherein said organic solvent is selected from the group
consisting of ethanol, propylene glycol and glycerine.
5. A composition as claimed in claim 1, wherein emulsification of l-.alpha.-cadinol is accomplished
with a surfactant.
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6. A composition as claimed in claim 1, wherein said pharmaceutically acceptable carrier is chewing
gum, candy, troche and wheat gluten
7. A composition as claimed in claim 1, wherein said pharmaceutically active carrier is toothpaste or
mouthwash.
8. A composition as claimed in claim 1, wherein said pharmaceutically active carrier is tooth powder.
9. A composition as claimed in claim 1, containing l-.alpha.-cadinol in an amount sufficient to inhibit
growth of Streptococcus mutans RIMD 3125001.
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47. EP0190202 - 30.01.1986
SOLID ESSENTIAL OIL FLAVOR COMPOSITION AND METHOD OF MANUFACTURE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP0190202
Inventor(s):
MUTKA JERRY R (US); MILLER DENNIS H (US)
Applicant(s):
SUNKIST GROWERS INC (US)
IP Class 4 Digits: A23L
IP Class:
A23L1/222
E Class: A23L1/22B2
Application Number:
WO1985US01319 (19850712)
Priority Number: US19840631302 (19840716)
Family: WO8600502
Equivalent:
AU4635285; JP61502656
Cited Document(s):
US2809895; US2856291; US2857281; US2899313; US2919989;
US2929722; US2929723; US3041180; US3704137; US4271202
Abstract:
A SOLID ESSENTIAL OIL FLAVOR COMPOSITION HAVING A HIGH ESSENTIAL OIL CONTENT AND
A PROCESS FOR PREPARING THE PRODUCT, THE PROCESS INVOLVING PREPARATION OF A
HEATED OR COOKED AQUEOUS MIXTURE OF A SUGAR AND STARCH HYDROLYSATE
TOGETHER WITH AN EMULSIFIER. A SELECTED ESSENTIAL OIL OR OTHER OIL-SOLUBLE
FLAVOR IS COMBINED AND BLENDED WITH A MIXTURE IN A CLOSED VESSEL UNDER
CONTROLLED PRESSURE CONDITIONS TO FORM A HOMOGENEOUS MELT, THE MELT BEING
EXTRUDED INTO A RELATIVELY COOL SOLVENT, DRIED AND COMBINED WITH A SELECTED
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ANTICAKING AGENT TO PRODUCE THE STABLE, RELATIVELY NON-HYGROSCOPIC
PARTICULATE FLAVOR COMPOSITION OF THE INVENTION. THE SELECTED QUANTITY OF
ESSENTIAL OIL FLAVOR BLENDED INTO THE HOMOGENEOUS MELT BEING SUFFICIENT TO
YIELD ABOUT 12 TO 35% BY WEIGHT OF ESSENTIAL OIL IN THE ENCAPSULATED SOLID
PARTICULATE COMPOSITION. DURING THE PROCESS, ENCAPSULATION EFFICIENCY IS
MAINTAINED PREFERABLY AT OR ABOVE ABOUT 60%, MORE PREFERABLY ABOVE ABOUT 70%
AND MOST PREFERABLY ABOVE ABOUT 75 TO 80%. ALSO, THE COOK TEMPERATURE FOR THE
PROCESS IS PREFERABLY MAINTAINED AT OR BELOW A MAXIMUM OF ABOUT 126C.Description:
Description
Solid essential Oil Flavor Composition
and Method of Manufacture
Background of the Invention
The present invention relates to a process for producing a solid essential oil flavor composition and
the product of the process and more particularly to such a process resulting in a product in the form
of a stable, extruded, solid essential oil flavor composition.
This is a continuation-in-part of U. S.
Patent Application Serial No 631,302 filed July 16, 1984 by at least one inventor in common with the
present application, under assignment to the assignee of the present invention.
In order to preserve the aroma and flavor of various essential oils and make them available for use in
consumer products such as beverages and the like, the prior art has developed a number of
techniques for producing solid essential oil compositions. These compositions permit combination of
the essential oils into various products such as beverages to which it is desirable to impart the aroma
and flavor of the oil. Such techniques have been found to be particularly useful and desirable, for
example, in connection with essential oils of various citrus fruits while being equally useful with
essential oils from other sources. Citrus fruit, for example, are characterized by essential oils having
particularly desirable characteristics of aroma and flavor which are useful not only in beverage
products but in various food products as well.
The prior art in this regard is believed to be best exemplified by a number of
197/1651
U. S. patents which are hereinafter discussed in greater detail. These references include U. S.
Patents 2,809,895 and 3,041,180 issued respectively on October 15, 1975 and June 26, 1962 to H.
E. Swisher under assignment to the assignee of the present invention. The references also include U.
S. Patent 3,704,137 issued November 28, 1972. to Beck and U S Patent 4,271,202 issued
June 2, 1981 to Giel.
Turning now to these references, the earlier Swisher patent disclosed a process for forming solid
essential oil flavoring composition particles wherein an essential oil was emulsified in hot corn syrup
solids (42 DE) glycerine solution, cooled, ground, rinsed with a solvent and dried. The flavoring
composition retained the aroma and flavor of the oils within the particles while making them available
for release in various consumer products such as beverages and other food products.
The second Swisher patent disclosed an improved process and solid essential oil flavoring
composition wherein glycerine and corn syrup solids (42 DE) were formed in':o an aqueous,
semiplastic mass which was then combined with the essential oil by means of an emulsifier, the
resulting combination being extruded into a cold solvent to form an extruded solid wherein the
essential oil was encapsulated by the glycerine and corn syrup solids combination. This extruded
solid was then dried and an anti caking agent added, yielding an extruded particulate solid having
an extended shelf life while facilitating its combination with beverage or other food products to
release the aroma and/or flavor of the oil.
The Beck patent related to a similar process and product as summarized above for the second
Swisher patent, except that the process and product included a simple sugar and hydrolyzed cereal
solids (less than 20 DE) with pyrogenic silica as an anticing agent,
The Giel patent related to a spray-drying process for forming solid flavoring material capable of
including high percentages of flavoring oil per total particulate unit of weight. Because of the high oil
content possible, such spray-dried products found wide use in a number of beverages and other
foods. However, it was also found that spray-dried flavors typically exhibit a relatively limited shelf
life.In addition, the high temperatures necessarily involved during spray-drying processes have been
found to impair the flavor and aroma of various heat-sensitive oil flavors, such as those in citrus fruit.
Furthermore, solids formed by spray-drying commonly exhibit hygroscopic characteristics making
them difficult to handle and store.
198/1651
As noted above, spray-dried oil flavors have been used in the production of various beverages and
foods where it is desirable to take advantage of their high oil content. At the same time, extruded
essential oil solids of the type covered by the second Swisher and Beck patents have also found a
substantial market, particularly where it is desirable to take advantage of the better preserved aroma
and flavor of the oil.
However, as was noted in the Beck patent, the process for forming such extruded essential oil flavor
compositions has heretofore been considered to have a practical maximum essential oil content of
about 12% in the extruded particles. This limitation has at times prevented or limited the use of
extruded flavor compositions in certain products where high oil. content is desirable.
A number of patents issued to T. H.
Schultz, either alone or with other inventors, including U. S. 2,856,291; 2,857,281; U. S.
2,899,313; U. S. 2,919,989; U. S. 2,929,722 and
U. S. 2,929,723. Certain of these patents related to processes for encapsulating essential oils in
generally the same manner as the Beck patent noted above. In Schultz et al U. S. 2,857,281,
reference was made generally to use of an essential oil or flavoring agent "to furnish about from 5 to
25% thereof in the emulsion." However, in the specific discloses and examples provided in the
Schultz et al patent as well as in the other patents where Schultz was an inventor, resulting oil
percentages in encapsulated form were far below the practical limit of 12% noted above and initially
stated in the Beck patent.
Accordingly, there remains a need for a process making possible the formation of stable, extruded,
solid essential oil or flavor compositions having a relatively high percentage of essential oil
encapsulated therein, preferably at least in excess of the practical limit of 12% as stated in the Beck
patent.
Summary of the Invention
It is therefore an object of the invention to provide an improved process for forming an extruded,
solid, essential oil flavor composition and a product of such process while overcoming one or more
problems of the type summarized above.
199/1651
It is a further object of the invention to provide such a process for producing a resulting product
characterized by a relatively high essential oil or oil-soluble flavor contact completely encapsulated
within the extruded particulate solids.
It is an even further object of the invention to provide such a process for producing a resulting
product characterized by a relatively high essential oil or oil-soluble flavor contact completely
encapsulated within the extruded particulate solids.
It is an even further object of the invention to provide such a process for forming a resulting product
in the form of a stable, melt-based and extruded, solid essential oil flavor composition characterized
by about 12 to 35% by weight of essential oil in substantially completely encapsulated form within the
extruded solids. A somewhat higher percentage of the essential oil or oil-soluble flavor is initially
added in the process to accommodate oil losses, for example, during emulsification and solvent
washing of the product.
It is a related object of the invention to provide such a process for forming a resulting product in the
form of a stable, melt-based and extruded, solid essential oil flavor composition wherein a selected
quantity of essential oil is combined and blended with an aqueous mixture of a sugar, starch
hydrolysate and selected emulsifier and at least preferably about 60% by weight, more preferably
70% by weight and most preferably about 75 to 80% by weight of the selected quantity of essential
oil is present in encapsulated form within the resulting particulate essential oil composition.
Although, as noted above, the solid essential oil flavor composition of the invention is preferably
characterized generally by about 12 to 35% by weight of essential oil in substantially completely
encapsulated form, the present invention more preferably contemplates the solid essential oil flavor
composition as being characterized by about 14 to 30% by weight of essential oil in substantially
completely encapsulated form within the extruded solids.
In accordance with the present invention, it has been found that such a process and product are
possible by first forming an aqueous mixture of a sugar and starch hydrolysate in combination with a
suitable emulsifier, the aqueous mixture and emulsifier is combined and blended with a selected
quantity of an essential oil or oil-soluble flavor in a closed vessel to form a homogeneous melt under
controlled pressure conditions substantially greater than atmospheric pressure.
200/1651
It is an even further object of the invention to provide such a process and product of the process
wherein the blending step is carried out in a closed vessel pressurized within the range of from about
7 to 50 pounds per square inch (psi) or more.
It is yet a further related object of the invention to cook the aqueous mixture of the sugar and starch
hydrolysate preferably to a maximum temperature of about 1260 C before the aqueous mixture and a
selected emulsifier are combined and blended with the essential oil in a closed vessel as described
above. More preferably, the aqueous mixture is heated to a maximum temperature of about 124" C
and most preferably to a temperature in the range of about 122 to 1240 C generally under
atmospheric pressure conditions. These temperatures are especially applicable where the essential
oil comprises at least about 28% by weight of the combination just prior to emulsification.
A still further related object of the invention is to carry out the heating step whereby the resulting
particulate essential oil composition has a relatively higher water content, preferably at least about
5% by weight.
In connection with the present invention, the term "sugar" is intended to include simple sugars such
as sucrose, lactose, levulose, dextrose, fructose and maltose, as well as polyols such as glycerin
and even other sweetners having generally similar characteristics. Similarly, the term "starch
hydrolysate" is intended to include all hydrolyzed starches, both hydrolyzed cereal solids of about 20
DE or less and corn syrup solids of about 20 DE or higher. The term "emulsifier" is used herein to
indicate any emulsifier which is satisfactory for use particularly in combination with the selected
flavoring oil. Specific examples of suitable emulsifiers are set forth within the following detailed
description.In addition, the term "essential oil" is intended to include other oil soluble flavors which
are capable of incorporation in the process and product of the present invention
Additional objects and advantages of the invention are made apparent in the following description
having reference to the accompanying drawings.
Brief Description of the Drawings
FIGURE 1 is a block-type flow sheet including steps of the process of the present invention and for
forming the product of that process.
FIGURE 2 is a graphic representation of the effect of increased pressure on encapsulation of the
essential oil flavoring within the product of the process.
201/1651
Description of the Preferred Embodiments
As noted above, the present invention relates to a process for forming or preparing a stable, meltbased and extruded solid essential oil flavor composition in particulate form as well as the product of
the process. Generally, the process comprises the steps of (1) heating to a suitable cook
temperature an aqueous mixture of a sugar and a starch hydrolysate together with a selected
emulsifier, the cook temperature being approximately the boiling point of the aqueous mixture, (2)
blending a selected quantity of an essential oil flavor with the aqueous mixture to form a
homogeneous melt, (3) extruding the homogeneous melt into a relatively cool liquid solvent to form
extruded solids of selected size and shape, and (4) drying the particles and blending with a selected
anti caking agent to produce a stable and relatively non-hygroscopic composition in particulate form.
The process is improved by the present invention in that the step of blending or emulsifying the
essential oil with the aqueous mixture is carried out in a closed vessel and the quantity of essential oil
flavor added to the homogeneous melt is preferably selected to provide about 12 to 35% by weight
and more preferably about 14 to 30% by weight of essential oil flavor in completely encapsulated
form within the particulate oil composition.
The present invention further contemplates a process and product of the process wherein preferably
at least about 60% by weight, more preferably at least about 70% by weight and most preferably at
least about 75 to 80% by weight of a selected quantity of essential oil combined and blended with
the aqueous mixture is present in enca-psulated form within the resulting particulate essential oil
composition.
The invention also contemplates that the sugar and starch hydrolysate, either together with or prior
to combination of the selected emulsifier therein, is preferably heated to a maximum temperature of
about 1260 C in order to minimize flavor deterioration of the essential oil flavor and also to facilitate
encapsulation according to the present invention. More preferably, the heating temperature is limited
to a maximum of about 1240 C and most preferably, the aqueous mixture is heated to a temperature
in the range of about 122 to 1240 C generally under atmospheric pressure conditions. These
reduced temperatures are of greatest value when the essential oil comprises at least about 28% by
weight of the combination.
These temperature limits are discussed in connection with the present invention in greater detail
below. In addition to minimizing deterioration of flavor and other undesirable characteristics of'the
essential oil which commonly result at higher temperatures, the reduced cook temperature is also
believed to permit a relatively increased amount of water to remain in the melt prior to extrusion. It is
202/1651
theorized that this additional water assists in stabilizing and facilitating emulsification' and
encapsulation of the higher quantities of essential oil within the particulate solid in accordance with
the process of the present invention. Preferably, the invention contemplates that the solid resulting
from the process of the present invention comprise at least about 5% by water.
At the same time, the above temperature conditions for the heating step are preferably stated as
maximums at least within the broad and preferred ranges since a number of variations in the process
may be carried out for accomplishing similar results under even further reduced temperatures. For
example, it has been found that a lower cook temperature may be used where a lower
DE rated sugar or sweetener is employed. For example, if a 10 DE sweetener were employed in
place of the 20 DE sweetener described below in connection with a number of examples, it would be
possible to further reduce the cook temperature in accordance with the present invention.
Similarly, it. would also be possible to reduce the cook temperature while otherwise achieving the
objects of the present invention by either employing a greater degree of agitation during the cooking
process in order to facilitate removal of excess water therefrom or by carrying out the cooking
process under vacuum conditions for the same purpose.
The second Swisher patent, and the Beck patent referred to above discussed in substantial detail
the manner in which a homogeneous melt can be formed from an aqueous mixture of a sugar and
starch hydrolysate together with a separate flavor component to form an extruded solid capable of
being dried in the manner summarized above. Those references also discussed the manner in
which such a homogeneous melt can be extruded into a cool liquid solvent to form particle of
selected shape and size as well as the selection of a suitable anti caking agent for combination with
the extruded solid particles in order to maintain them in a more stable condition. Accordingly, those
references are incorporated herein as though set forth in full with respect to the particular features
referred to above.
Referring now to the drawings and particularly to FIGURE 1, a selected sugar and starch
hydrolysate are mixed together as indicated at 12. The mixture is then agitated in order to uniformly
mix together the sugar and starch hydrolysate. As noted above, the sugar may be any of the simple
sugars such as sucrose, levulose, dextrose, fructose or maltose, as well as a polyol such as
glycerine or other similar sweeteners.
203/1651
Any preferred sugar or sweetner may be used for any of a variety of reasons, such as to achieve
improved flavor of the resulting product and/or to reduce hygroscopcity of the product. The mixture
12 is then heated to a cook temperature preferably approximating its boiling point as indicated at 14.
A suitable cook temperature for such mixtures including most sugars extends across a range of
approximately 110 to 130 C. For example, with the sugar being sucrose and the starch hydrolysate
being 20 DE corn syrup, the boiling point of the mixture is approximately 125-130 C and the mixture
is preferably heated to a temperature within that range.
An emulsifying agent is preferably added to the aqueous mixture 12 after the heating step. Within
FIGURE 1, addition of the emulsifying agent is indicated at 16. The emulsifier is selected to facilitate
emulsification or dispersion of essential oil described below into the mixture 14. Selection of the
particular emulsifier and the quantity of the emulsifier added to the aqueous mixture 14 is one of the
important features of the present invention permitting from 12 to 35% of a selected essential oil to be
encapsulated within the final extruded product. Suitable emulsifiers for use within the present
invention include sulfoacetate of monoand diglycerides as well as polyglycerol esters and
lecithin.Polyglycerol esters suitable for use within the present invention are available, for example,
under the trademark identification DREWPOL 6-2-S available from California Fats & BR<
Oils, Richmond, California. Generally, the polyglycerol esters have been found satisfactory within the
present invention for the lower end of the specified range.
One preferred emulsifier for emulsifying and encapsulating up to 35% essential oil within the final
extruded product is a sulfoacetate of mono- and diglycerides containing 1% by weight water and
available under the trademark identification EMARGOL KL available from the Witco Company.
Emulsifiers such as those referred to above are added to the molten mixture 14 in the amount of
approximately 0.5 to 5% by weight of the aqueous mixture. However, it is to be noted that the amount
of emulsifier used in such an application can vary depending upon other factors. Accordingly, the
above noted range is set forth only as a general indication in connection with the present invention.
Another emulsifier which has been found to be particularly satisfactory in terms of the present
invention but possibly less preferred than the EMARGOL KL product referred to above is lecithin,
available for example from Ross & Rowe under the trademark YELKIN TS.
Examples employing both of the emulsifiers noted above are set forth below.
204/1651
An essential oil or other oil-soluble flavor contemplated for combination with the mixture 14 and
emulsifier 16 is generally indicated at 18 and may be an essential oil, for example1 of a citrus fruit
contemplated for use in beverage or other food products.
The addition of a small amount of an oil-soluble heat-stable antioxidant (indicated at 20 in FIGURE 1)
such as 4-methyl-2, 6-ditertiary butyl phenol or butylated hydroxyanisole is optional. Generally, from
about 0.05 to about 0.5% by weight of the antioxidant, based on the weight of the essential oil, is
sufficient.
The essential oil 18, alone or in combination with the antioxidant 20, is then added to the aqueous
mixture 14 and emulsifier 16 in a vessel 22. In accordance with the present invention, it is particularly
important that the vessel 22 be closed during blending of the essential oil 18 with the cooked
aqueous mixture 14 and emulsifier 16. It has been found that the carrying out of this blending or
emulsification step in a closed vessel is essential to insure uniform and consistent encapsulation of
relatively large quantities of essential oil within the solid product.
The closed vessel 22 is charged with gas, preferably an inert gas such as nitrogen or carbon
dioxide, for example, to maximize encapsulation of the oil or flavor. Even more preferably, the vessel
22 is pressurized after addition of the inert gas to a pressure from about 7 to 50 psi. In FIGURE 1,
addition of the inert gas is generally indicated at 24. Pressurization and its effects within the closed
vessel 22 are described in greater detail below with further reference to the graph of FIGURE 2.
Referring to FIGURE 2, encapsulation of substantially increased quantities of essential oils or other
oil-soluble flavors is illustrated as being possible with pressurization in the vessel 22 generally from
about 7 to about 100 psi.
Destabilization of the resulting product sometimes occurs with higher pressures at or above
approximately 100 psi. Best results are obtained with the closed vessel 22 if pressure is maintained
within the approximate range of 7-50 psi.
In this regard, a pressure of about 7 psi is developed from vapor pressure alone resulting from
combination of the essential oil 18 with the molten mixture 14 and emulsifier 16 within the closed
vessel. In such an event, the vessel 22 is initially charged either with air or an inert gas at
atmospheric pressure.
205/1651
Referring to FIGURE 2, the upper limit of 50 psi for pressurization of the vessel 22 is not a precise
limit. In some applications, it is possible to pressurize the vessel substantially above 50 psi and even
above 100 psi without causing destabilization. However, since the amount of essential oil capable of
encapsulation within the final extruded product tends to diminish when pressure is increased above
50 psi, that pressure has been selected as the generally preferred upper limit for pressurization of
the vessel 22.
Mixing of the essential oil 18, aqueous mixture 14 and emulsifier 16 in the closed vessel 22 under
pressure is continued until those components are uniformly mixed and emulsified to result in a
homogeneous melt of the type also discussed in the Beck and Swisher references, for example.
Generally, the homogeneous melt is defined as having a plastic condition suitable for forming a solid
product in the manner defined below with an amphorous character for achieving high stability over
an extended period of time.
The homogeneous melt from the vessel 22 is then extruded under pressure, using either gas or
mechanical pressure, for example, into a cold organic solvent such as isopropanol to form the melt
into extruded filaments.
Extrusion is carried out in an extruder 26 having die openings of a size selected in accordance with
the size and shape desired for the resulting particles. For example, where small particles are desired
for use in beverage or food products, the homogeneous melt from the vessel 22 is extruded through
openings (not shown) having diameters, for example, of about 1/32 inch.
Extruded filaments of the homogeneous melt pass from the extruder 26 into a cold cold organic
solvent, such as isopropanol at about -200 C, as generally indicated at 28. The function of the
isopropanol or other solvent is two-fold. Initially, it acts as a coolant to rapidly solidify the extruded
shapes of homogeneous melt. Secondly, it removes any essential oil on the surface of the extruded
solids which would otherwise be susceptible to oxidation.
The extruded filaments are preferably broken up into small rod-like particles while within the solvent
28 in order to permit removal of any essential oil exposed on the smaller or separated particles. For
example, the filaments can be divided by impact action of an agitator impeller (not shown) to
produce a desired particle size and shape.
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Following the solvent washing step 28, the particles from the extruded filaments are then screened
or centrifuged at 30 to remove the organic solvent. The solvent is transferred to a holding tank 32 and
may be returned to the washing step 28 if desired.
The particles from the separation step 30 are dried in a vacuum oven 33 and blended with a suitable
anticaking agent 36. The particles are then screened by passage over a succession of sizing
screens (not shown) and packaged, preferably in a dehumidified room, as indicated at 34.
The anticaking agent, as generally indicated at 36, is added to the particles after drying to facilitate
their further handling and to prevent the particles from sticking together. The anticaking agent is
preferably silica, introduced either before or after the particles are treated in the oven 33.
The process described above may be used for preparing extruded solids containing essential oils
from various sources. In particular, the process of the invention is contemplated for use in
conjunction with various citrus fruits such as oranges, grapefruit, lemons, etc. However, it will be
apparent that the process of the invention is also useful with other essential oil or oil-soluble flavors,
either for use in beverages or food products.
The product of the process described above is novelly characterized as a stable, melt-based and
extruded, solid essential oil composition in particulate form. The particles are of a solid amorphous
character with a shape determined by the extruder 26 and further divided, for example, by impact
breaking at 28. The particles consist of a sugar and starch hydrolysate as defined above, a selected
emulsifier and a selected essential oil flavor.
The essential oil flavor preferably forms about 12 to 35%, more preferably about 15 to 30%, by
weight of the particles while being present therein completely encapsulated form.
The preceding process is particularly adapted for assuring reproducible production of particles
having a high oil content as defined above. The process is also particularly adapted for forming
about 12 to 35% by weight of the particles with the essential oil flavor being present therein in
completely encapsulated form.
The following examples of various embodiments of the invention are presented to further illustrate
and exemplify but not to limit the scope of the invention.
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Example 1
6025 grams of 20 DE corn syrup (708 solids), 4125 grams sugar and 200 grams EMARGOL KL
were mixed in a steam jacketed stainless steel vessel. The vessel was fitted with a thermometer and
an agitator-assembly produced by C. E. Howard
Company, os Angeles, California and having a flat bladed turbine type agitator about 4 1/2 inches in
diameter. After heating to 1300 during an initial cook, 2200 grams of cold-pressed orange oil were
added to the vessel. The vessel was immediately closed. After 5 minutes mixing with the agitator, the
pressure inside the vessel had increased to 7 psi. During mixing, the cold-pressed orange oil
lowered the temperature of the aqueous mixture below its cooking temperature, for example, to
about 1250 C.After mixing was complete, nitrogen was added to pressurize the vessel to 30 psi and
the melt was extruded through a plate with 0.030 inch diameter holes into 19 liters of cold (-20 C)
isopropanol to solidify the filaments.
After impact breaking of the filaments, the excess isopropanol was removed on a vacuum screen
and the material was dried for 3 hours in a vacuum oven (500 C, 27 in. Hg vacuum). After addition of
2% silica as an anticaking agent, the product contained 16.7% by weight flavor.
Example 2
6025 grams of 20 DE corn syrup (70% solids), 4125 grams sugar and 200 grams EMARGOL KL
were mixed in a steam jacketed stainless steel vessel. The vessel was fitted with an agitator and
thermometer as in Example 1. After heating to 1300 C in an initial cook, 2200 grams of cold-pressed
orange oil were added to the vessel.
The vessel was immediately closed and pressurized to 50 psi with nitrogen. After 5 minutes mixing
and agitation, the melt was extruded through a plate with 0.030 inch diameter holes into 19 liters of
cold (-200 C) isopropanol to solidify the filaments. The excess isopropanol was removed on a
vacuum screen and the material was dried for 3 hours in a vacuum over (50" C, 27 in Hg.
vacuum). After blending in 2% silica, the product contained 20.7% by weight flavor.
ExamDle 3
6025 grams of 20 DE corn syrup (70% solids), 4125 grams sugar and 450 grams EMARGOL KL
were mixed in a steam jacketed stainless steel vessel. The vessel was fitted with an agitator and
thermometer again as in Example 1. After heating to 1300 C in an initial cook, 2500 grams of coldpressed orange oil were added to the vessel. The vessel was immediately closed and pressurized to
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50 psi with nitrogen. The melt was then extruded through a plate with 0.030 inch diameter holes into
19 Liters of cold (-20 C) isopropanol to solidify the filaments The excess isopropanol was removed
on a vacuum screen and the material was dried for 3 hours in a vacuum oven (50 C, 27 in. Hg.
vacuum). After blending in 28 silica, the product contained 19.88 by weight flavor.
Example 4
The steps of Example 3 were repeated except that the vessel was pressurized to 100 psi with
nitrogen. Upon extrusion of the resulting product, the solids were found to be destabilized as
indicated at 38 in FIGURE 2. Thus, Example 4 represents instability of the resulting product upon
pressurization to about 100 psi.
The steps of Examples 1-3 are also capable of reproduction with other essential oils, for example,
from citrus fruit other than oranges or other oil-soluble flavors.
In addiction, the steps of Example 1 were repeated with a number of other combinations of essential
oil and emulsifier as typified below in Table I. Table I summarizes Examples 1-4 and illustrates
additional Examples 5-8 carried out with the same steps and amounts described above for Example
1 except where different amounts of various components are indicated in Table I. As noted above,
about 7 psi pressure was developed within the vessel 22 for each of these examples by vapor
pressure of the components being mixed therein. At the same time, the temperature in the vessel
was reduced from the initial cook temperature primarily by addition of the essential oil to the cooked
aqueous mixture.
TABLE I
Examples 1 2 3 4 5 6 7 8
Component
Weight EMARGOL KL (grams) 200 200 450 450 450 240 200 200
Weight Flavor Initially Added (grams) 2,200 2,200 2,500 2,500 2,500 4,200 2,500 2,350
Initial Emulsifier Content (%) 1.82 1.82 3.90 3.90 3.90 1.87 1.78 1.72
Initial Flavor Content (%) 20.1 20.1 21.7 21.7 21.7 32.8 22.2 20.
Pressure Developed During Mixing (psi) 7 50 50 100 7 7 7 7
Encapsulated Flavor (%) 16.7 20.7 19.8 unstable 17.1 27.6 18.4 19 Cold-pressed orange oil Coldpressed lemon oil Cold-pressed tangerine oil
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Note : Each of the examples of Table I resulted in encapsulation efficiency, as defined above, at least
equal to the msot preferred level of about 75 to 80% in accordance with the present invention.
The information set forth in Table I is summarized as follows. Initially, for Examples 5-8, the
processing steps described in connection with Example 1 were again followed including the identity
and weight of sugar and starch hydrolysate. The amount of EMARGOL KL and flavor or essential oil
is set forth in Table I for each of the examples. Also, the identity of the flavor or essential oil for each
of the examples is indicated in the footnotes to Table I.
Thereafter, the initial emulsifier content and flavor or essential oil content are set forth as percentages.
These values were calculated based on the total weight of the product prior to extrusion. Accordingly,
the percentages are based on a total weight of the sugar, starch hydrolysate, emulsifier and flavor
assuming loss of all but about 5% of the water from the corn syrup or starch hydrolysate.
Encapsulation efficiency, referred to in the note following
Table I, was determined directly from the values for initial flavor content and encapsulated flavor. For
example, encapsulation efficiency for
Example 1 was determined by dividing 16.7 by 20.1 and multiplying by 100 to result in encapsulation
efficiency of about 83.1%.
Information set forth below for additional examples was determined in the same manner described
immediately above. It is again noted that, for each of the examples, all but about 5% by weight of the
water from the starch hydrolysate was removed during the initial cooking step.
Abbreviated data for Examples 9-13 is set forth in Table II to demonstrate the effect of cook
temperature on encapsulation efficiency. The examples set forth in Table II were carried out in the
same pilot plant reactor used for each of
Examples 1-8. At the same time, each of Examples 9-13 was carried out according to the specific
steps set forth in connection with Example 6. The only variation for Examples 9-13 was the heating or
cooking temperature to which the aqueous mix was heated during the initial cook.
VIABLE II
Encapsulation Efficiency vs. Cook Temperature
Oil Encapsulation Cook Example No. Encapsulated Efficiency Temperature, C
9 20.5 63.5 118
10 22.9 70.9 122
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11 21.1 65.3 126
12 19.3 59.8 130
13 19.2 59.4 134
Note: In each of Examples 9-13, 6025 grams of 20 DE corn syrup (70% solids), 4125 grams sugar
and 240 grams
EMARGOL KL were mixed in a steam jacketed stainless steel vessel fitted with an agitator and
thermometer as described for preceding examples. The mixture was then heated to a cook
temperature as set forth above in Table II.Thereafter, 4200 grams of cold-pressed orange oil was
added, the vessel immediately closed and agitation commenced. A pressure of about 7 psi
developed after about five minutes of agitation. The resulting rrelt was then extruded through a plate
with 0.030 inch openings into 19 liters of cold (-20 C) isopropanol. The solidified filaments were
impact broken as described above, excess isopropanol removed by vacuum, the material dried and
blended with 2% by weight silica. Resulting encapsulating efficiency for examples 9-13 is set forth in
Table II.
The data of Table II is set forth independently of the rest of the examples 9-13 were all run at about
the same time with the same lots or batches of emulsifier, essential oil, etc.
Accordingly, Table II is believed to very clearly demonstrate a trend according to the present
invention in terms of encapsulation efficiency as determined by the cook temperature.
At the same time, Examples 9-13 represent a relatively limited number of temperatures in the range
between 1180 C and 1350 C. Table III sets forth a larger number of examples run in a similar manner
as the examples of Table II but at different times and possibly with different lots of emulsifier,
essential oil, etc. Although the examples of Table III were run in different equipment from those Table
II, they are believed sufficiently similar so that Tables
II and III taken together tend to establish the same trend, referred to above in connection with
Table II alone, as to the effect of cook temperature on encapsulation efficiency according to the
invention.
Table III, below, sets forth Examples 14-39 which were also carried out in a similar manner as
described above for Examples 9-13 of
Table II. The examples of Table III were run in a large scale plant reactor rather than the pilot plant
reactor used in Table II. However, results in Tables II and III are believed to be clearly capable of
correlation to further demonstrate consistency for the process of the present invention.
211/1651
TABLE III
%
Emulsifier % Cook % %
Added Orange Oil Temperature Oil Encapsulation
Example No. (EMARGOL KL) Added C Encapsulated Efficiency 14 2.03 26.6 130 19.0 71.6 15 2.06
28.3 128 21.9 77.2 16 2.06 28.3 130 19.9 70.2 17 1.97 28.35 124 22.6 79.7 18 1.97 28.35 124 22.2
78.3 19 2.06 28.35 124 21.4 75.5 20 2.06 28.35 125 22.3 78.6 21 2.84 28.4 132 14.7 51.8 22 1.97
28.8 130 20.7 71.9 23 1.91 29.3 131 20.5 70.0 24 2.09 29.8 130 20.1 67.4 25 2.09 29.8 132 20.1 67.4
26 2.01 30.2 130 15.2 50.4 27 2.03 30.2 132 16.2 53.7 TABLE III (CONT.)
%
Emulsifier % Cook % %
Added Orange Oil Temperature Oil Encapsulation
Example No. (EMARGOL KL) Added C Encapsulated Efficiency 28 2.03 31.9 124 25.9 80.9 29 1.96
31.9 124 24.0 75.2 30 1.96 31.9 124 25.8 81.0 31 1.96 31.9 124 26.1 81.9 32 2.03 31.9 121.7 25.4
79.7 33 2.03 31.9 121.7 25.9 81.2 34 1.96 31.9 125 25.0 78.4 35 2.03 31.9 126 25.1 78.7 36 1.96
31.9 126 25.6 80.4 37 1.96 31.9 126 26.5 83.2 38 1.86 32.9 131 14.7 44.7 39 2.41 32.5 134 12.8 39.4
It may also be seen in connection with
Table III that unacceptable encapsulation efficiency resulted particularly in connection with Examples
26, 27, 38 and 39. Each of these examples included a generally high cook temperature varying from
about 130 to about 134 C. In addition, those same examples included relatively high initial essential
oil contents ranging from about 30.2 to about 32.9% b weight.
Accordingly, Table III is believed to even further emphasize the importance of cook temperature in
accordance- with the present invention.
Table IV, below, sets forth yet an additional series of Examples 40-42, each carried out using lecithin
as an emulsifier.
TABLE IV
%
Emulsifier % Cook % %
Added Orange Oil Temperature Oil Encapsulation
Example No. (EMARGOL KL) Added C Encapsulation Efficiency 40 2.21 22.1 130 18.1 81.9 41 1.95
22.2 130 18.4 82.9 42 1.43 28.6 124 22.7 79.4
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Table IV illustrates the utility of the present invention including lecithin as an emulsifier. In each of
Examples 40-42 of Table
IV, lecithin available from Ross & Rowe under the tradename YELKIN TS was employed.
Table IV in particular demonstrates that lecithin was quite effective as an emulsifier where the
essential oil was initially present in an amount of about 22% by weight. With an initial essential oil
percentage of about 28, for example, it is particularly important to employ a lower cook temperature
of no more than about 1260 C and preferably no more than about 123 to 1240 C in order to achieve
effective encapsulation efficiency.
Further Discussion of Prior Art
In order to further illustrate advantages of the present invention, Table V sets forth Examples 43-51
only for the purpose of representing the prior art for purposes of comparison. Examples 43-51 were
conducted in essentially the same manner as Examples 9-13 of
Table II but with the vessel remaining open during mixing of the essential oil with the aqueous mix.
TABLE V (PRIOR ART) % % % %
Emulsifier Flavor Flavor Encapsulation
Example No. Added Added Encapsulated Efficiency 43 1.41 16.4 14.7 90 44 1.41 16.4 10.8 66 45
1.87 16.4 13.4 82 46 1.87 16.4 10.8 66 47 2.78 16.2 14.4 89 48 2.78 16.2 11.9 77 49 2.71 18.1 6.0 33
50 2.71 18.1 12.2 67 51 2.65 19.9 10.0 50
Examples 43-51 are believed, by contrast, to demonstrate further advantages of the present
invention.A cursory review of Table V indicates some high encapsulation efficiencies achieved even
with an open mixing vessel, in particular, Examples 43, 45 and 47. However, it is especially important
to note that the initial amount of essential oil employed in each of
Examples 43-51 was very low compared to that in
Examples 1-42.
Even with the advantage of lower initial oil content, encapsulation efficiency was not repeatable even
for the limited purpose of accomplishing uniform encapsulation with oil content in the range of about
12 to 15%. For example, note that whereas Example 43 resulted in encapsulation efficiency of 90%,
substantially identical Example 44 resulted only in encapsulation efficiency of 66% with an oil content
in encapsulated form of only 10.8%. The other examples of Table V demonstrate similar inconsistent
results and thus are believed to further assist in emphasizing the novel features of the present
invention.
213/1651
In view of the preceding description and Examples 1-42, other modifications of the process and
resulting product of the present invention, in addition to those noted above, will be apparent to those
skilled in the art.
Accordingly, the scope of the present invention is defined only by the following appended claims.
Claims:
WHAT IS CLAIMED IS:
1. In a process for preparing a stable1 melt-based, extruded, solid essential oil flavor composition in
a process where an aqueous mixture of a sugar, a starch hydrolysate and a selected emulsifier is
heated to about the melting point of the aqueous mixture, an essential oil flavor is combined and
blended with the aqueous mixture to form a homogeneous melt and the homogeneous melt is
extruded into a relatively cool solvent to form a solid extruded material which is dried and combined
with an anticaking agent to produce a resulting stable and relatively non-hygroscopic particulate
essential oil composition, the improvement comprising
carrying out the step of combining and blending of the essential oil flavor with the aqueous mixture
by agitating the essential oil flavor and aqueous mixture together in a closed vessel in order to form
the homogeneous melt under controlled pressure conditions greater than atmospheric pressure, and
selecting a quantity of the essential oil flavor for combination and blending with the aqueous mixture,
the selected quantity of essential oil flavor being sufficient to provide about 12 to 35% by weight of
the essential oil flavor in encapsulated form within the particulate essential oil composition.
2. The improved process of Claim 1 further comprising the step of developing a pressure in the
range of about 7 to 50 psi in the closed vessel during the step of combining and blending the
essential oil flavor with the aqueous mixture by agitation in the closed vessel.
3. The improved process of Claim 2 wherein the emulsifier is selected from the class consisting of
sulfoacetates of mono- and diglycerides, polyglycerol esters and lecithin.
214/1651
4. The improved process of Claim 1 wherein at least about 60% by weight of the selected quantity of
essential oil combined and blended with the aqueous mixture is present in encapsulated form within
the resulting particulate essential oil composition.
5. The improved process of Claim 4 wherein at least about 70% by weight of the selected quantity of
essential oil combined and blended with the aqueous mixture is present in encapsulated form within
the resulting particulate essential oil composition.
6. The improved process of Claim 5 wherein at least about 75 to 80% by weight of the selected
quantity of essential oil combined and blended with the aqueous mixture is present in encapsulated
form within the resulting particulate essential oil composition.
7. The improved process of Claim 1 wherein the step of heating the aqueous mixture of the sugar,
starch hydrolysate and selected emulsifier is limited to a maximum temperature of about 1260 C.
8. The improved process of Claim 7 wherein the step of heating the aqueous mixture of the sugar,
starch hydrolysate and selected emulsifier is limited to a maximum temperature of about 1240 C.
9. The improved process of Claim 7 wherein the step of heating the aqueous mixture of the sugar,
starch hydrolysate and selected emulsifier is carried out generally under atmospheric pressure
conditions and at a temperature in the range of about 122 to 1240 C.
10. The improved process of Claim 1 wherein the step of hearing the aqueous mixture of the sugar,
starch hydrolysate and selected emulsifier is carried out in a manner to limit water loss from the
mixture whereby the resulting particulate essential oil composition has relatively higher water content.
11. The improved process of Claim 10 wherein the resulting particulate essential oil composition
comprises at least about 5% by weight water.
12. The improved process of Claim 1 wherein the essential oil flavor is an oil of a citrus fruit.
13. A stable, melt-based and extruded solid essential oil composition in particulate form produced
by the process of Claim 1 and comprising solid amorphous particles of extruded shape, the particles
consisting of a sugar, starch hydrolysate, selected emulsifier, selected essential oil flavor and water,
215/1651
the essential oil flavor forming about 12 to 35% by weight of the particles in substantially completely
encapsulated form.
14. The extruded solid essential oil composition of Claim 13 wherein the emulsifier is.
selected from the class consisting of sulfoacetates of mono- and diglycerides, polyglycerol esters
and lecithin.
15. The extruded solid essential oil composition of Claim 13 wherein the essential oil flavor forms
about 14 to 30% by weight of the particles in substantially completely encapsulated form.
16. The extruded solid essential oil composition of Claim 15 wherein the solid amphorous particles
comprise at least about 5% by weight water.
17. The extruded solid essential oil composition of Claim 13 wherein the solid amphorous particles
comprise at least about 5% by weight water.
18. The extruded solid essential oil composition of Claim 13 wherein the essential oil flavor is an oil
of a citrus fruit.
216/1651
48. EP0596067 - 11.05.1994
ESSENTIAL OIL.
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP0596067
Inventor(s):
EHRET CHARLES (FR); PETRZILKA MARTIN (FR)
Applicant(s):
GIVAUDAN ROURE INT (CH)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
EP19930909979 (19930513)
Priority Number: EP19920108469 (19920520); WO1993EP01195 (19930513); EP19930909979
(19930513)
Family: EP0596067
217/1651
49. EP0717925 - 26.06.1996
PLANT EXTRACTS FROM HERBS E.G. ROSEMARY HAVE HIGH ANTIOXIDANT AND ESSENTIAL
OIL CONTENT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP0717925
Inventor(s):
AESCHBACH ROBERT (CH); MASSERET BERNARD (FR)
Applicant(s):
NESTLE SA (CH)
IP Class 4 Digits: A23L; A01H
IP Class:
A23L1/221; A01H1/04
E Class: A23L1/221E; A01H1/04
Application Number:
EP19950810790 (19951213)
Priority Number: FR19940015343 (19941220)
Family: EP0717925
Equivalent:
DE69509483; ES2103683; ES2132583; FR2728138; GR3030325; IL116449;
MA23748; TR960572
Cited Document(s):
EP0454097; FR2548523; FR2547981
Abstract:
HERBAL PLANT MATERIAL HAS A HIGH ANTIOXIDANT AND ESSENTIAL OIL CONTENT SUCH
THAT THE FRESH MATERIAL CONTAINS MORE THAN 1.5 WT% ANTIOXIDANTS AND MORE THAN
0.3 WT% ESSENTIAL OILS AND ITS DRIED FORM CONTAINS MORE THAN 3.5 WT%
ANTIOXIDANTS AND MORE THAN 1.5 WT% ESSENTIAL OILS. ALSO CLAIMED IS A PROCEDURE
FOR SELECTING PLANTS WITH A HIGH ANTIOXIDANT AND ESSENTIAL OIL CONTENT
COMPRISING: (I) CALIBRATION OF THE ANTIOXIDANT AND ESSENTIAL OIL CONTENT AGAINST
218/1651
A STATISTICALLY VIABLE POPULATION; (II) SCREENING PLANTS CONTG. ABOVE AVERAGE
CONTENTS; AND (III) MULTIPLYING THE NUMBER OF SELECTED PLANTS. ALSO CLAIMED IS A
RESIDUE WITH AN ANTIOXIDANT CONTENT OF GREATER THAN 3.5 % RESULTING FROM DISTN.
OF AQ. PLANT MATERIAL.Description:
La prйsente invention est relative а des nouveaux plants d'йpices, notamment de sauge ou de
romarin, prйsentant simultanйment un contenu йlevй en antioxydants et en huile essentielle, ainsi
qu'au procйdй de sйlection de ces plants et а leur utilisation comme matiиre premiиre, а la fois
pour l'obtention d'antioxydants а des fins notamment d'additifs alimentaires et йgalement comme
source d'huile essentielle pour la parfumerie.
La connaissance et l'emploi des йpices remontent aux pйriodes les plus anciennes de notre
civilisation ; non seulement pour leur utilisation en tant qu'aromates et de condiments ou pour leurs
propriйtйs mйdicamenteuses, mais aussi dans un rфle fonctionnel important pour la prйservation
des aliments ; cet effet est dы non seulement а un effet de masquage des odeurs rйsultant de la
dйtйrioration de l'aliment, mais surtout а une action protectrice antioxydante et tout
particuliиrement un effet bactйricide et bactйriostatique permettant de retarder la dйtйrioration
des aliments par les micro-organismes ; cet effet a йtй dйcrit par Pruthi (1980) (1) et Shelef (1983)
(2).
Les numйros entre parenthиse renvoient aux rйfйrences bibliographiques en fin de description.
La mise en йvidence des propriйtйs anti-oxygиne de certaines йpices remonte а une quarantaine
d'annйes, quand JR Chipault (1952, 1955, 1956) (3,4,5) entreprit l'йtude desdites йpicйs. Les
travaux de Chipault ont trouvй un regain d'intйrкt il y a une vingtaine d'annйes, lorsque des doutes,
confirmйs par la suite, furent йmis sur l'innocuitй du butyl-hydroxy-toluиne (BHT), antioxydant de
synthиse trиs performant et largement utilisй avec le butyl-hydroxy-anisole (BHA) pour la protection
des aliments. L'intйrкt pour le rфle antioxydant de certaines йpices s'est amplifiй depuis peu, avec
l'engouement des consommateurs occidentaux pour les produits alimentaires naturels, et plusieurs
olйorйsines d'йpices, notamment de romarin, sont proposйs actuellement sur le marchй pour
prйvenir l'oxydation des aliments.
219/1651
Parmi ces йpices et herbes aromatiques possйdant une activitй anti-oxygиne, la sauge et le
romarin sont parmi les plus prometteuses. Leur pouvoir antioxydant est dы а la prйsence dans ces
plantes de composйs tels que l'acide carnosique et l'acide rosmarinique, qui agissent en synergie
avec un ensemble de flavonoпdes suivant des mйcanismes complexes qui n'ont pas йtй
complиtement йlucidйs.
Au cours des quinze derniиres annйes, plusieurs types d'olйorйsines, de romarin ont йtй mis au
point, offerts sur le marchй et utilisйs par l'industrie alimentaire. Leur activitй antioxygиne dans les
matiиres grasses et les produits alimentaires a йtй dйmontrйe. Ces olйorйsines s'utilisent en
gйnйral а un dosage voisin de 500 ppm calculй sur la matiиre grasse des aliments, dosage
proche de celui des matiиres aromatisantes naturelles et employйes pour amйliorer l'appйtence
des produits alimentaires.
Diffйrents procйdйs ont йtй proposйs pour extraire l'olйorйsine des йpices et plus
particuliиrement, du romarin. L'extraction peut кtre rйalisйe en plusieurs йtapes en utilisant des
solvants polaires ou non, ainsi que leurs mйlanges : huile vйgйtale ou graisse animale (6), l'hexane,
le benzиne, l'йther йthylique, le chloroforme, le dichlorure d'йthylиne, le dioxane ou le mйthanol
(7,8), l'йthanol ou le benzиne (9), l'hexane ou l'йthanol (10, 11), le CO2 supercritique (12, 13, 14) ;
on peut citer йgalement les brevet EP 307 626 et la demande de brevet EP 507 064. L'ensemble de
l'йtat de la technique dйcrit dans ces demandes de brevet et dans les articles citйs ci-dessus est
incorporй ici par rйfйrence, en particulier pour ce qui est des procйdйs d'extraction des
antioxydants des plantes, procйdйs qui peuvent кtre йgalement appliquйs aux plants de
l'invention.
L'extraction s'accompagne souvent d'une dйsodorisation et/ou d'une dйcoloration de l'olйorйsine ;
certains traitements permettent de traiter l'olйorйsine pour йliminer les insolubles dans les corps
gras (brevet US 4.877.635, brevet EP 0.009.661 et rйfйrences 14, 15, 16).
Aeschbach (Brevets Europйens 0.307.626 et 0.507.064) a dйveloppй des procйdйs pour obtenir
des extraits antioxydants de romarin ou de sauge sous forme de poudre ou de liquide translucide.
Ces extraits sont riches en antioxydants, plus particuliиrement en acide carnosique et carnosol, les
deux antioxydants principaux du romarin et de la sauge. L'acide carnosique a йtй isolй et identifiй
par Aeschbach et Philippossian (Demande de Brevet Europйen EP 0.480.077). L'oxydation de
l'acide carnosique conduit au carnosol qui lui-mкme est douй de propriйtйs antioxydantes ; la
220/1651
prйsence d'un groupe isopropyle dans ces deux composйs jouent un rфle important dans la
stabilisation des radicaux formйs en cours d'oxydation.
Aeschbach (17) a mis en йvidence l'existence de 13 hйtйrosides dans le romarin, contribuant de
faзon mineure (synergisme), comme l'acide rosmarinique, а l'effet antioxydant.
Plusieurs travaux ont йtй publiйs sur l'effet antioxygиne des olйorйsines de romarin dans les
aliments (8, 14, 15). Dans les trois cas et bien que les olйorйsines utilisйes soient d'origine
diffйrente elles exercent dans les systиmes йtudiйs un effet protecteur voisin de celui apportй par
le BHT seul ou en mйlange avec le BHA et le gallate de propyle, ces derniers йtant utilisйs toutefois
а une dose plus faible. La qualitй des olйorйsines obtenues et plus prйcisйment leur effet
antioxygиne va dйpendre non seulement des paramиtres d'extraction (type de solvant,
tempйrature, durйe) mais йgalement de la qualitй du vйgйtal mis en oeuvre, de son origine, des
conditions climatiques, des conditions de culture et de rйcolte ainsi que l'indique l'йtude de
Granger (18) sur l'essence de romarin.Dans ce contexte, les plants de romarin ou de sauge utilisйs
habituellement ont une application orientйe vers l'extraction des huiles essentielles.
Aussi les matiиres vйgйtales obtenues rйsultant aprиs une distillation aqueuse permettant
d'obtenir l'huile essentielle ont une composition en antioxydants йminemment variable les rendant
impropres а une utilisation industrielle comme matiиres premiиres а l'obtention d'antioxydants ou
d'йpices utilisables а titre d'additifs alimentaires, et ont toujours йtй jetйes.
Rйsumй de l'invention
L'invention rйsulte de la dйcouverte selon laquelle il йtait possible d'obtenir, а partir de certaines
йpices, une matiиre vйgйtale ayant а la fois des teneurs йlevйes et stables en antioxydants et en
huiles essentielles.
L'obtention de plants desdites йpices, et de matiиres vйgйtales issues desdits plants offre un
nouvel intйrкt йconomique qui est leur valorisation а la fois dans l'industrie agro-alimentaire et dans
la parfumerie.
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Aucune sйlection d'йpices au regard de leur teneur en antioxydants n'a jamais йtй effectuйe et les
populations naturelles de plantes les contenant prйsentent une grande variabilitй quant а cette
teneur et l'activitй antioxydante y associйe.
Dans l'objectif d'obtention des plants prйsentant la caractйristique d'une haute teneur en
antioxydant, il йtait dans un premier temps important de savoir si une telle caractйristique йtait liйe
ou non а leur contenu en huile essentielle.
Pour effectuer le criblage de plants de romarin prйsentant les caractйristiques requises, il fallait
prйalablement mettre au point une mйthodologie. Celle-ci consiste dans un premier temps а
sйlectionner une collection de plants de romarin prйsentant des gйnotypes diffйrents, puis
d'effectuer une propagation vйgйtative de chacun des plants collectйs et ce, en champs, а raison
de cinq rйplications de cinq plants par gйnotypes soit 25 plants par gйnotypes. Dans le prйsent
texte seront utilisйs indiffйremment les termes de gйnotype, ou de clone pour dйsigner des
individus identiques gйnйtiquement et propagйs par voie vйgйtative.Le plant est dйfini comme la
plante sйlectionnйe avant sa mise en place en terre, autrement dit un plant donnй correspond
nйcessairement а un clone donnй ; en revanche а un clone peuvent correspondre plusieurs plants ;
cet ensemble de plants gйnйtiquement identiques est dйfini comme un cultivar.
Matiиre vйgйtale signifie toute matiиre premiиre issue d'un plant ou d'un cultivar destinй а кtre
transformй pour en extraire une substance ; dans le cas de la prйsente invention, il peut s'agir de la
plante entiиre fraоche ou sиche, ou des feuilles fraоches ou sйchйes.
Dans la mйthodologie de criblage des clones rйpondant aux critиres choisis, il йtait nйcessaire
d'utiliser plusieurs sites d'essais en champs avec la mкme collection sйlectionnйe au dйpart, les
analyses des йchantillons collectйs se faisant par la suite en parallиle et en aveugle.
L'autre paramиtre essentiel de la mйthodologie de criblage est la dйfinition d'un procйdй
d'extraction et ou de purification commun pour tous les laboratoires travaillant sur le projet et pour
les diffйrents sites d'essais en champs.
Un troisiиme paramиtre essentiel dans la prйsente mйthodologie est la mise au point de
procйdures analytiques communes et l'йvaluation de la dйviation standard obtenue а partir de la
rйcolte des 25 plants des clones considйrйs ; la mйthodologie implique enfin la mise en йvidence
d'йventuelles modifications physiologiques en fonction soit du rythme journalier soit du rythme
222/1651
mensuel ; il va de soi que le rythme saisonnier conduit а des modifications notamment dans la
teneur en huile essentielle, la production йtant plus importante pendant les mois d'йtй (de chaleur)
que dans les mois d'hiver.
Aprиs avoir calculй la dйviation standard des paramиtres que sont : le contenu en huile essentielle
soit aprиs dйcantation soit aprиs extraction, le temps d'induction de l'extrait йthanolique mesurй
par le test Rancimat (19, 20), le contenu en carnosol, en acide carnosique, en verbenone ainsi que
leur rendement d'extraction respectif, chaque paramиtre est mesurй et les diffйrents cultivars
provenant d'une collections de 44 clones de cultures effectuйes sur deux sites diffйrents, en France
(Francereco) ou en Espagne (Hispareco) ont йtй criblйs au regard de ces diffйrents paramиtres et
les rйsultats sont les suivants :
a) les variations journaliиres du contenu en huile essentielle, ainsi que en carnosol + acide
carnosique (antioxydants) sont insignifiantes quelque soit le lieu de culture.Malgrй tout par souci
d'homogйnйisation toutes les rйcoltes sont faites en dйbut d'aprиs-midi ;
b) pour ce qui concerne des variations bimensuelles en huile essentielle et en acide carnosique +
carnosol (antioxydants) il a йtй montrй une bonne stabilitй entre aoыt et octobre en France et
entre juillet et septembre en Espagne. Des exemples et des courbes dйtaillйs sont prйsentйs plus
loin et on peut en conclure que la meilleure pйriode de rйcolte est le mois d'aoыt en Espagne et le
mois de septembre ou octobre en France.
La figure 1 est un schйma reprйsentant le procйdй de distillation а la vapeur d'eau des clones de
romarin pour obtenir l'huile essentielle d'une part et les rйsidus de romarin d'autre part.
Les rйsidus obtenus aprиs distillation acqueuse de la matiиre vйgйtale sont appelйs <>, et ils
sont traitйs ensuite pour en extraire les antioxydants, comme schйmatisй sur la figure 2.
L'ensemble du procйdй de sйlection de cultivars de romarin par la mйthodologie dйcrite plus haut
ainsi que les diffйrentes йtapes dudit procйdй font partie de l'invention, l'objectif du travail rappelй
au dйbut йtant d'obtenir une matiиre premiиre valable au plan industriel et permettant d'extraire
des antioxydants utilisables notamment en agro-alimentaire ; si, en outre, le contenu en huile
essentielle y est relativement important, la mкme matiиre premiиre pourrait alors par une sorte de
<> кtre utilisйe а la fois dans l'industrie de la parfumerie et dans l'industrie agro-alimentaire.
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Grвce aux diffйrents paramиtres calibrйs de la faзon dйcrite plus haut, il a йtй possible de
sйlectionner des plants d'йpices, caractйrisйs en ce que la matiиre vйgйtale qui en est issue
prйsente simultanйment un contenu йlevй en antioxydants et en huile essentielle. Cette matiиre
vйgйtale, objet de l'invention, est en outre caractйrisйe par son contenu en antioxydants qui est
supйrieur а 1% en poids du vйgйtal frais ou supйrieur а 3,5% en poids de matiиres sйches, et
leur contenu en huile essentielle qui est supйrieur а 0,3% en poids sur le vйgйtal frais ou supйrieur
а 1,5% en poids de matiиres sйches. Les plants d'йpices possйdant ces caractйristiques font
partie de l'invention. Le romarin et la sauge sont deux йpices particuliиrement propices а
l'obtention de la matiиre vйgйtale de l'invention. La description dйtaillйe ci-dessous met en
йvidence que deux clones de romarin sont particuliиrement intйressants de ce point de vue : les
clones 28 et 39.
Les teneurs en huile essentielle (EO) et en antioxydants (AO) dans la matiиre vйgйtale permet de
calculer la quantitй totale d'EO et AO pouvant кtre obtenue par plant (EOP et AOP) soit le produit :
teneur (en pourcentage) x par matiиre sиche (gramme par plant). Les plantations d'йpices et
notamment de romarin prйsentent un rendement а l'hectare йminemment variable notamment pour
ce qui concerne le rendement en poids de feuilles sйchйes, source aussi bien des antioxydants
que de l'huile essentielle. Les plants de romarin de l'invention, sйlectionnй par la mйthodologie de
l'invention prйsentent l'intйrкt d'avoir un rendement а l'hectare supйrieur а 7000 Kg/Ha,
permettant d'obtenir un rendement а l'hectare d'antioxydants d'au moins 270 kg/Ha et un rendement
а l'hectare d'huile essentielle d'au moins 120 Kg/Ha.
Les plants de romarin de l'invention, et sйlectionnйs par la mйthodologie dйcrite plus haut
prйsentent une variation journaliиre ou bimensuelle de leur teneur en antioxydants et/ou en huiles
essentielles infйrieure а 20%.
Les clones ainsi sйlectionnйs peuvent кtre caractйrisйs sur le plan molйculaire par une empreinte
molйculaire (finger print) la technique utilisйe йtant celle dйcrite dans (22) et plus loin dans
l'exemple sur les empreintes molйculaires.
La prйsente invention est relative йgalement au procйdй de sйlection de plants permettant
l'obtention de drкches а teneur йlevйe en antioxydants consistant en la mise en oeuvre d'au moins
les йtapes suivantes :
une calibration des paramиtres йtudiйs sur une population statistiquement valable,
224/1651
un criblage parmi les plants а disposition de ceux prйsentant des taux supйrieurs а la moyenne
de ceux observйs dans les plants sauvages,
la multiplication vйgйtative des plants ainsi sйlectionnйs,
lesdits paramиtres йtant les mesures des teneurs en huile essentielle et en antioxydants.
Dans le procйdй de l'invention, la matiиre vйgйtale issue des plants sйlectionnйs a en outre une
teneur en huile essentielle supйrieure а 0,3% en poids de vйgйtal frais ou а 1,5% en poids de
matiиres sиches, et une teneur en antioxydant supйrieure а 1% en poids du vйgйtal frais et 3,5%
en poids de matiиres sиches. Les antioxydants sont constituйs au moins de carnosol et d'acide
carnosique.
La prйsente invention est йgalement relative а l'utilisation de la matiиre vйgйtale issue des plants
d'йpices sйlectionnйs par un procйdй de sйlection tel que dйcrit plus haut pour l'obtention de
drкches а haute teneur en antioxydants et utilisable comme additifs alimentaires ou comme йpices ;
l'utilisation de ces plants de romarin permet en outre, par une distillation aqueuse des feuilles
sйchйes l'obtention de l'huile essentielle utilisable en parfumerie de faзon trиs avantageuse dans
la mesure oщ son taux est йgal ou supйrieur а celui du taux des plantes sauvages habituellement
utilisйes en parfumerie.
Enfin, l'invention est relative а des compositions utilisables dans un additif alimentaire et contenant
des antioxydants caractйrisйes en ce que lesdits antioxydants sont obtenus а partir de matiиre
vйgйtale sйlectionnйe par un procйdй tel que dйcrit sommairement ci-dessus et en dйtail cidessous.
La mйthodologie utilisйe a йtй appliquйe de faзon systйmatique sur des plants de romarin et
dйcrite ci-aprиs. La transposition а d'autres types d'йpices notamment la sauge, le thym, l'origan
ou la girofle est aisйment transposable par l'homme du mйtier, йtant connus les diffйrents
procйdйs d'extraction utilisables (6 а 13).
Le procйdй de sйlection des nouveaux plants de romarin selon le critиre d'activitй antioxydante
dйfini plus haut permet en outre l'obtention de plants prйsentant une DHS (diffйrence,
homogйnйitй, stabilitй) qui permet, par multiplication vйgйtative, d'avoir une matiиre premiиre
constante et donc valable а des fins d'utilisation industrielle. Dans la prйsente description, la
mйthodologie employйe pour la sйlection des clones d'йpices prйsentant les caractйristiques
souhaitйes et les exemples а l'appui de cette mйthodologie sont prйsentйs pour des plants de
225/1651
romarin.Il est clair qu'а partir du moment oщ l'on recherche des йpices qui prйsentent а la fois les
caractйristiques d'кtre une matiиre premiиre pour des additifs alimentaires et pour l'obtention
d'huiles essentielles utilisables en parfumerie, la mйthodologie observйe et dйcrite en dйtail plus
loin peut кtre transposйe а l'obtention de nouveaux clones prйsentant ces caractйristiques ; aussi
tout ce qui dans le texte est relatif au romarin, peut s'appliquer йgalement а d'autres types de
plantes aromatiques.
Description dйtaillйe de l'invention
La description dйtaillйe ci-dessous et les figures qui l'accompagnent mettent bien en йvidence la
mйthodologie utilisйe dans le procйdй de sйlection de clones ayant а la fois une haute teneur en
huile essentielle et en antioxydants, et les caractйristiques mкmes de ces plantes sйlectionnйes.
Dans un premier temps les dйtails sur les diffйrentes йtapes du procйdй notamment : la
mйthodologie de criblage, la rйalisation des essais en champs, la mйthode de distillation, les
procйdйs analytiques, les rйsultats de dosages en huile essentielle obtenus dans les clones
sйlectionnйs ainsi que des dosages en antioxydants, enfin les rendements а l'hectare obtenus
aussi bien pour l'huile essentielle que pour les antioxydants ont йtй calculйs.
Les lйgendes des figures citйes ci-aprиs sont les suivantes :
La figure 1 est un exemple de schйma montrant le <> ou la distillation du romarin conduisant а
l'obtention de l'huile essentielle d'une part par distillation aqueuse et de rйsidus de romarin appelйs
drкches.
La figure 2 dйcrit le procйdй d'obtention d'un extrait d'antioxydant а partir des drкches. RE-S
signifie l'extrait sec.
La figure 3 reprйsente les variations journaliиres de la teneur en EO et AO de deux clones puis au
hasard : les clones 28 et 30.
HE = huiles essentielles (йquivalent а EO).
AO = antioxydants.
226/1651
La figure 4 reprйsente les variations bimensuelles en EO (HE) et en AO en fonction de la date de
rйcolte ; la figure 4a reporte les rйsultats obtenus en France (Francereco) et la figure 4b ceux
obtenus en Espagne (Hispareco).
La figure 5 reprйsente le contenu en huile essentielle des 44 clones exprimйs en pourcentage de
poids (en g pour 100 gr) de matiиre sиche, obtenus en Espagne et (EOH) et en France (EOF).
La figure 6 reprйsente le contenu en antioxydants, en g pour 100 gr de matiиre sиche, en France
(AOF) et en Espagne (AOH) pour les 44 clones analysйs.
La figure 7 reprйsente l'йvaluation du contenu en huile essentielle de 44 clones testйs, exprimйs
soit en pourcentage de matiиres sиches, soit en gramme par plante.
La figure 8 reprйsente l'йvaluation du contenu en antioxydants de ces mкmes clones, exprimйs
soit en pourcentage de matiиres sиches, soit en gramme par plante.
1) METHODES ET PROCEDES.
1.1 Mйthodologie de criblage.
Jusqu'а prйsent les plants de romarins n'ont jamais йtй considйrйs quant а leur activitй
antioxydante. Cela signifie que dans la population naturelle ce critиre est йminemment variable
aussi la mйthodologie utilisйe a-t-elle йtй de :
rйaliser une prospection botanique,
de rйaliser une propagation vйgйtative de chacun des plants collectйs,
de rйaliser un criblage de la collection de clones par un essai randomisй sur deux lieux distincts.
Prйalablement а ces essais, il йtait nйcessaire de dйfinir un procйdй de distillation et d'extraction
commun pour tous les sites d'expйrimentation, puis d'йvaluer la dйviation au standard des
227/1651
procйdйs analytiques mis au point, et de mettre s'il existe en йvidence un effet possible de la
pйriode de rйcolte soit dans un jour donnй soit dans un mois donnй, et enfin une йvaluation d'un
effet possible de la date de rйcolte pendant la saison de croissance active.
Dans l'optique de limiter le nombre d'analyses, il a йtй rйcoltй un йchantillon de chaque clones
rйpliquйs au sein d'un cultivar et de les mйlanger avant l'analyse. Cela permet de diviser par 5 le
nombre d'analyses par clone. Cela permet, d'observer l'annйe suivante chaque rйplication de
chaque meilleur clone sйlectionnй et des 5 parmi les plus mauvais tels que dйterminйs pendant
l'annйe prйcйdente.
1.2 Essais en champs.
Il a йtй йtabli une collection d'environ cent plants de romarins ; un premier groupe de 44
gйnotypes a йtй rassemblй.
Chacun de ces gйnotypes a йtй ensuite propagй en champs ; les essais en champs randomisйs
incluent 5 rйplications de 5 plants par gйnotype ce qui donne 25 plants par clone, l'ensemble de
ces 25 plants reprйsentant un cultivar.
1.3. Procйdйs de distillation et d'extraction.
Les figures 1 et 2 sont un exemple de procйdй utilisй pour l'obtention de l'huile essentielle et des
antioxydants.
Dans la figure 2 les rйsidus de romarin sont extraits deux fois а l'hexane (en proportion 1:4) suivi de
deux extractions а l'йthanol (1:4). L'extrait а l'hexane est contrelavй avec йthanol 80% (p/p) et la
phase йthanolique est ajoutйe а l'extrait а l'йthanol. Cet extrait est ensuite dйcolorй par 3 % de
charbon actif, concentrй, prйcipitй а l'eau puis filtrй et sйchй. Le procйdй utilisй est dйcrit en
dйtail dans le brevet EP 307 626 et dans la demande de brevet EP 507 064 lorsque l'on souhaite
obtenir un extrait liquide d'antioxydant.
228/1651
D'autres variantes d'extraction d'antioxydants sont йgalement dйcrites dans la demande de brevet
EP 480 077, et incorporйes ici par rйfйrence.
Les procйdйs utilisйs dans les diffйrents sites d'essais en champs sont les mкmes d'un site а
l'autre. Les rйsidus obtenus aprиs distillation de la poudre de romarin et rйextraite avec du
diйthylйne ; ultйrieurement, cette seconde extraction a йtй supprimйe car inutile : trиs peu
d'huiles essentielles ont йtй obtenues par distillation au diйthylйne, la classification des clones
йtait semblable que ce soit uniquement par distillation simple ou par les deux distillations
successives aussi des considйrations simples d'amйlioration du rendement conduisent а йliminer
cette deuxiиme distillation.
Les huiles essentielles sont obtenues par broyage des parties terminales de tiges sйchйes puis
extraction par hydro-distillation а raison de 15 ml/gr de poudre puis l'huile essentielle est extraite par
de l'йther puis filtrйe aprиs refroidissement et rincйe avec 50 ml d'eau, suivie par deux extractions
en phase aqueuse volume а volume avec du diйthylether.
1.4 Procйdйs analytiques
a) Evaluation de l'activitй antioxydante.
La concentration des composйs impliquйs dans l'activitй antioxydante est йvaluйe par des
analyses rйalisйes sur un extrait йthanolique de la poudre brute de romarin.
L'activitй antioxydante rйsulte essentiellement de l'acide carnosique et du carnosol ; la quantitй de
chacune des ces deux substances dans l'extrait est йvaluйe par HPLC (21).
L'activitй antioxydante de l'extrait est mesurйe par la mйthode Rancimat (19, 20) sur une graisse
de poule.
Test Rancimat
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Le test Rancimat a йtй utilisй а 100 DEG C selon des mйthodes publiйes dans Woestenburg (20).
Un aliquot d'extrait, correspondant а 500 ppm de matiиre sиche, a йtй ajoutй а une graisse de
poule dйsodorisйe et on a dйterminй le temps d'induction de cette graisse <>. La graisse de
poule dйsodorisйe a йtй prйparйe selon une mйthode publiйe (19) ; il a йtй vйrifiй que
l'йthanol introduit dans la graisse pendant la prйparation des йchantillons n'influence pas les
rйsultats obtenus.
Les mesures de Rancimat obtenues sur les 36 clones testйs sont rйsumйs dans le tableau 1 cidessous, qui en outre donne les valeurs obtenues pour le contenu en acide carnosique + carnosol
exprimй en pourcentage de matiиre sйche.
Id=Tableau 1 Columns=4
Head Col 1: CLONES
Head Col 2: E.O.DECANTES mg/100g DM
Head Col 3: RANCIMAT (h)
Head Col 4: ACIDE CARNOSIQUE + CARNOSOL (Poids %)
2025317.20.85
4435622.51.06
2953619.82.26
3377024.52.01
4378119.81.76
4079422.31.85
1279620.62.09
30102724.21.7
8104031.11.75
2106538.32.46
32114225.61.79
26117832.52.57
35118629.12.46
4121339.12.75
5126536.02.90
41129525.62.89
9135531.63.09
21136337.22.31
230/1651
25148233.53.54
10148638.43.65
31174540.93.74
13175830.63.87
22183330.83.2
42185234.33.25
28200240.23.80
37201934.13.29
38208433.22.65
19208539.83.07
24219653.34.86
34232532.13.26
23233543.04.74
14236538.43.24
17238340.03.91
27239634.13.76
18239733.43.73
39264131.13.78
Valeur moyenne152232.12.82
SD6517.70.97
SD/Valeur moyenne (%)432434
Ce tableau fait clairement apparaоtre une corrйlation entre la quantitй d'huile essentielle
dйcantйe et la valeur de Rancimat mкme si des variations existent.
SD signifie <>.
Evaluation de carnosol et d'acide carnosique par HPLC.
Cette technique est bien connue de l'homme du mйtier ; un exemple de rйalisation est dйcrit dans
(21), et les rйsultats obtenus prйsentйs dans le tableau 1 ci-dessus.
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b) Analyse de dйviation standard des diffйrents paramиtres.
La dйviation standard a йtй йvaluйe pour les paramиtres suivants :
le contenu en matiиre sиche de la poudre,
le volume et le poids des huiles essentielles extraites par distillation vapeur,
le poids d'huiles essentielles extraites d'un rйsidu diйthyl-ether,
le test Rancimat,
et la concentration de certains des composйs impliquйs dans les activitйs antioxydantes.
Le tableau 2 ci-dessous indique les valeurs moyennes obtenues sur les diffйrents paramиtres, la
dйviation standard et le pourcentage de la dйviation standard sur la valeur moyenne et ce pour le
pourcentage de matiиres sиches, les huiles essentielles dйcantйes exprimйes en ml pour 100 gr
de matiиre sиche, les huiles essentielles dйcantйes exprimйes en ml pour 100 gr de matiиre
sиche, les huiles essentielles extraites exprimйes en mg pour 100 gr de matiиre sиche, le test
Rancimat rйalisй en Espagne, le test Rancimat rйalisй en France et pour ce qui est des extraits а
activitй antioxydante sont mesurйs le contenu en carnosol, le contenu en acide carnosique, la
somme des deux, le verbenone et le rendement (йgalement en pourcentage) ; pour ce qui est de
l'activitй antioxydante, ES signifie les valeurs obtenues avec les essais en Espagne et (FR) signifie
les rйsultats obtenus а partir des essais en France.
Le coefficient de variation le plus important est observй pour l'йvaluation du Rancimat pour laquelle
il atteint 25%. Au contraire les mesures analytiques obtenues а partir d'un extrait brut, ou sur un
composй dйfini prйsente toujours un coefficient de variation infйrieur а 9% sauf pour le volume
d'huile essentielle obtenu pour 100 gr de matiиre sиche qui est de 11,8% ; ce dernier paramиtre
n'est probablement pas si fiable que les autres du fait des difficultйs de mesures sur un petit
volume ; aussi la mesure du poids/poids plutфt que celle du volume/poids est beaucoup plus fiable
et doit кtre adoptйe.
Ces rйsultats indiquent donc que les paramиtres mesurйs et les procйdйs mis en oeuvre sont
fiables et aptes а кtre utilisйs dans un processus de sйlection de clones а haute teneur en EO et
en AO.
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1.5. Variations climatiques
En dehors des variations inhйrentes aux procйdйs analytiques, il йtait nйcessaire d'йtudier les
variations journaliиres d'une part et les variations bimensuelles d'autre part
a) Evaluation des variations journaliиres.
Deux clones choisis au hasard (28 et 30) ont йtй rйcoltйs chaque deux heures entre 6 heures et 18
heures en France et en Espagne; les paramиtres analysйs ont йtй le contenu en huile essentielle
distillйe ou extraites d'une part et en carnosol plus acide carnosique d'autre part ; la figure 3
reprйsente les rйsultats obtenus et indique que les variations journaliиres ne sont pas significatives
et ce pour aucun des paramиtres mesurйs
b) Evaluation de variations bimensuelles
Les mкmes clones ont йtй rйcoltйs chaque deux semaines entre la mi-juin et la fin du mois
d'octobre (en France) et entre la mi-juillet et la fin du d'octobre en Espagne. Les mкmes paramиtres
ont йtй utilisйs pour йvaluer une йventuelle variation. Les figures 4a et 4b reprйsentent ces
variations bimensuelles. Il apparaоt :
des variations importantes dans le contenu en huile essentielle selon la pйriode de rйcolte, ce
contenu йtant relativement stable de la fin aoыt а la fin octobre en France et de la fin juillet а la fin
aoыt en Espagne ; ceci est parfaitement logique compte tenu des diffйrences climatiques entre la
France et l'Espagne. Le contenu en activitй antioxydante est stable dans la pйriode utilisйe. Ces
rйsultats indiquent que la pйriode de rйcolte optimale est aoыt en Espagne , septembre ou
octobre en France.
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2) CRIBLAGE DES CLONES.
L'ensemble de ces paramиtres йtant calibrй, le criblage des clones parmi les 44 plants йtudiйs a
pu кtre rйalisй sur tous les gйnotypes.
La figure 5 indique le contenu en huile essentielle des 44 clones exprimйs en pourcentage de poids
(de matiиre sиche) obtenu en Espagne et (EOH) et en France (EOF).
La figure 6 reprйsente le contenu en antioxydants en g pour 100 gr de matiиre sиche en France
(AOF) et en Espagne, (AOH) pour les 44 clones analysйs.
La figure 7 reprйsente la teneur en huile essentielle et la quantitй d'huile essentielle obtenue par
plants (EOP); de faзon parallиle la figure 8 reprйsente la teneur en antioxydants (en pourcentage)
et le contenu d'antioxydants par plante (AOP). Il apparaоt clairement dans ces figures que les deux
paramиtres ne sont pas corrйlйs et que certains plants peuvent avoir une forte teneur en
antioxydants (figure 8) et par contre prйsenter un contenu relativement faible (cas des clones n DEG
1, 23 ou 37 par exemple).En revanche, les clones intйressants selon l'invention sont ceux qui ont а
la fois une bonne teneur en antioxydants et un contenu par plante йlevй ce qui est observй sur les
clones 28 et 39.
De la mкme faзon on voit qu'il n'y a guиre de corrйlation entre la teneur en huile essentielle et le
contenu par plantes ; les clones 11, 19, 27, 28, 34 et 39 sont particuliиrement intйressant quand а
la valeur. des deux critиres rйunis.
Les conclusions que l'on peut tirer de l'observation des figures 5 а 8 sont les suivantes :
Une grande variabilitй est observйe dans la collection des 44 clones dans la mesure oщ le
contenu en huile essentielle varie entre 253 а 3130 mg pour 100 gr de matiиres sиche pour une
rйcolte en France au mois d'aoыt. Cette variabilitй est reprйsentйe dans le tableau 3 ci-dessous.
Il apparaоt clairement des figures 7 et 8 ainsi que du tableau 1 ci-dessus que les clones n DEG 28
et 39 prйsentent le contenu le plus avantageux en EO et en AO. Aussi ces deux clones ont-ils йtй
йtudiйs de faзon beaucoup plus approfondie pour leur contenu en huiles essentielles, en
antioxydants et pour le rendement а l'hectare de l'un et de l'autre.
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3) CONTENU EN HUILES ESSENTIELLES DES CLONES 28 ET 39.
1660 kg du clone n DEG 28 et 312 kg du clone n DEG 39 ont йtй distillйs en utilisant les
techniques d'extraction habituelles. La charge est d'environ 300 kg de vйgйtal frais (50% environ
d'humiditй) auquel on ajoute 200 l d'eau. Le chauffage est rйalisй par vapeur directe (introduction
par le fond de l'appareil) et circuit coquillй. Il est important, avant toute opйration, de vidanger le
circuit de vapeur entiиrement pour йliminer les particules de fer qui se trouvent dans la canalisation.
Le chauffage est de 30 mn environ pour arriver au dйbut de la coulйe.
La distillation a une durйe de 2 h 30 а partir du dйbut de la coulйe puis l'eau est vidangйe par
ouverture de la vanne de fond d'appareil. L'ensemble est ensuite sйchй par mise sous vide de
l'appareil et chauffage au circuit coquillй ; la durйe de ces opйrations de vidange, sйchage et
chauffage est de 45 mn а 1 h et le processus est arrкtй lorsque qu'il ne distille plus d'eau.
L'appareil est ensuite dйchargй par ouverture de fond basculant. Les branches sont sйchйes sur
aire bйtonnйe en les йtalant sur une hauteur de 10 cm environ et en les retournant frйquemment.
Par triage manuel on sйpare ensuite les йpis de romarin des branches.Les rйsultats des
distillations pour les clones 28 et 39 sont donnйs dans les tableaux 4a et 4b ci-dessous.
Rйsultats des distillations :
Id=1) Tableau 4a : clone 28 Columns=4
Head Col 1 AL=L: Charge
Head Col 2 AL=L: Essence obtenue
Head Col 3 to 4: Rendement %
SubHead Col 1:
SubHead Col 2:
SubHead Col 3: sur vйgйtal frais
SubHead Col 4: sur vйgйtal sec (calculй)
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293 Kg1,020 Kg0,350,65
305 Kg2,580 Kg0,430,79
299 Kg
304 Kg2,725 Kg0,450,84
295 Kg
164 Kg0,735 Kg0,45 Kg0,83
1660 Kg7,060 Kg0,4250,92
Id=2) Tableau 4b : Clone n DEG 39 Columns=4
Head Col 1 AL=L: Charge
Head Col 2 AL=L: Essence obtenue
Head Col 3 to 4:Rendement %
SubHead Col 1:
SubHead Col 2:
SubHead Col 3: sur vйgйtal frais
SubHead Col 4: sur vйgйtal sec (calculй)
312 Kg1,830 Kg0,581,15
Les huiles essentielles sont ensuite йvaluйes quant а leur qualitй olfactive d'une part et quant а
leur constituant d'autre part.
Les huiles essentielles ont йtй йvaluйes sur mouillettes fraоchement trempйes puis <>, en
comparaison avec un йchantillon commercial standard d'origine espagnole.
Les constituants des huiles essentielles des clones 28 et 39 sont dйterminйs par chromatographie
en phase gazeuse ; l'huile essentielle issue du clone 28 possиde une composition trиs voisine de
celle de l'huile essentielle expйrimentale. Toutefois la teneur en camphre n'y est que de 28% au lieu
de 43,4%. Les teneurs en terpиne ( alpha et beta pinиne et camphиne) y sont en revanche plus
йlevйes (22% environ, entre 6% pour l'йchantillon expйrimental).
L'huile essentielle du clone 39 se caractйrise par une teneur йlevйe en cinйole (22%) quasiment
identique а celle de l'йchantillon expйrimental de Francereco.
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3.1. Mesures des antioxydants dans les clones 28 et 39.
Aprиs la distillation vapeur qui permet d'obtenir les huiles essentielles comme dйcrit plus haut, les
rйsidus de la distillation (les drкches) sont extraits dans un rйacteur avec 200 1 d'йthanol, pendant
4 heures et а 25 DEG . Le rйsultat de cette extraction, appelй extrait AR (pour <>) est ensuite filtrй
et concentrй pour donner un produit brun vert qui va кtre dosй. Les rйsultats du contenu en
antioxydant sont reprйsentйs dans le tableau 5 ci-dessous ; il y apparaоt que aussi bien le contenu
en antioxydant sur la matiиre premiиre que de l'extrait est au moins deux fois supйrieur а celui des
extraits courants.
Dans un autre essai, des йchantillons diffйrents des feuilles de romarin ont йtй analysйs par HPLC.
Il s'agit de deux йchantillons classiques : Murcia et Nogales, les clones 28 et 39 et le clone 28
aprиs hydro-distillation.
Id=Tableau 6 : Teneur en antioxydants Columns=4
Head Col 1: Echantillon
Head Col 2: Teneur en acide carnosique
Head Col 3: Teneur en Carnosol
Head Col 4: Teneur en * antioxydants
Murcia dist.1.80.42.2
Nogales dist.1.70.52.2
Clone 394.50.34.8
Clone 284.90.35.2
Clone 28 dist.2.31.13.4
Teneurs en % poids
* Somme d'acide carnosique + carnosol
Le tableau 6 ci-dessus montre que la teneur en antioxydant mesurйe par la somme d'acide
carnosique et de carnosol est deux а trois fois plus forte que dans les йchantillons courants, cette
teneur йtant lйgиrement diminuйe aprиs hydro-distillation mais restant cependant bien supйrieure
а la normale. L'analyse du contenu en carnosol et acide carnosique par HPLC des feuilles montre
237/1651
que l'hydro-distillation avec la vapeur directe est trиs mйnageante en ce qui concerne les
antioxydants. Le traitement thermique (3 heures de distillation) suivi de sйchage dйtruit un tiers des
antioxydants. La comparaison de clones de romarin sauvage et de romarin sйlectionnй traitйs et
triйs de la mкme maniиre montre que les clones sont nettement plus performants au regard de la
teneur en AO.
Dans une expйrience ultйrieure la teneur antioxydante de six йchantillons diffйrents de romarin
ont а nouveau йtй йtudiйs par HPLC sur feuilles sйchйes aprиs extraction Soxtec. Outre la
teneur en carnosol et acide carnosique, la teneur en acide rosmarinique, antioxydant hydrosoluble
du romarin, ont йtй mesurйes.
Le tableau 7 ci-dessous donne les rйsultats obtenus pour les clones 28 et 39.
Id=Tableau 7 Columns=6
Head Col 1: Code
Head Col 2: Age des plantes [ans]
Head Col 3 to 6: Teneur en antioxydants (% poids)
SubHead Col 1:
SubHead Col 2:
SubHead Col 3: Acide rosmarinique
SubHead Col 4: Carnosol (C)
SubHead Col 5: Acide carnosique (CA)
SubHead Col 6: Somme C+CA
H 2830.80.354.655.0
AM 2820.250.45.25.6
AM 28.120.950.355.455.8
CM 2810.20.55.45.9
H 3931.10.354.95.25
AM 3920.50.35.35.6
Les termes H 28 et H 39 signifient que les clones ont йtй cultivйs sur un terrain de Hispareco. Les
autres йchantillons reprйsentent des clones qui ont йtй cultivйs sur plusieurs hectares sur deux
238/1651
autres sites AM et CM ; l'йchantillon AM 28.1 provient d'un petit lot qui a йtй rйcoltй un mois
aprиs les clones codйs AM28.
3.2 Rendement des cultivars 28 et 39.
Les cultivars 28 et 39 de romarin ont 2 а 2,5 fois plus d'activitй antioxydante comparйs aux
souches sauvages.
Cette augmentation du contenu dans ces composйs а activitй oxydante est accompagnйe par une
augmentation du contenu en huile essentielle (voir tableau 1)
Deux essais en champs en Espagne sur deux fois 2500 m2 avec chacun des clones 28 et 39 ont
йtй rйalisйs. Les rendements de ces clones est de 5,6 tonnes de feuilles de romarin sйchйes par
hectare contenant 4% de la matiиre sиche en composants actifs antioxydants.
Le tableau 8 ci-aprиs les rйsultats obtenus avec les clones 28 et 39, comparйs а des clones
sauvages (Nogales et Murcia) en termes de rendement obtenu pour les huiles essentielles et pour
les A.R. (extraits antioxydants obtenus а partir des drкches).
4. EMPREINTES MOLECULAIRES
Des empreintes molйculaires (ou "Finger Prints" en anglais") ont йtй rйalisйes parmi une
population de 50 clones de romarin renfermant notamment les clones 28 et 39. Les rйsultats
montrent qu'il est possible de diffйrencier sans ambiguitй les clones 28 et 39.
La mйthode utilisйe est la technique AFLP (qui est l'abbrйviation anglaise de "Amplified Fragment
Length Polymorphism") dйcrite dans EP534858 (Keygene). Le principe de la mйthode repose sur
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l'amplification sйlective de fragments de restriction grвce а des amorces nuclйotidiques
spйcifiques. Pour chaque combinaison "enzyme de restriction et amorces" (EA) un polymorphisme
spйcifique est rйvйlй en gel d'acrylamide. Une seule combinaison EA permet la lecture de
plusieurs dizaines de bandes, qui sont chacunes assimilables а une allиle.
REFERENCES
(1) PRUTHI J.S. (1980) - <>, Academic Press, London.
(2) SHELEF L. A. (1983) - J. Food Safety 6, 29.
(3) CHIPAULT .J.R. et al (1952) - Food Res. 17, 46.
(4) CHIPAULT .J.R. et al (1955) - Food Res. 20, 443.
(5) CHIPAULT .J.R. et al (1956) - Food Tech. 10, 209.
(6) BERNER D.L. et al (1985) -Brevet EU 3'732'111.
(7) CHANG S.S. et al (1973) - Brevet EU 3'950'266.
(8) CHANG S.S. et al (1977) - J.Food Sci. 42, 1102.
(9) HARTMANN V.E. et al (1980) - Parfums, cosmйtiques, arфmes No 36, 33.
(10) KIMURA Y. et al (1981) - Brevet Europйen 0'038'959.
(11) CALAME J.P. (1985) - Brevet Europйen 0'154'258 (12) TATEO F. et al (1988) Perfumer &
Flavorist 13 (10/11), 27.
(13) CUVELIER M.E. et al (1991) - dans <> Rivista Italiana EPPOS 2 (3), 374.
(14) BERSET C. et al (1989) - Lebensm. Wiss u. Technol. 22, 15.
(15) BARBUT S. et al (1985) - J. Food Sci. 50, 1356.
(16) BRACCO U. et al (1981) - JAOCS 58, 686.
(17) AESCHBACH R. et al (1986) - Bull. Liaison Groupe Polyphйnol 13, 56.
(18) GRANGER R. (1973) - Parf. Cosm. Sav. France 3, 133, 307.
(19) LAMBELET P., SAUCY F., LOLIGER J., (1985) Chemical Evidence for interactions between
Vitamin E and C. ; Experientia 41, 1384-88.
(20) WOESTENBURG W.J., ZAALBERG J., - Determination of Stability of Edible Oils - Inerlaboratory
test with the Automated Rancimat Method; Fette, Seifen, Anstrichmittel 88, 53-6 (1986).
(21) Aruoma O.J. et al., (1992) Xenobiotica 22, 257.
(22) William J.G.K. et al. (1990), Nucleic Acids Research 18, 6531
240/1651
Claims:
1. Matiиre vйgйtale de plants d'йpices caractйrisйe en ce qu'elle prйsente simultanйment un
contenu йlevй en antioxydants et en huiles essentielles, de telle faзon que :
le contenu en antioxydants soit supйrieur а 1,5% en poids du vйgйtal frais ou supйrieur а 3,5%
en poids de matiиres sиches, et
le contenu en huile essentielle soit supйrieur а 0,3% en poids de vйgйtal frais ou supйrieur а
1,5% en poids de matiиres sиches.
2. Matiиre vйgйtale selon la revendication 1 caractйrisйe en ce les plants dont elle est issue
prйsentent en outre un rendement а l'hectare en huile essentielle d'au moins 120 Kg/Ha et en
antioxydants d'au moins 270Kg/Ha.
3. Matiиre vйgйtale selon l'une des revendications 1 а 2 caractйrisй en qu'elle est issue de plants
de romarin.
4.Plants d'йpices utilisables comme matiиre premiиre а l'obtention de la matiиre vйgйtale selon
l'une des revendications 1 а 3.
5. Drкches obtenues aprиs distillation aqueuse de matiиre vйgйtale selon l'une des
revendications 1 а 3 caractйrisйes en qu'elles prйsentent un contenu en antioxydant supйrieur а
3,5 % en poids desdites drкches.
6.Procйdй de sйlection de plants d'йpices permettant l'obtention de matiиre vйgйtale а teneur
йlevйe en antioxydants consistant en la mise en oeuvre d'au moins les йtapes suivantes:
une calibration des paramиtres йtudiйs sur une population statistiquement valable,
un criblage parmi les plants de ceux prйsentant des taux supйrieurs а la moyenne de ceux
observйs dans les plants sauvages,
241/1651
la multiplication vйgйtative des plants ainsi sйlectionnйs,
lesdits paramиtres йtant les mesures des teneurs en antioxydants et en huile essentielle.
7. Procйdй selon la revendication 6 caractйrisй en ce que la matiиre vйgйtale issue des plants
sйlectionnйs a une teneur en antioxydants supйrieure а 1% en poids du vйgйtal frais ou 3,5% en
poids de matiиres sиches.
8.Procйdй selon la revendication 7 caractйrisй en ce que la matiиre vйgйtale issue des plants
sйlectionnйs a en outre une teneur en huiles essentielles supйrieure а 0;3% en poids de plante
fraоche ou а 1,5% en poids de matiиres sиches.
9. Procйdй selon la revendication 7 caractйrisй en ce que les antioxydants contiennent au moins
du carnosol et de l'acide carnosique.
10. Procйdй selon l'une des revendications 7 а 9 caractйrisй en ce que l'йpice est le romarin.
11. Utilisation de matiиre vйgйtale issue de plants d'йpices sйlectionnйs par un procйdй selon
l'une des revendications 7 а 10 comme matiиre premiиre pour l'obtention de drкches ayant une
teneur en antioxydants reprйsentant au moins 1% en poids du vйgйtal frais ou 3,5% en poids de
matiиres sиches.
12. Utilisation selon la revendication 11 caractйrisйe en ce que la matiиre vйgйtale sйlectionnйe
permet en outre l'obtention d'huiles essentielles utilisables en parfumerie.
242/1651
50. EP0744177 - 27.11.1996
COMPOSITION CONTAINING AT LEAST ONE ESSENTIAL OIL AND A PROVITAMIN, USEFUL IN
THE PREVENTION AND TREATMENT OF PRESSURE SORES
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP0744177
Inventor(s):
HARTWIG GISELA (DE)
Applicant(s):
HARTWIG GISELA (DE)
IP Class 4 Digits: A61K
IP Class:
A61K35/78
E Class: A61K35/78+M
Application Number:
EP19960107867 (19960517)
Priority Number: DE19951018836 (19950523)
Family: EP0744177
Equivalent:
DE19518836
Cited Document(s):
WO9311780
Abstract:
COMPSN. (I) FOR PREVENTION AND TREATMENT OF BEDSORES, COMPRISES AN EMULSION
CONTG. A VEHICLE, AT LEAST ONE ESSENTIAL OIL, AN EMULSIFIER AND A PRO-VITAMIN. THE
ESSENTIAL OILS ARE: (A) A CELL-GROWTH PROMOTER; (B) A CIRCULATION STIMULATOR; (C)
AN ANTI-VIRAL, ANTI-BACTERIAL OR ANTI-MYOTIC; AND (D) AN ANALGESIC.Description:
243/1651
Die Erfindung betrifft eine Substanz, insbesondere zur Verhьtung und Behandlung von Dekubitus,
mit einem Trдgerstoff, mindestens einem дtherischen Цl und einem Emulgator zum Bilden einer
Emulsion des дtherischen Цles mit dem Trдgerstoff und mit einem Pro-Vitamin.
Aus der "Roten Liste 1995", Arzneimittel-Verzeichnis des BPI und VFA, ECV-Editio Cantor
AULENDORFF/WЬRD; Nummer 84067, ist unter dem Handelsnamen "Heloekzem noro" eine
Heilsalbe bekannt, die neben Pantenol und einem Emulgator auch Ol. Chamomillae enthдlt.
Aus B. Schurch, "DEUTSCHE MEDIZINISCHE WOCHENSCHAU"119/13 (1994), Seite 485 ist es zur
Behandlung von Dekubitus, insbesondere zur Epithelisierung bekannt, neben einer Salbe mit dem
Handelsnamen "Solkoseryl" auch ein Hautverstдrkungsmittel mit Panthenolum, einem Emulgator und
Chamomillae zu verwenden. Aus der AU 630,561 ist eine Creme zur Behandlung von Verbrennungen
bekannt, welche neben Chamomillae Цl auch Myrrhe-Цl aufweist.
Alle diese Substanzen setzen als дtherisches Цl Kamillenцl ein, welches in der Hauptsache ein
antiseptische Wirkung entfaltet und das Zellwachstum bzw. die Durchblutung der Haut nur
geringfьgig fцrdert.
In der Alten- und Krankenpflege kommt es hдufig vor, dass bettlдgerige Patienten an Dekubitus
leiden. Bei dieser Krankheit sind grosse Teile des Gewebes wundgelegen und kцnnen nur schwer
abheilen, da die Patienten aufgrund ihrer Krankheit oder allgemeinen Schwдche weiterhin auf den
wunden Stellen liegen mьssen.
Davon ausgehend liegt der Erfindung die Aufgabe zugrunde, eine Substanz zu schaffen, die dem
Dekubitus vorbeugt bzw. seine Heilung beschleunigt.
Als technische Lцsung dieser Aufgabe wird eine Substanz vorgeschlagen, die ein erstes, das
Zellwachstum anregendes дtherisches Цl, ein zweites, die Durchbltung fцrderndes дtherisches Цl,
ein drittes, antivirales, antibakterielles oder antimykotisches, дtherisches Цl und ein viertes,
schmerzstillendes, дtherisches Цl enthдlt.
Es hat sich gezeigt, dass eine Substanz, bei der ein дtherisches Цl auf Niaouli-Basis, ein
дtherisches auf Grapefruit-Basis, eine Bohnenkraut-Цl, ein Lemonengras-Цl, ein Cajeput-Цl oder
ein Lawendel-Цl unter Zuhilfenahme eines Emulgators in destilliertem Wasser gelцst ist und die
darьber hinaus ein Provitamin aufweist, den Dekubitus von bettlдgerigen Patienten erfolgreich heilt.
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Bei dieser Substanz liegt der Anteil der дtherischen Цle im Gesamt-Volumen zwischen 1 und 10
Volumen-%, vorzugsweise 5 %, wдhrend der Anteil des Provitamins am Gesamt-Volumen der
Substanz zwischen 3 und 5 Volumen-% liegt.
Durch den Einsatz mehrerer, verschiedener дtherischer Цle ist es mцglich, mit ein und derselben
Substanz in gleichzeitig unterschiedliche Wirkungen zu realisieren, so dass der Heilungsprozess
beschleunigt wird.
Diese Substanz wird vorzugsweise als Lotion verabreicht und beschleunigt das Zellwachstum und
fцrdert die Durchblutung. Die hierdurch beschleunigte Heilung der Patienten wird allgemein
begrьsst.
Durch die Hinzunahme eines Dickungsmittels, vorteilhafterweise Xanthan, wird die Substanz
dickflьssig gemacht und kann als Lotion verabreicht werden. Dies hat den Vorteil, dass die die
Wunde verklebende Wirkung einer Salbe vermieden wird und die Substanz aber dennoch solange
an der entsprechenden wunden Stelle verbleibt, das sie ihre volle Wirkung entfalten kann.
Xanthan hat ausserdem den Vorteil, dass es Wasser speichert und so die Wunde lange feucht hдlt,
so dass sich im Bereich der Wunde ein eigenes, feuchtes Mikroklima ausbildet.
Es ist weiterhin heilungsfцrdernd, der Substanz Provitamine, insbesondere D-Panthenol, Vitamin E
Acetat oder Vitamin A Palmitat hinzufьgen. Hierbei sollte der Volumenanteil des D-Panthenol 16
Volumen-%, der Volumenanteil Vitamin E Acetat 8 Volumen-% und der Volumenanteil des Vitamin A
Palmitat 0,1 Volumen-% nicht ьberschreiten.
In einer besonders bevorzugten Ausfьhrungsform wird die erfindungsgemдsse Substanz dadurch
gebildet, dass 1 - 8 Volumen-% LV 41 Emulgator, 0,2 - 1 Volumen-% Niaouli-Цl, 0,2 - 2 Volumen-%
Grapefruit-Цl, 0,1 - 1 Volumen-% Bohnenkraut-Цl, 0,2 - 2 Volumen-% Lemonengras-Цl, 0,2 - 2
Volumen-% Cajeput-Цl, 0,2 - 2 Volumen-% Lawendel-Цl, 0,05 - 0,4 Volumen-% Xanthan, 2 - 16
Volumen-% D-Panthenol, 1 - 8 Volumen-% Vitamin E Acetat und 0,1 - 1 Volumen-% Vitamin A
Palmitat hinzugemischt werden, wobei zum Schluss destilliertes Wasser hinzugegeben wird.
Mit dieser Substanz wurden bisher die besten Heilungserfolge erzielt.
245/1651
Erstes Ausfьhrungsbeispiel:
Substanz mit destilliertem Wasser als Trдgermittel, dem дtherisches Niaouli-Цl und дtherisches
Grapefruit-Цl unter Zuhilfenahme eines Emulgators hinzugefьgt wurden, wobei der Volumenanteil
der Summe der дtherischen Цle zwischen 1 und 10 %, vorzugsweise 5 % des Gesamtvolumes liegt.
Darьber hinaus sind dem destilliertem Wasser 3 - 5 Volumen-% D-Panthenol zugesetzt.
Zweites Ausfьhrungsbeispiel:
Substanz zusammengesetzt aus
0,2 - 1 Vol.% Niaouli-Цl,
0,2 - 1 Vol.% Grapefruit-Цl,
0,1 - 0,5 Vol.% Bohnenkraut-Цl,
0,2 - 1 Vol.% Lemonengras-Цl,
0,2 - 1 Vol.% Cajeput-Цl,
0,2 - 1 Vol.% Lawendel-Цl,
1 - 4 Vol.% LV 41 Emulgator,
0,05- 0,2 Vol.% Xanthan,
2 - 8 Vol.% D Pathenol,
1 - 4 Vol.% Vitamin E Acetat,
0,1 - 0,6 Vol.% Vitamin A Palmitat,
und destilliertem Wasser.
Claims:
1. Substanz, insbesondere zur Verhьtung und Behandlung von Dekubitus,
mit einem Trдgerstoff, mindestens einem дtherischen Цl und einem Emulgator zum Bilden einer
Emulsion des дtherischen Цles mit dem Trдgerstoff und mit einem Provitamin,
246/1651
dadurch gekennzeichnet,
dass die Substanz
ein erstes, das Zellwachstum anregendes дtherisches Цl,
ein zweites, die Durchblutung fцrderndes дtherisches Цl,
ein drittes, antivirales, antibakterielles oder antimykotisches дtherisches Цl, und
ein viertes, schmerzstillendes дtherisches Цl
enthдlt.
2. Substanz nach Anspruch 1,
dadurch gekennzeichnet, dass das Zellwachstum anregende дtherische Цl ein Niaouli-Цl ist.
3. Substanz nach wenigstens einem der vorhergehenden Ansprьche,
dadurch gekennzeichnet, dass das die Durchblutung fцrdernde дtherische Цl ein Grapefruitund/oder Lemonengras-Цl ist.
4.Substanz nach wenigstens einem der vorhergehenden Ansprьche,
dadurch gekennzeichnet, dass das antivirale, antibakterielle oder antimykotische дtherische Цl ein
Bohnenkraut-Цl und/oder ein Lemonengras-Цl ist.
5. Substanz nach wenigstens einem der vorhergehenden Ansprьche,
dadurch gekennzeichnet, dass das schmerzstillende дtherische Цl ein Cajeput-Цl und/oder ein
Lawendel-Цl ist.
6. Substanz nach wenigstens einem der vorhergehenden Ansprьche,
dadurch gekennzeichnet, dass das Provitamin ein 1 D Panthenol oder ein Provitamin B ist.
7. Substanz nach Anspruch 6,
dadurch gekennzeichnet, dass das Provitamin B ein Vitamin E Acetat oder ein Vitamin A Palmitat ist.
8. Substanz nach wenigstens einem der vorhergehenden Ansprьche,
dadurch gekennzeichnet, dass der Emulgator ein LV 41-Emulgator ist.
9.Substanz nach wenigstens einem der vorhergehenden Ansprьche,
gekennzeichnet durch
ein Dickungsmittel, insbesondere Xanthan.
247/1651
10. Substanz nach wenigstens einem der Ansprьche 2 -9, dadurch gekennzeichnet, dass das
Niaouli-Цl und das Grapefruit-Цl zusammen einen Volumenanteil von 1 - 10 Volumen-% der
Substanz ausmachen.
11. Substanz nach wenigstens einem der vorhergehenden Ansprьche,
dadurch gekennzeichnet, dass sich die Substanz zusammensetzt aus
0,2 - 2 Vol.% Niaouli-Цl,
0,2 - 2 Vol.% Grapefruit-Цl,
0,1 - 1 Vol.% Bohnenkraut-Цl,
0,2 - 2 Vol.% Lemonengras-Цl,
0,2 - 2 Vol.% Cajeput-Цl,
0,2 - 2 Vol.% Lawendel-Цl,
1 - 8 Vol.% LV 41 Emulgator,
0,05- 0,4 Vol.% Xanthan,
2 -16 Vol.% D-Pathenol,
1 - 8 Vol.% Vitamin E Acetat,
0,1 - 1 Vol.% Vitamin A Palmitat,
und destilliertem Wasser.
12. Substanz nach wenigstens einem der vorhergehenden Ansprьche zur Anwendung in einem
Verfahren zur chirurgischen oder therapeutischen Behandlung des menschlichen oder tierischen
Kцrpers, insbesondere zur Verhьtung und Behandlung von Dekubitus.
13. Substanz nach wenigstens einem der vorhergehenden Ansprьche,
dadurch gekennzeichnet, dass die Substanz als Lotion verabreicht wird.
14. Verwendung einer Substanz, enthaltend einen Trдgerstoff, ein Niaouli-Цl, ein Grapefruit
und/oder Lemonengras-Цl, einen Emulgator und ein Provitamin, zur Verhьtung und Behandlung von
Dekubitus.
248/1651
51. EP0908460 - 14.04.1999
A PROCESS FOR THE SIMULTANEOUS PRODUCTION OF ARTEMISININ AND ESSENTIAL OIL
FROM THE PLANT ARTEMISIA ANNUA
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP0908460
Inventor(s):
JAIN DHARAM CHAND (IN); TANDON SUDEEP (IN); KUMAR SUSHIL (IN);
BHAKUNI RAJENDRA SINGH (IN); BHATTACHARYA ASISH KUMAR (IN); KAHOL ATUL PRAKASH
(IN); SHARMA RAM PRAKASH (IN); SIDDIQUE MOHAMMED SHAFIQUE (IN)
Applicant(s):
COUNCIL SCIENT IND RES (IN)
IP Class 4 Digits: A61K; C11B; C07D
IP Class:
C11B9/02; C07D493/20; A61K31/365
E Class: C11B9/02B; C11B9/02E; C07D493/20+323D+321D+311B
Application Number:
EP19970402349 (19971006)
Priority Number: EP19970402349 (19971006)
Family: EP0908460
Cited Document(s):
US4952603
Abstract:
THE PRESENT INVENTION RELATES TO A NOVEL PROCESS FOR THE SIMULTANEOUS
PRODUCTION OF ESSENTIAL OIL AND ARTEMISINIC ACID OPTIONALLY CONVERTED INTO
ARTEMISININ, FROM THE PLANT ARTEMISIA ANNUA, COMPRISING THE FOLLOWING STEPS: A)
EXTRACTING SAID PLANT WITH A NON POLAR ORGANIC SOLVENT, THEREBY OBTAINING A
NON POLAR ORGANIC EXTRACT; B) PARTITIONING THE NON POLAR ORGANIC EXTRACT
BETWEEN AN ORGANIC PHASE AND AN AQUEOUS PHASE; C) EVAPORATING THE ORGANIC
PHASE SUBSTANTIALLY TO DRYNESS THEREBY OBTAINING AN ORGANIC PHASE RESIDUE,
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AND PERFORMING A HYDRO-DISTILLATION OF THE RESIDUE PREFERABLY ADMIXED WITH THE
PLANT MARC YIELDING SAID ESSENTIAL OIL D) PURIFYING THE AQUEOUS PHASE TO YIELD
ARTEMISINIC ACID; AND E) OPTIONALLY CONVERTING ARTEMISINIC ACID INTO ARTEMISININ.
THE PRESENT INVENTION ALSO RELATES BOTH TO THE USE OF ARTEMISININ OBTAINED FROM
SAID PROCESS AS AN ANTI-MALARIAL DRUG, AS WELL AS THE USE OF THE ESSENTIAL OIL
PRODUCED FROM THE PROCESS IN PERFUMERY, COSMETICS, AND
AROMATHERAPY.Description:
FIELD OF THE INVENTION
[0001] The present invention relates to a process for the simultaneous production of essential oil
and artemisinin from the plant Artemisia annua. More particularly, the invention is related to a
process for the production of essential oil and artemisinin and conversion of artemisinic acid into
artemisinin.
BACKGROUND OF THE INVENTION
[0002] Artemisia annua L. (Asteraceae) is a herb of Asiatic and Eastern European origin that has
been also naturalised in USA. This species is receiving considerable attention because of the
antimalarial activity of artemisinin of formula (1) shown in the accompanying drawings, a
sesquiterpene lactone endoperoxide which is present in its aerial parts. In clinical trials, mainly
performed in southeast Asia, artemisinin and a series of semi-synthetic derivatives have been proved
to be effective against Plasmodium parasites with resistance to the commonly used antimalarial
drugs. Now, efforts are being made to make these drugs cheaply available worldwide. In addition, A.
annua is valued for its essential oil which has characteristic sweet aroma. Its application in perfumery,
cosmetics, aromatherapy and as an antimicrobial, dermatological, fungicidal agents may provide an
additional market for essential oil.
250/1651
[0003] Artemisinic acid of formula (2) shown in the accompanying drawings is the biosynthetic
precursor of artemisinin, which are generally present in greater quantity than artemisinin in A. annua
plant. Artemisinic acid can be converted into artemisinin in good yield, thereby artemisinin amount
obtained directly from the plant is increased 3-4 folds.
PRIOR ART REFERENCES OF THE INVENTION
[0004] So far, no prior art literature has provided a method for the simultaneous isolation of
artemisinin and essential oil from A. annua plant without destroying any of them. At present, the herb
A. annua is processed for obtaining the essential oil by hydrodistillation method (Woerdenbag, H.J.;
Pras, N; Chen, N.G., Bang Bui-Thi; Bos, R., Uden Wim Van; Pham Van Y; Boi, N.V; Batterman, S. and
Lugt. C. (1994), Artemisinin related sesquiterpenes and essential oil in Artemisia annua, during
vegetation period in Vietnam, Planta Medica, 60, 272-75). In this process, the fresh herb and water
are heated in Clevenger apparatus at 100 DEG C for 3-4 hrs. The steam distillate is condensed and
essential oil is collected but in this process artemisinin gets destroyed. As artemisinin is a thermally
labile compound, it gets decomposed during hydrodistillation.
[0005] In another process, to isolate artemisinin and other biogentic precursors, the dried plant
material is extracted with non polar solvent (hexane), partitioning the hexane extract between hexane
and acetonitrile, following by chromatographying the acetonitrile phase over silica gel, elution with
solvent afforded different fractions, which on concentration and crystallization yielded artemisinin,
artemisinic acid, arteannuin B, but no essential oil is recovered in this process. Klayman, D.L.; Lin,
A.J. Acton, N; Scovill, J.P.; Hoch, J.M.; Michous, W.K.; Theoharidis, A.D. and Dobek, A.S. J. Nat.
Prods. 47, (1984) 715. Another disadvantage in the above process is that the artemisinic acid being
predominant, it tends to elute with artemisinin, thus affecting the purity of the desired compound.
[0006] An improved method for the isolation of artemisine acid from A.annua plant (Vonwiller, S.C,
Hayne, R.K, King, G. and Wang, H. Planta medica 59, 562-563 (1993) was reported. In this process,
methanolic extract of A.annua were partitioned between water and ether solvent. Ether residue was
treated with base to separate artemisinic acid fraction from artemisinin. The basic solution was
neutralized and further methylation of residue stirring with acid. After methylation the same base
extraction process was repeated to obtain artemisinic acid. The residue left after base extraction was
chromatographed to obtain artemisinin which afforded 57 % of yield. In this process, total extract
251/1651
was treated with base which destroyed some amount of artemisinin. The solvent namely ether used
in the process is low boiling and highly inflammable.
[0007] Artemisinic acid is the most abundant metabolite of A.annua and its conversion to
artemisinin would increase the yield of artemisinin. Roth. R.J and Acton, N., J.Chem.Edu 68,612
(1991) have prepared dihydroartemisinic acid by using excess quantity of NaBH4 and NiCl2.6H2O in
methanol. Dihydroartemisinic acid was photo-oxidised at (-) 78 DEG C in dichloro methane or at 0
DEG C in solvent acetone with methylene blue as photosynthesiser and oxygen was passed through
the solution with irradiating with high intensity lamp. The solution was evaporated and the residue
was taken up in ether and filtered the solution to remove dye. The solvent was evaporated, residue
was re-dissolved in pet. ether, containing a few drops of trifluoroacetic acid and the photolysate was
left for four days to afford 17-30% artemisinin. In this process, photo oxidation was carried out at low
temperature and also used number of solvents, chemical and process steps.
SUMMARY OF THE INVENTION
[0008] The present invention provides a simple and efficient process for the simultaneous
production of artemisinin and essential oil from the plant A. annua and also a method for better
recovery of artemisinic acid and artemisinin without the use of chromatography and finally conversion
of artemisinic acid into artemisinin.
NOVELTY OF THE INVENTION
1. In the prior art, essential oil is obtained by hydro-distillation of fresh/dried plant material in which
artemisinin gets destroyed and the essential oil is obtained after 3 hrs. contact with steam, whereas
in this present invention, the dried plant material is extracted with n-hexane and the extract is
partitioned with aqueous acetonitrile. In this step, fatty material is seperated from artemisinin, so that
purification and recovery of artemisinin is improved as well as essential oil is obtained by
hydrodistillation of marc and hexane residue obtained in the partition step in which no artemisinin is
present. Therefore, in this process, no loss of artemisinin takes place. For the first time, 50% essential
252/1651
oil is obtained from the marc of the plant. The quality of the oil is better and less time is required for
hydrodistillation. For the first time, the applicants have achieved the simultaneous production of
artemisinin and essential oil without destroying either of them.
2. In the previous process artemisinic acid was seperated from aqueous acetonitrile phase by the
treatment with sodiumcarbonate of chromatography. In this process, artemisinin present also gets
decomposed and only 57% artemisinin was recovered. But in the present invention, artemisinin acid
will be seperated from artemisinin before treatment with base, so that both the compounds are
recovered in 90% yield.
3. The conversion of artemisinic acid (obtained from A.annua) into artemisinin results in the best
utilization of the compounds obtained during the process as well as increases the yield of artemisinin
from the plant. As the synthesis of artemisinin is not economically viable plant remains the sole
source for its large scale production. In the present improved process, conversion takes place in
only two steps instead of the three steps as used in the prior art. The present process does not use
any catalyst, photosynthesiser and oxygen. The reaction takes place at room temperature and work
up of the reaction is very simple to obtain artemisinin.
SUMMARY OF THE INVENTION
[0010] According to a first aspect, the present invention relates to a process for the simultaneous
production of essential oil and artemisinic acid optionally converted into artemisinin, from the plant
Artemisia annua, comprising the following steps:
a) extracting said plant with a non polar organic solvent, thereby obtaining a non polar organic
extract;
b) partitioning the non polar organic extract between an organic phase and an aqueous phase;
c) evaporating the organic phase substantially to dryness thereby obtaining an organic phase
residue, and performing a hydrodistillation of the residue preferably admixed with the plant marc
yielding said essential oil
d) purifying the aqueous phase to yield artemisinic acid; and
e) optionally converting artemisinic acid into artemisinin.
253/1651
[0011] According to a second aspect, the present invention relates to a process which consists of
the following steps:
i) drying and powdering A. annua plant,
ii) extracting said powdered A. annua plant with hexane,
iii) reducing the hexane extract obtained from step ii) above to 5-20% of its original volume under
vacuum;
iv) partitioning the hexane extract between hexane and acetonitrile water mixture;
v) evaporation of the hexane phase obtained in step iv) to dryness,
vi) hydro-distillation of the hexane residue obtained from step v) and the marc (extracted plant
material) to yield essential oil,
vii) removal of water from the aqueous acetonitrile phase obtained in step iv),
viii) further fractionation of the resultant acetonitrile phase obtained in step vii) between a hexanebenzene mixture to obtain hexane-benzene phase and acetonitrile phase,
ix) treating the hexane-benzene phase obtained in step viii) with a base followed by neutralisation,
extraction with chloroform, drying and crystallisation to obtain artemisinic acid,
x) converting artemisinic acid obtained in step ix) into artemisinin by reduction and photo -oxidation,
xi) chromatographing the evaporated acetonitrile residue obtained from step viii) over silica gel
with hexane, thereby providing fractions containing artemisinin, and
xii) evaporating the different fractions obtained from step xi) and crystallisation of said fractions
containing artemisinin obtained from step xi) and thereby producing substantially pure artemisinin.
[0012] According to a third aspect, the present invention relates to the use of artemisinin obtained
from the process according to the invention as an antimalarial drug. Furthermore, in a fourth aspect,
the present invention relates to the use of the essential oil produced from the process according to
the invention in perfumery, cosmetics, and aromatherapy.
[0013] Advantageous embodiments of all these aspects of the present invention are set forth in the
description that follows, together with the sub-claims.
DETAILED DESCRIPTION OF THE INVENTION
254/1651
[0014] In accordance with the method of the invention, employing n-hexane solvent for extraction
of the plant in which complete extraction of artemisinin and other bio-precursors and 50% of
essential oil. The step of partitioning separates the fatty material from other products containing
artemisinin, whereas defatting of crude extract with n-hexane, alcohol etc., results in the loss of
artemisinin and filteration of fat is a difficult operation which is avoided in this process. In the previous
process, the hydrodistillation of plant material to obtain essential oil, due to high temperature
artemisinin gets destroyed during operations but here the applicants have separated the artemisinin
fraction from fatty material which on hydrodistillation yield essential oil. In this process, the remaining
essential oil in plant which is not extracted during hexane extraction which is to be identified and
recovered from the extracted plant material (Marc) by hydrodistillation. The hydrodistillation of marc
and concentrated hexane residue took less time and size of distillation unit is drastically reduced
which is required during fresh plant extraction. During drying, the structure changes of the cells of
plant material favour the diffusion of the oil components out of them.
[0015] The partitioning step in liquid-liquid extraction done in Karr type column at particular flow
rate and stirring, transfer the artemisinin and two major sesquiterpene, in the acetonitrile phase (polar
solvent ) with concomitant reduction of in the amount of extract, i.e. of the order of 20 - 24 % of the
original hexane extract in the single operation.
[0016] The acetonitrile phase rich in artemisinin acid only 10% of the acid isolated by crystallization
before chromatography. Here in this process, complete extraction of artmisinic acid by partitioning
between acetonitrile and hexane-benzene mixture, which reduced the bulkness of the acetonitrile
extract further by 50%. Using the method of the present invention, the second partitioning step which
remove artemisinic acid prior to elution at artemisinin without chromatography, enhancing the
purification of artemisinin, less consumption of silica gel, time and solvent and economize the cost of
production of the drug-artemisinin. In the Vonwiller process, artemisinic acid was isolated from the
ether extract by treatment with a base. In the ether extract, artemisinin which was also present get
decomposed during the base extraction. Here the applicants have separated the artemisinic acid
fraction from artemisinin.
[0017] In the chromatography step of the invention, ratio of (1:3) (solute to adsorbent) was
discovered to yield excellent results. In the known process, a ratio of 1:10 has been required. In the
solvent system of the invention, n-hexane was found to be quite effective rather than 10-20% ethyl
acetate in n-hexane mixture. The silica gel used as a packing material in the example here is silica
gel-H.(Mesh size - 200). The elution of compounds done under reduced pressure. In this way elution
255/1651
of artemisinin by n-hexane rather than 15% ethyl acetate-hexane mixture, artemisinin B was
recovered by 5% ethyl acetate hexane mixture. By way of chromatography step of the process of
elution, artemisinin was obtained from the oily greenish yellow fraction eluted with hexane and
purification of artemisinin was carried by crystallization from ethyl acetate-hexane (1:4). In
accordance with the description herein used, solvent, silica gel and time for chromatography
reduced drastically.
[0018] Accordingly, the present invention provides a novel process for the simultaneous production
of essential oil and artemisinin from the Artemisia annua, said process comprising (i) drying and
powedering A. annua plant ; (ii) extracting the said powdered herb of A. annua with hexane : (iii)
reducing the hexane extract obtained from step (ii) above to 5-20% of its original volume under
vacuum : (iv) partitioning the hexane extract between hexane and acetonitrile water mixture ; (v)
evaporation of the hexane phase obtained in step (iv) to dryness ; (iv) hydrodistillation of hexane
residue obtained from the step (v) and Marc (extracted plant material) to yield essential oil ; (vii)
removal of water from aqueous acetonitrile phase obtained from step (iv); (viii) further fractionation of
resultant acetonitrile phase after removal of water as obtained from step (vii) between hexanebenzene mixture to obtain hexane-benzene extract and acetonitrile phase ; (ix) treating hexanebenzene fraction obtained from step (viii) with a base followed by neutralization, extraction with
chloroform, drying and crystallisation to obtain artemisinic acid ; (x) converting artemisinic acid
obtained from step (ix) into artemisinin by reduction and photo oxidation ; (xi) chromatographying of
the evaporating acetonitrile residue obtained from step (viii) over silica gel with hexane ; (xii)
evaporation of the different fractions obtained from step(xi) and crystallization of the said fractions
containing artemisinin obtained from step (xi) and thereby producing substantially pure artemisinin.
[0019] The dried parts of the plant used for the extraction can be selected from any part of the
plant, preferably leaves, influroscence and small stems and the hexane extract of the A. annua as
used in step (i) is reduced to 10 % of its original volume under vacuum. Preferably, the partitioning
between hexane and aqueous acetonitrile phase is done in the ratio of 2:3 in liquid-liquid extraction
column and the aqueous acetonitrile mixture used is in the ratio of 1:1 to 1:5.
[0020] In the present process, the single extraction step (ii) is carried out between two phases for 3
hrs. and the hydrodistillation of Marc (extracted plant material) in step (i) and residue obtained from
(iii) yield essential oil upto 2.0 hrs.
256/1651
[0021] Also, in the present process, further partitioning between acetonitrile and hexane-benzene
mixture after removal of water is done to isolate artemisinic acid and 10-30 % benzene used in
hexane solvent was used for the extraction of artemisinic acid.
[0022] Preferably, extraction of artemisinic acid is carried out where hexane-benzene mixture is
evaporated, extracted with 5% of sodium carbonate solution and the basic solution is neutralized
with 5% HCl solution, extracting with chloroform, drying the solvent and crystallization with ethyl
acetate yielding artemisinic acid.
[0023] One embodiment of the invention provides a process for the conversion of artemisinic acid
into artemisinin employing steps such as reduction and photo oxidation and the reduction is carried
out by the following steps comprising (i) dissolving artemisinic acid and NiCl2.6H2O in dry methanol ;
(ii) adding sodium borohydride to the resultant solution at 0 DEG C over a 2 hr. period ; (iii)
neutralising the solution obtained in step (ii) with 5% aqueous HCl solution and (iv) isolating and
crystallizing the dihydro artemisinic acid in ethyl acetate to obtain pure dihydro artemisinic acid.
However, the step of photo oxidation is carried out by comprising (i) dissolving the
dihydroartemisinic acid in the solvent dichloromethane - ethyl acetate ; (ii) oxidising the solution
obtained in the step (i) in the presence of fluorescent light (40W) daily for two hours upto 8 days ; (iii)
concentrating the solution obtained in step (ii) and recrystallizing the residue in hexane to isolate
artemisinin.
[0024] Preferably, in the present process, the chromatographic step is carried out in SiO2column
comprising a solute having adsorbent ratio 1:3. The elution with n-hexane solvent is being done
under vacuum at 100-150 mm Hg absolute pressure and the chromatographic adsorbent used is
Silica gel H with mesh size 200.
[0025] The process of invention is illustrated by the following examples which should not be
construed to limit the scope of the present invention.
[0026] The following examples also illustrates the specific embodiments of the method of the
invention.
Example 1
257/1651
[0027] Dried powdered herb of A. annua (40 kg) was percolated with hexane ( 60 - 80 DEG C) ( 6 x
200 liter) in a soxhlet for 8 hrs. The extracted solvent was reduced to 20 liter. The non polar phase
(hexane extract) was partitioned with aqueous acetonitrile phase (1:5) presaturated each other in the
liquid-liquid extraction (Karr type) column. After 3 hrs. two phases were separated. The aqueous
acetonitrile phase was back washed using 10% of its volume with presaturated hexane (2.0 litre).
Evaporation of non polar phase provided (2.20kg) residue. The residue was boiled in Clevenger
apparatus with 10 litre water for 1.5 hrs. which yielded the essential oil (80ml). The marc (extracted
plant material) (40kg) was hydrodistilled in a distillation unit, which yield essential oil (100 ml) in 1 hr.
The water from aqueous acetonitrile phase was removed by adding 1 kg sodium chloride. The
acetonitrile solvent (25.0 litre) was further partitioned between acetonitrile extract and 10% benzenehexane mixture in the same karr type column. After separation of two phases, evaporated the
benzene-hexane mixture yielded (200gm) of residue. The residue (200gm) was dissolved in
chloroform (400 ml) and extracted with 5% Na2 CO3, solution (3 x 500 ml). Basic solution was
neutrilized with 10% HCI solution (400 ml). The neutral solution was extracted with chloroform,
concentrated and crystallization with ehtylacetate yielded artemisinic acid (71.8 gm). The acetonitrile
phase after concentration provide a residue (300 gm) which was filtered over silica gel (900 gm)
under vacuum at 100 - 150 mm Hg absolute pressure. Artemisinin was obtained from the viscous
greenish yellow fraction elutes with n-hexane. Purification of artemisinin was carried by
recrystallization with ethyl acetate/hexane (1:4) to yield artemisinin (18 gm) Arteannuin B was
obtained from the fraction eluted with 5% ethyl acetate in hexane. Evaporation of the fraction and
crystallization yielded arteannuin B (36.5kg).
[0028] The above procedure was repeated two times on the same scale and consistently provided
the same yield of artemisinin and other constituents.
Example 2
[0029] The process followed as in example 1 in which the organic phase (20 litre) was partitioned
with aqueous acetonitrile phase ( 1:5, 30 litre) in same extraction column for the same period of time.
The acetonitrile phase after removal of water was dried over anhydrous sodiumsulphate and
concentrated under reduced pressure to yield a residue (0.55 kg). This residue was
chromatographed over silica gel (2.5 kg) and eluted with different ratio of ethyl acetate-hexane.
258/1651
Artemisinin was obtained from column fractions eluted with 8% ethyl acetate-hexane. Evaporation
and crystallization with hexane ethyl acetate mixture afforded pure artemisinin (18.0 gm). fraction
eluted from 5% ethyl acetate-hexane yielded artemisinic acid (70.6gm) where as 12% ethyl acetate
in hexane fraction afforded arteannuin B (35.8 gm).
Example 3
[0030] The process of extraction of A. annua was followed as in example 1 in which the hexane
phase (20 litre) was partitioned with aqueous acetonitrile phase (1:3, 30 litre) in same extraction
column for the same period of time and speed. After partitioning the hexane phase was concentrated
to yield (1.82 kg)residue which on hydrodistillation yielded essential oil (50 ml). The acetonitrile
extract was concentrated after removal of water and yielded viscous mass (0.8 kg). This viscous
mass was chromatographed over silica gel ( 4.0 kg ) and eluted with different ratio of solvent ethyl
acetate-hexane. Artemisinin was obtained from column fractions eluted with 10% ethyl acetatehexane. Evaporation and crystallisation with hexane ethyl acetate mixture afforded pure artemisinin
(17.0 gm).
Example 4
[0031] Dried herb of A.annua (40.0kg) was extracted with n-hexane in a soxhlet apparatus. The
extracted solvent was reduced to 20 litre. The hexane soluble fraction (10 litre) was partitioned with
aqueous acetonitrile phase (1:1. 30 litre) in same extraction column. The hexane soluble fraction
obtained after partitioning was evaporated and residue (1.70 kg) was boiled in Clevenger apparatus
with 8 liter water for 3 hrs. which yield the essential oil (40ml). The acetonitrile phase was
concentrated and yielded viscous mass (1.24kg) which on chromatograph on silica gel as per
example 3 yielded pure artemisinin (16.2gm).
Example 5
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[0032] Artemisinic acid is isolated from A. annua extract as in example 1 was used for conversion
into artemisinin. Artemisinic acid (100 mg) was dissolved in 100 ml methanol containing 150 mg
NiCl2.6H2O, 300 mg of NaBH4 powder was added in small portions over 2 hr. period to a stirred and
cooled solution. After the reaction was completed excess reducing agent was destroyed by adding
20 ml of 5% aqueous HCl. The mixture was filtered to remove the insoluble impurities and then the
aqueous methanolic solution was extracted with ether which was washed with water, dried and
concentrated to afford 105 mg of crude dihydroartemisinic acid. Dihydroartemisinic acid (100 mg)
was dissolved in dichloromethane-ethyl acetate (7:3, 20 ml), and the reaction mixture was left for 8
days at room temperature and irradiated with fluorescent light (tubelight) (40W) for a period of 2 hrs.
per day. Solvent was removed under vacuum and the residue was recrystallized with n-hexane to
afford artemisinin(25 %). The new process of production of essential oil and artemisinin, the subject
matter of this patent, offered a number of advantages such as :
1. The process for the dual production of artemisinin and essential oil (80 %) from A.annua has
been developed for the first time.
2. Consumption of silica gel has decreased due to reduction of charging material upto 10% of its
original hexane extract and ratio of adsorbent to solute is (1:3).
3. The partitioning step between n-hexane and aqueous acetonitrile phase allowed the selective
transfer of artemisinin and other sesquiterpenes into polar phase leaving non polar constituents in
hexane solvent which results in a better method for the removal of large quantity of fat and other
impurities, whereas removal of fats is difficult operation.
4. Hydrodistillation of extracted plant and hexane residue is a better alternative to recover major
portion of the essential oil than hydrodistillation from fresh herb where artemisinin gets destroyed.
5. In this process, after recovery of essential oil from hexane residue, the applicants also obtained
major fatty acids material which on further purification yield free fatty acids.
6. Isolation of artemisinic acid without chromatography, as by product, can be converted into
artemisinin which will increase the overall yield of the artemisinin from the plant by 2-3 folds.
7. Conversion of artemisnic acid into atemisinin in two simple steps without using catalyst, dye. few
solvents and oxygen. The present reaction takes place at room temperature.
8. The process is highly efficient and economical as most of the solvents and adsorbents used in
the process are being recovered and reused.
9. All these advantages are significant economic value for large scale production of antimalarial
drug artemisinin.
Claims:
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1. A process for the simultaneous production of essential oil and artemisinic acid optionally
converted into artemisinin, from the plant Artemisia annua, comprising the following steps:
a) extracting said plant with a non polar organic solvent, thereby obtaining a non polar organic
extract;
b) partitioning the non polar organic extract between an organic phase and an aqueous phase;
c) evaporating the organic phase substantially to dryness thereby obtaining an organic phase
residue, and performing a hydrodistillation of the residue preferably admixed with the plant marc
yielding said essential oil
d) purifying the aqueous phase to yield artemisinic acid; and
e) optionally converting artmisinic acid into artemisinin.
2. The process of claim 1 wherein said non polar organic solvent comprises hexane.
3. The process according to claims 1 or 2, wherein said partitioning step of the non-polar organic
extract is performed by adding an acetonitrile/water mixture to said non polar organic extract solvent
which is preferably hexane.
4. The process according to any one of claims 1 to 3 wherein, prior to said partitioning step, said non
polar organic extract is evaporated to 5-20% of its original volume, preferably under vacuum.
5. The process according to any one of claims 1 to 4, wherein said purification of the aqueous phase
comprises the removal of water and further fractionation of resultant acetonitrile phase between a
hexane-benzene mixture to obtain hexane-benzene phase and acetonitrile phase.
6. The process according to claim 5 wherein said hexane-benzene phase is neutralised with a base,
extracted with chloroform thereby giving a chloroform phase, said chloroform phase is dried, and
artemisinic acid is crystallised therefrom.
7. The process according to claim 6, wherein artemisinic acid is converted into artemisinin by
reduction and photo-oxidation.
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8. The process according to claim 5 wherein said acetonitrile phase is chromatographed over silica
gel eluting with hexane and artemisinic acid or preferably artemisinin is recovered therefrom.
9. The process according to any one of claims 1 to 8, wherein said non polar organic solvent
extraction of a) is performed on A. annua plant which has been dried and powdered.
10. A process for the simultaneous production of essential oil and artemisinin from the Artemisia
annua, said process comprising:
i) drying and powdering A. annua plant,
ii) extracting said powdered A. annua plant with hexane,
iii) reducing the hexane extract obtained from step ii) above to 5-20% of its original volume under
vacuum;
iv) partitioning the hexane extract between hexane and acetonitrile water mixture;
v) evaporation of the hexane phase obtained in step iv) to dryness,
vi) hydro-distillation of the hexane residue obtained from step v) and the marc (extracted plant
material) to yield essential oil,
vii) removal of water from the aqueous acetonitrile phase obtained in step iv),
viii) further fractionation of the resultant acetonitrile phase obtained in step vii) between a hexanebenzene mixture to obtain hexane-benzene phase and acetonitrile phase,
ix) treating the hexane-benzene phase obtained in step viii) with a base followed by neutralisation,
extraction with chloroform, drying and crystallisation to obtain artemisinic acid,
x) converting artemisinic acid obtained in step ix) into artemisinin by reduction and photo -oxidation,
xi) chromatographing the evaporated acetonitrile residue obtained from step viii) over silica gel
with hexane, thereby providing fractions containing artemisinin, and
xii) evaporating the different fractions obtained from step xi) and crystallisation of said fractions
containing artemisinin obtained from step xi) and thereby producing substantially pure artemisinin.
11. The process according to any one of claims 1 to 10 wherein said Artemisia. annua plant used for
the extraction can be any part of the plant, preferably the leaves, inflorescence and small stems.
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12. The process according to any one of claims 1 to 11 wherein the partitioning the non polar organic
extract between said organic phase and said aqueous phase is done in the ratio of 2:3 in a liquidliquid extraction column.
13. The process according to any one of claims 3 to 12 wherein said aqueous phase is an
acetonitrile water mixture in the ratio of 1:1 to 1:5.
14. The process according to any one of claims 1 to 13 wherein partitioning step b) is carried out
between said organic phase and said aqueous phase for 3 hours.
15. The process according to any one of claims 1 to 14 wherein said hydrodistillation of the residue is
carried out for a period of time ranging from 30 minutes to 120 minutes.
16. The process according to any one of claims 5 to 15 wherein the benzene used in said hexanebenzene mixture used as solvent is used at a rate of between 10-30%.
17. The process according to any one of claims 6 to 16 wherein said base is 5% sodium carbonate
solution.
18. The process according to any one of claims 7 to 17 wherein said reduction is carried out by the
following steps comprising :
i) dissolving artemisinic acid and NiCl2.6H2O in dry methanol;
ii) adding sodium borohydride to the resultant solution at 0 DEG C over a 2 hour period;
iii) neutralising the solution obtained in step ii) with 5% aqueous HCl solution, and
iv) isolating and crystallising the dihydro artemisinic acid in ethyl acetate to obtain pure dihydro
artemisinic acid.
19. The process according to any one of claims 7 to 18 wherein said photo-oxidation comprises:
i) dissolving the dihydro artemisinic acid in a dichloromethane-ethyl acetate mixture;
ii) oxidising the solution obtained in the step i) in the presence of fluorescent light daily for two
hours up to 8 days;
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iii) concentrating the solution obtained in step ii) and recrystallising the residue in hexane to isolate
artemisinin.
20. The process according to any one of claims 8 to 19 wherein said chromatographic step is carried
out on a silica gel column which comprises a solute having an adsorbent ratio of 1:3.
21. The process according to any one of claims 8 to 20 wherein the elution with hexane solvent in
said chromatographic step is done under vacuum of 100-150 mm Hg absolute pressure.
22. The process according to any one of claims 8 to 21 wherein the chromatographic adsorbent
used in said chromatographic step is silica gel H with a mesh size of about 200.
23. The use of artemisinin obtained from the process according to any one of claims 1 to 22 as an
anti-malarial drug.
24. The use of essential oil produced from the process according to any one of claims 1 to 22 in
perfumery, cosmetics, and aromatherapy.
264/1651
52. EP1085915 - 16.12.1999
DISPOSABLE ABSORBENT ARTICLE CONTAINING AN ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP1085915
Inventor(s):
TRAMONTANA PRISCILLA M (--)
Applicant(s):
MCNEIL PPC INC (US)
IP Class 4 Digits: A61L
IP Class:
A61L15/46; A61L15/18
E Class: A61F13/15H8; A61F13/15M; A61L15/18; A61L15/46
Application Number:
WO1999US12307 (19990603)
Priority Number: US19980088962P (19980611)
Family: EP1085915
Equivalent:
AU4673999; BR9912187; CA2334673; ZA200007372
Cited Document(s):
WO9738738; WO9725106; DE4136540; US3688985; DE3331573;
WO8905661; CN1083145; HU212933; HU57601
Abstract:
THE INVENTION RELATES TO DISPOSABLE ABSORBENT ARTICLES CONTAINING AN ADDITIVE
TO CONTROL ODORS ASSOCIATED WITH BODILY FLUIDS. THE INVENTION IS PARTICULARLY
USEFUL IN ARTICLES USED TO MANAGE URINE AND MENSTRUAL FLUIDS. THE SINGLE
ADDITIVE PROVIDES BOTH A PLEASANT AROMA AND ANTIMICROBIAL ACTIVITY.Description:
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DISPOSABLE ABSORBENT ARTICLE CONTAINING
AN ESSENTIAL OIL
FIELD OF THE INVENTION
The present invention relates to a disposable absorbent article containing a fragrant emitting and
microbe inhibiting additive, and methods for making the same.
The additives are essential oils and/or derivatives thereof.
BACKGROUND OF THE INVENTION
There are two common forms of disposable articles that are designed to absorb menstrual fluids
discharged from a female's cervix. The first article is intended to be wholly inserted into the vaginal
canal, and positioned near or against the cervical os.
These articles are commonly referred to as catemenial tampons, or simply tampons.
Some of the disadvantages related to tampons are the following: they can be attributed to excessive
vaginal drying, they have been associated with toxic shock syndrome, they can be uncomfortable to
insert and remove, especially on light flow days, and they have limited absorbing capacity, due to
the regulations set by the U. S. Food and
Drug Administration.
The second widely known and used article for collecting menstrual fluids is the sanitary napkin. This
product is designed to be worn external to the vagina.
Sanitary napkins can also be used to absorb urine, due to the size and positioning against the
perineum. The product can be attached to the crotch of undergarments, attached directly to the
vulvar region with body adhesives, and also worn partially or totally between the labia minora and
majora. Many consumers choose to wear external absorbent articles because of their concern of
toxic shock syndrome, they have difficulty inserting and removing tampons, they have difficulty
wearing tampons, and they have a need for higher absorbing capacity than that available from
tampons. As with tampons however, there are disadvantages that have been voiced by consumers
who rely on external absorbing articles for their fluid management needs.
266/1651
One perceived disadvantage of external sanitary napkins is their association with odors. Menstrual
fluid contains a variety of substances including proteins and lipids. Microbial action on proteins has
been recognized as a source of malodor.
Urine is another fluid that can be absorbed by sanitary protection products, and microbial activity
can form ammonia from urea in excreted urine. Consumers complain of not feeling"fresh"during their
period, and hence seek out products that claim to control odor issues.
There have been a number of technologies developed for controlling odors associated with bodily
fluids; particularly those attributed to perspiration, menstrual fluid degradation products, urine
degradation products, and miscellaneous urine odors.
Nearly all of the technologies can be placed into three main subcategories. The first is the use of
added materials to absorb or adsorb volatile odors in an effort to restrict their release to the
environment surrounding the consumer. Materials or compositions that adsorb and/or absorb volatile
odors include sodium bicarbonate, sodium salts or ethylenediamine tetraacetic acid (EDTA),
activated carbon, zeolites, and mixtures of sodium bicarbonate, EDTA, and activated carbon. These
approaches are disclosed in
US Patent Numbers 4,237,591 and 5,306,487. The second is the use of masking materials, such as
perfumes, and the third is the use of substances to inhibit the production of bodily fluid degradation
products. US Patent Number 5,733,272 discloses absorbent articles containing compositions of
moisture-activated encapsulated perfumes and odor-controlling agents, including anti-microbial
compounds.
The discussion thus far has highlighted technologies that are believed to remedy either malodors
directly by inhibiting microbial activity, thereby decreasing the level of urine and menses degradation
products, or indirectly by suppressing or overcoming the odors as they exist.
SUMMARY OF THE INVENTION
The object of the present invention is to utilize a single additive in disposable absorbent articles to
both provide a pleasant aroma, and inhibit microbial growth.
The single additive is an essential oil, derivative, or variation therefrom.
267/1651
In accordance with one embodiment of the present invention, there has now been provided a
disposable absorbent article containing an essential oil in an amount effective to provide a pleasant
aroma and inhibit microbial growth.
In accordance with a second embodiment of the present invention there has been provided a
method of making a disposable absorbent article containing an essential oil in an amount effective to
provide a pleasant aroma and inhibit microbial growth comprising:
a) providing an absorbent material;
b) providing a liquid permeable material;
c) providing a liquid impermeable material;
d) encasing the absorbent material with the liquid permeable material
and liquid impermeable material; and
e) contacting at least one of the absorbent material, the liquid
permeable material, the liquid impermeable material, or a combination
thereof with an essential oil.
DETAILED DISCUSSION OF THE INVENTION
The present invention is directed to a disposable absorbent article containing one or more essential
oils. Essential oils are highly concentrated, volatile liquids originating from a single botanical source.
A typical essential oil is a complex mixture of alcohols, aldehydes, esters, ketones, oxides, phenols
and terpenes.
Essential oils can be extracted by steam distillation, and other techniques known in the art, from a
variety of plant components, including, but not limited to, roots, leaves, bark, flowers and pulp. The
majority of the oil-producing plants are represented by 90 species, and these are derived from about
30 different plant families.
The present invention provides an absorbent article containing one or more essential oils in an
amount effective to provide two functions: emit a pleasant aroma, and inhibit microbial growth.
Rosemary oil, clove oil, ginger oil, turmeric oil, chamomile oil, lemon grass oil, thyme oil, achillea oil,
thulasi oil, clary sage oil, cedar (hinoki) oil, and derivatives, variations, and mixtures thereof, are all
suitable for use as the essential oil. Synthetic forms of the oils described above can also be
employed in the present invention. The preferred essential oil is rosemary oil, which is commercially
available from Lorann Oils.
268/1651
Malodors attributed to bodily fluids are most likely the result of bacteria degrading components
residing in the bodily fluids. Bacteria can transform phospholipids into amines and fatty acids, and
urea in urine to ammonia. Rosemary oil, for example, is an effective inhibitor of a number of gram
positive and gram negative bacteria, such as, but not limited to Staphylococcus aureus, Eschericia
coli, and Pseudomonas aeruginosa. Further to its inhibiting affect on bacteria, rosemary oil also has
an inhibiting affect on a variety of fungi and yeast. Of particular interest to feminine hygiene,
rosemary oil has been seen to inhibit the growth of Candida albicans.
In addition to its antimicrobial activity, rosemary oil emits a pine-like, camphorous odor. Synergistic
odor control is thus achieved in that rosemary oil both inhibits the microbial growth that degrades
bodily fluid components and provides a pleasant aroma.
The effectiveness of an essential oil as a fragrance may be determined by gathering organoleptic
data from a panel presented with a series of absorbent article samples containing increasing
concentrations of essential oil. The samples are then evaluated in a variety of environments,
including but not limited to prior to wearing and during wearing. The panelists are asked a series of
questions relating to their perceptions of the effectiveness of essential oil, at various add-on amounts,
to provide an aroma.
Test methods for determining the amount of essential oil necessary to inhibit microbial growth
include the following: analytical methods employed to investigate microbial growth in the presence of
essential oil, and analytical/organoleptic methods employed to investigate the level of malodorous
degradation products generated by microbial activity on cervical and urethral discharge As used
herein, inhibition means substantially maintaining an existing microbe colony by the prevention of the
additional growth of microbes. Inhibition does not require the killing of existing microbes or a
reduction in size of the colony, although this is a possible result.
One test method that may be used to determine the microbial inhibition properties of essential oils is
the zone of inhibition test. Another useful test method is the Durham's Fusion test. Those skilled in the
art are familiar with other test methods in the microbiology community that can be used to determine
microbial inhibition as described in the present invention.
In general, the amount of essential oil used in the absorbent article is between about 0.1 and about
8 weight percent, more preferably between about 0.2 and about 4 weight percent, and most
preferably between about 0.5 and about 1.5 weight percent.
269/1651
Due to the relatively high volatility of essential oils, additional binder materials or mechanisms are
preferably employed to reduce the premature loss of the essential oil once it has been added to the
disposable absorbent article. (If compounding means are employed, then the level can be adjusted
to yield a similar range of add-on available at the surface after migration has occurred.)
The disposable absorbent article of the present invention can take a plurality of forms including, but
not limited to, sanitary napkins, tampons, diapers, surgical gowns, bedsheets, incontinence products,
and wipes. The present invention is particularly advantageous for articles designed for managing
cervical and urethral discharge. As used here, and throughout the text, sanitary napkin means any
feminine hygiene product worn external to the vagina.
Essential oils can be added to any of the elements used in manufacturing disposable absorbent
articles, during their individual manufacture or during their configuration into the article itself, or
added to the final product once constructed from the elements.
One method of incorporating essential oils into the articles is by compounding the essential oils with
a base polymer and then forming a film or fiber from the blend.
These films or fibers can be used to form the elements utilized in the manufacture of disposable
absorbent articles. Additives compounded into polymers, which then migrate at least partially to the
surfaces of the solidified materials, are commonly referred to as"blooming agents."Blooming agents
are known in the art to be useful in altering the surface of a material. A representative, non-limiting list
of uses of blooming agents, include making the surface more lubricious, protecting the polymer from
degradation, making the surface wettable, and making the surface releasable, as used in the
molding business. A benefit of compounding the essential oil additives with a base polymer, is
reducing the amount of additive lost, or lengthening the time elapsed before effective levels of
essential oils are diminished, because of the migration and total separation from the base polymer
that is required.
Another method of adding essential oils to materials used in disposable absorbent articles is to
apply the essential oils to a finished product, typically by a coating means. Simplicity and efficiency
are two benefits of using coating techniques. Coating means that can suitably be used in the present
invention include, but are not limited to dip, slot, spray, melt blown, control coat, and swirl spray.
270/1651
Sanitary napkins are commercially available in multiple sizes and shapes, and can vary according to
individual needs. Without limitation, the common names for the variety of externally worn sanitary
napkin products include pantyliners, full-size pads, and ultrathins. The majority of sanitary napkins
are either rectangular or hourglass shaped to fit in the crotch of undergarments. Most products are
attached directly to a user's undergarment, and contact the perineum intimately when the
undergarments are pulled up. Alternatively, sanitary napkins can be attached directly to the body
with body adhering adhesives, or held in place against the body from pressures exerted by the labia.
Many of the incremental changes that have evolved in the development of new sanitary napkins are
targeted to improve protection of the products. Compressive forces acting on the pads from body
position and activity, can distort the pad in proximity of the vaginal opening, resulting in a limited
area for the fluid to contact the product when exiting the vaginal opening. Therefore, lateral
extensions, commonly referred to as wings, accompany many products in an effort to reduce
leakage that can occur due to the reduced area. The lateral extensions also act to keep the sanitary
napkin in the location it was originally placed. Lateral extensions can be both flexible and stiff, can
contain adhesive or not, can be wrapped around the underside of undergarments, can attach to the
underside of undergarments, or can be held against or attached to the body. Sanitary napkins
typically contain two lateral extensions, but one of ordinary skill in the art, would recognize that more
than two lateral extensions could be used to enhance a product's performance.
Sanitary napkins typically are packaged loosely into a primary package, such as a box or bag, and
can have secondary packaging that allows the consumer to transport individual products and protect
them from any unwanted environmental affects. The individually packaged napkins are often times
folded and then wrapped to facilitate the ease and discretion of transporting the products. Products
and methods of individually folded and wrapped sanitary products are disclosed in US
Patent Numbers 4,556,146 and 4,917,675; both of which are herein incorporated by reference.
Sanitary napkins are typically made from a number of separate elements. A simplistic configuration
would include the following elements: a liquid permeable material representing the body-contacting
surface, a liquid impermeable material representing a barrier as the opposite surface, and an
absorbent material or combination of absorbent materials contained between the two surface
defining materials. Adhesives can be added, with or without the presence of heat and pressure, to
adhere the separate elements to one another. Adhesives can also be applied to the outer surfaces of
the product for either attaching to undergarments, or directly to the body. A transfer layer or material
may optionally be placed between the liquid permeable material and the absorbent material (s) to
271/1651
improve the transfer of fluid into the absorbent materials. The foregoing statements are intended to
describe the basic elements contained within the majority of sanitary napkins commercially available;
however, the present invention is not limited to disposable absorbent articles comprising the
disclosed elements. The art is replete with many additional technologies aimed towards improving
the performance and comfort of sanitary napkins, all of which would not alter the utility of the present
invention.
The liquid permeable material may be a nonwoven fabric such as a spunbonded fabric, a thermal
bonded fabric, a resin bonded fabric, and the like; an apertured polymeric film such as DRI-WEAVE
commercially available from the
Procter and Gamble Company, and the like; or any other suitable covering surface that is capable of
allowing fluid to permeate and be comfortably worn against the perineum. The fibrous structures can
be coated with essential oils, or a solution of
essential oils, as the individual fibers are spun, or during, or after a nonwoven
structure is made with the fibers. Polymeric films can be coated with essential oils by
any number of methods known by one skilled in the art. The preferred material to be
used as the body-contacting surface is a non-woven.
After menstrual fluid or urine contacts the cover of the napkin, the fluid is transferred from the cover
material to the absorbent materials for storage. This can include the use of an additional transfer
layer to facilitate the kinetics of this step. A representative, non-limiting list of materials useful as the
absorbent includes cellulosic fibers, such as wood pulp and cotton pulp; synthetic fibers, such as
polyesters and polyolefins; superabsorbent polymers, such as polyacrylic acid, and the like. Another
unexpected benefit of the present invention is that it has been found that essential oils can be added
to superabsorbent polymers without significant premature swelling of the polymers. Preferably, the
structure includes wood pulp and about 5 to 80 % fusible, thermoplastic fibers. As with the cover
materials, essential oils can be added to the absorbent materials during their manufacture.
To prevent any absorbed fluid from leaking out of the bottom of the napkin and onto the body or
clothing, a liquid impermeable material is added as a barrier.
Useful barriers include, without limitation, polymeric films or coatings, such as polyolefins (e. g.,
polyehtylene and polypropylene), polyvinyls (e. g., polyvinyl acetate, polyvinyl chloride, and
poyvinylidene chloride), copolymers (e. g., ethylene vinyl acetate), and blends or laminates of one or
more of the above polymers; bodily fluid repellant structures such as nonwovens, apertured flims,
272/1651
and repellant fiber layers integrated into the bottom layer of the absorbent materials. Preferred
barriers include polypropylene and bodily fluid repellant nonwovens. The most preferred barrier is
constructed out of polypropylene films. Without limitation, two methods to apply essential oils to the
preferred barrier materials is by externally coating the materials, or by compounding in essential oils
prior to fiber or film extrusion, after which the essential oils will migrate to the surface of the materials.
Adhesives are often times included in the construction sanitary napkins to adhere the multiple
elements described above. Positioning adhesive can also be applied to the impermeable barrier
material, allowing the sanitary napkin to be attached to the crotch of undergarments. To eliminate
gaps between the body and the
sanitary napkin, there has also been innovations disclosing methods of using
adhesives on portions of the liquid permeable surface for attaching the napkins
directly to the perineum. A direct body adhering sanitary napkin is disclosed in US
Patent Number 5,658,270, herein incorporated by reference. Adhesives are excellent carriers for
essential oils. The additive can readily be dispersed in many adhesive types, such as hot melts and
warm melts. Using adhesives as a carrier can improve the add-on level and placement of essential
oils. The adhesives also serve as binder material that can reduce the amount of essential oils lost
prior to use. A representative, non-limiting list of materials useful as either construction or positioning
adhesives includes acrylics, starch based hot melts, adhesives based on block copolymers of vinyl
aromatic hyrdocarbon and one or more conjugated diene or hyrogenated aliphatic blocks, polylactic
acids, hot melts based polyolefins such as amorphous poly alpha olefins which may consist of one or
more of the following monomers: propylene, ehtylene, butene, and hexene; hot melts based on low
density polyethylene or low density polyethylene copolymers including ethylene vinyl acetate, methyl
acrylate, n-butyl acrylate, and acrylic acid. Typical positioning adhesives that are well known in the
art are based styrenic block copolymers as disclosed in US Patent
Numbers 5,149,741; 5,143,968; and 5,057,571.
It is also possible for the material used for wrapping the individual products to contain essential oils.
Typically the wrapping material is constructed with either polyolefin films, such as polypropylene, or
with a form of paper. One method of utilizing the wrapping material to apply essential oils to the
napkin, is to coat the paper or polymeric film with known techniques, such as spraying, slot coating,
or extrusion. The essential oils can then be transferred or migrate to the napkin itself during the
packaging process or anytime prior to the consumer opening the individually packaged product.
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The disclosure thus far has focused on sanitary napkins, the multitude of elemental features that can
be included in their construction, and methods of adding essential oils to one or more of the
individual elements. The essential oils can be added to sanitary napkins during their manufacture, or
to the final product. Adding the essential oils during the article manufacture is the most preferred
method of incorporation of the present invention. This approach can be accomplished through a
number of techniques, including but not limited to, spraying, slot coating, transfer coating, solid
gravimeteric feeders, via positioning adhesives and construction adhesives, and dip coating.
Preferably, essential oils are applied by spraying onto the sanitary napkin during its manufacture.
Essential oils can also be added to tampons, and other internally worn disposable absorbent articles.
Consistent with the techniques for incorporating essential oils into externally worn articles, there are
multiple methods suitable for the present invention, including, but not limited to adding essential oils
to an element used to manufacture tampons, adding essential oils to a tampon during its
manufacture, and adding essential oils to the tampon after its manufacture. The majority of tampons
are constructed of absorbent fibers, such as viscose rayon and cotton, and the like. The tampons
may optionally have a cover material on the outside surface to provide ease of insertion and removal,
and also to reduce fiber sloughing during use in the vaginal canal. A representative, non-limiting list
of materials useful as the cover includes apertured polymeric films, nonwovens constructed from
polyester fibers, polyolefin fibers, bicomponent fibers, and the like; and other materials that will allow
fluid to pass through and into the absorbent material contained by the cover. US Patent Numbers
4,294,253 and 4,642,108 disclose tampon constructions and processes of manufacture.
Preferably, essential oils would be added to the tampon cover material. The technique for adding
the essential oils to the cover could be any known in the art, such as dip, slot, spray, melt blown,
control coat, and swirl spray.
Another disposable absorbent article the present invention is appropriate for is wipes or towelettes.
Wipes are typically in the form of a fibrous web constructed from a single layer of fibers, or multiple
layers. The fibers can be woven or nonwoven in nature. Preferably the construction is a nonwoven
made from spunbound, meltblown, or combination thereof. A representative, non-limiting list of
materials useful in manufacturing the non-wovens is polyolefins, polyesters, acrylics, and cotton.
Wipes are used for numerous fluid management purposes, including, but not limited to during baby
diaper changes, during menses management article changes, after urination, after a bowel
movement, and after sexual intercourse. Those of ordinary skill in the art would readily appreciate
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that a wipe containing an effective amount of essential oil to provide a pleasant aroma and inhibit
microbial growth, would be beneficial for the above purposes.
In the following examples, a series of essential oils were subjected to the zone of inhibition test with
a variety of bacteria as follows. The selected bacterium, as shown in Table 1 below, was uniformly
added to a medium such as blood or nutrient agar. An essential oil was added to a small stainless
steel cylinder embedded in the agar, and incubated overnight. The size of the bacteria-free zones
around the cylinders were then measured. Typically, multiple cylinders, with varying levels of the
agent, were used. Table 1 shows the results for a number of essential oils when tested with various
bacteria test cultures.
TABLE 1: Zone of Inhibition
Zone of Inhibition, millimeters
Essential Oil S. aureus E. coli Ps. aeruginosa Str. faecalis C. albicans
type, 0.1 ml. ATCC 6538 ATCC 8739 ATCC 9027 ATCC 7080 ATCC 10231
Rosemary 36 24 18 23 20
Clove bud 30 21 17 17 19
Ginger 16 12 12 14 10
Thulasi 27 20 16 17 20
Turmeric 21 14 15 13 9
Lemon grass 25 18 17 18 19
A series of essential oils were also subjected to the Durham's fusion tube test using a variety of
bacteria. The tests were conducted as follows. Agar slants were innoculated with the desired culture,
and a measured amount of hexane extracted essential oil (i. e., 0.1 ml) was placed in a sterile
Durham's Fusion tube (2mm inner diameter). The Durham's tube was introduced to the agar slant
and incubated at a 30 angle such that the vapors emerging from the tube covered the surface of
the agar slant.
Table 2 shows the percent inhibition of the volatile component of selected essential oils after 48
hours of residence in the innoculated agar slant.
Tables 3 and 4 show the minimum inhibitory concentrations for Hinoki Oil and
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Achillea Oil, using the Durham's fusion tube method.
TABLE 2: Durham's Fusion Test
Inhibition after 48 hours
Essential Oil S. aureus E. coli Ps. aeruginosa Str. faecalis C. albicans
type, 0.1 ml. ATCC 6538 ATCC 8739 ATCC 9027 ATCC 7080 ATCC 10231
--+++++Rosemary++++
Clove----Ginger + +
Thulasi
Turmeric
Lemongrass ~ ~ ~ ~
+-NotThyme++ tested
Key inhibition gradient: -= 0% inhibition on start + = 25% inhibition ++ = 50% inhibition +++ = 75%
inhibition ++++ = 100% inhibition
TABLE 3: Hinoki Oil: Minimum Inhibition Concentrations
Conc., ppm Ps. aeruginosa Proteus S. aureus C albicans L. acidophillus P. mirabilis E. coli
ATCC 9027 vulgaris ATCC 6538 ATCC 10231 ATCC 4356 ATCC 29906 ATCC 8739
++++++400+
++++++600+
++++++800+
1000
+-+-++110+
1200 + + + + +
1600 + + + + +
1800 +
2000 + + + + +
2400 + +
2600 + +
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2800 + +
--+--+3000TABLE 4: Achillea Oil: Minimum Inhibition Concentrations
Conc., ppm Ps. aeruginosa Proteus S. aureus C. albicans L. acidophillus P. mirabilis E. coli
ATCC 9027 vulgaris ATCC 6538 ATCC 10231 ATCC 4356 ATCC 29906 ATCC 8739
400
++++++600+
800 + + + + + + +
1000+++++++
+-+-++1100+
1200 -+-+++
1600 + + + + +
1800 + + + + +
2000 + + + + +
2400 + + + + +
2600 + + + +
2800 + + +
3000 + + +
The invention has been illustrated by, but is not intended to be limited to, the above description and
examples. The scope of the invention is to be determined by the claims attached hereto.
Claims:
What is claimed is: 1. A disposable absorbent article containing an effective amount of essential oil to
provide an aroma and inhibit microbial growth.
2. The disposable absorbent article of Claim 1 wherein the essential oil is rosemary
oil.
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3. The disposable absorbent article of Claim 1 wherein the amount of essential oil is
from about 0.1 to about 8.0 weight percent.
4. The disposable absorbent article of Claim 1 wherein essential oil is added to the
disposable absorbent article during its manufacture.
5. The disposable absorbent article of Claim 1 wherein the article is defined to be
sanitary napkins, tampons, or wipes.
6. The disposable absorbent article of Claim 1 wherein any one of the elements used
in making the article is combined with essential oil prior to manufacturing the
disposable absorbent article.
7. The disposable absorbent article of Claim 6 wherein the essential oil is contained
within adhesives used to adhere a plurality of elements making up the article.
8. The disposable absorbent article of Claim 6 wherein the essential oil is contained
within adhesives used to attach the article to undergarments.
9. The disposable absorbent article of Claim 6 wherein the essential oil is contained
within adhesives used to adhere the article directly to a user's body.
10. A disposable absorbent article contained with wrapping material, wherein the
wrapping material contains and effective amount of essential oil to provide an
aroma and inhibit microbial growth.
11. The disposable absorbent article of Claim 10 wherein the amount of essential oil is
from about 0.1 to about 8.0 weight percent.
12. A method of making a disposable absorbent article comprising the following
steps:
a) providing an absorbent material,
b) providing a liquid permeable material,
c) providing a liquid impermeable material,
d) encasing the absorbent material with the liquid permeable material and
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liquid impermeable material; and
e) contacting at least one of the absorbent material, the liquid permeable
material, the liquid impermeable material, or a combination thereof with an
effective amount of essential oil to provide an aroma and inhibit microbial
growth.
13. The method of Claim 12 wherein the process of contacting any one of said
materials with essential oil is selected from the group consisting of dip, slot, spray,
roll, and swirl.
14. The method of Claim 12 wherein the amount of essential oil is from about 0.1 to
about 8.0 weight percent.
15. The method of Claim 12 further comprising the step of adhering the absorbent
material to the liquid permeable material, or the absorbent material to the liquid
impermeable layer with adhesives.
16. The method of Claim 15 wherein said essential oil is found in the adhesives, in an
amount effective to provide an aroma and inhibit microbial growth.
17. The method of Claim 12 wherein the absorbent material contains superabsorbents.
18. The method of Claim 17 wherein said essential oil is found in the superabsorbents,
in an amount effective to provide an aroma and inhibit microbial growth.
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53. EP1159009 - 14.09.2000
USE OF NIAOULI ESSENTIAL OIL AS TRANSDERMAL PERMEATION ENHANCER
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP1159009
Inventor(s):
GIANNACCINI BORIS (IT); SAETTONE MARCO FABRIZIO (IT); MONTI DANIELA
(IT); BOLDRINI ENRICO (IT); BIANCHINI PIETRO (IT)
Applicant(s): GIANNACCINI BORIS (IT); SAETTONE MARCO FABRIZIO (IT); MONTI DANIELA
(IT); BOLDRINI ENRICO (IT); FARMIGEA SPA (IT); BIANCHINI PIETRO (IT)
IP Class 4 Digits: A61K; A61P
IP Class:
A61K47/44; A61P29/00; A61K47/22; A61P15/00
E Class: A61K47/44; A61K31/18; A61K31/192; A61K31/196; A61K31/405; A61K31/5415
Application Number:
WO2000IT00079 (20000309)
Priority Number: IT1999RM00151 (19990310)
Family: EP1159009
Equivalent:
AU3324000; IT1305303; ITRM990151
Cited Document(s):
EP0744177; WO9307901; WO9926589
Abstract:
COMPOSITIONS FOR TRANSDERMAL AND DERMAL ADMINISTRATION OF PHARMACEUTICALLY
ACTIVE PRINCIPLES, PARTICULARLY STEROIDS, AS FOR EXAMPLE ESTROGENS, STEROIDAL
PROGESTINS OR ANTI-PROGESTINS, AND NON STEROIDAL ANTI-INFLAMMATORY DRUGS
(FANS), AS FOR EXAMPLE, DICLOFENAC, AMMONIUM DIETHYL DICLOFENAC, KETOPROFEN,
PIROXICAM, NIMESULIDE, WHEREIN THE NATURAL ESSENCE KNOWN AS NIAOULI OIL, AS
ENHANCER OF THE PERCUTANEOUS PERMEATION AND ABSORPTION OF THE DRUG, IS
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INCLUDED. IN ADDITION TO THE ABSORPTION OF THE DRUGS AT SYSTEMIC LEVEL THE
FORMULATIONS CONTAINING NIAOULI OIL ARE SUITABLE FOR DERMATOLOGICAL
APPLICATIONS WHEREIN AN IMPROVED PENETRATION OF A DRUG, FOR EXAMPLE A
STEROIDAL OR NONSTEROIDAL ANTI-INFLAMMATORY DRUG, THROUGH THE HORNY LAYER IS
REQUIRED. THE INVENTION FURTHER RELATES TO THERAPEUTIC SYSTEMS FOR THE
TRANSDERMAL ADMINISTRATION (STT) INCLUDING NIAOULI ESSENTIAL OIL AS A
PENETRATION ENHANCER.Description:
USE OF NIAOULI ESSENTIAL OIL AS TRANSDERMAL PERMEATION
ENHANCER
The present invention relates to the use of niaouli essential oil as enhancer for the transdermal
permeation. More specifically the invention relates to formulations and systems for the transdermal
administration of pharmaceutically active principles, particularly steroids, as for example estrogens,
progestins and nonsteroidal anti-inflammatory drugs (FANS), as for example diclofenac, ammonium
diethyl diclofenac, ketoprofen, piroxicam, nimesulide, wherein as enhancer of the percutaneous
permeation and absorption of the drug, the natural essence known as niaouli oil, is included, or a
mixture whose composition at least approximates that of the niaouli oil.
In the relatively recent years the transdermal administration of drugs designed to be active at
systemic level has been the subject of a wide research and development activity in view of the
advantages so provided with respect to other systemic administration ways, as conventional
parenteral and oral. In fact, in comparison to the injection administration route the transdermal
application certainly is accepted with less discomfort by the patients and does not require the action
of skilled people, while in comparison to the oral administration way, which from the practical point of
view is simpler and less traumatic, it provides all the advantages resulting from the direct release of
the drug in the blood system. Particularly the transdermal way allows to reduce the variability of the
absorption amounts over the time and among the patients, providing a controlled and sustained
release of the active principle within the organism. Furthermore, by avoiding the passage of the drug
through the gastrointestinal tract, this administration way prevents the occurrence of any undesired
reaction or gastric or intestinal incompatibility from the drug itself and by avoiding the metabolism of
the first hepatic pass prevents a portion of the drug, major or minor depending on the nature thereof,
from being subjected to a metabolic degradation thus loosing partially its biological activity.
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In spite of the above reported advantages and the fact that the cutis is the widest and most easily
accessible organ of the human body the development of drugs for transdermal release is hampered
by the practical difficulty resulting from the necessity of the passage of the active compound through
the complex membrane constituted of different cutaneous layers.
Theoretically the cutis offers various possible penetration pathways, as the trans-eccrine through
the eccrine sudoriparous glands, trans-sebaceous through sebaceous glands, trans-follicular
through the hair follicles, inter-cellular, also called lipid pathway and trans-cellular, called also polar
pathway, but almost all diffusing agents permeate through the horny layer substantially by two
pathways: the inter-cellular and trans-cellular. Of these the tortuous intercellular pathway is
considered the main pathway and the most important barrier for the most drugs. Globally the
passage of the drug involves the overcoming of the external horny layer and the diffusion through
the epidermis and papillary derma and finally the penetration through the walls of the capillaries or
lymphatic vessels and it is clear that such a phenomenon meets different resistances depending on
each tissue type. In any case the horny layer, due to its dense and highly horny cells, represents the
primary barrier which contrasts the absorption of foreign substances in the skin and their passage
through the same.
In effect the main factors which affect the delivery of drugs through the skin are, in addition to the
chemical-physical properties of the permeating agent and characteristics of the carrier wherein the
drug is dissolved, the characteristics of the horny layer, which is to 500000 times less permeable for
various substances than the underlying derma. The permeability of the horny layer can depend not
only on factors as age, race, presence of occlusive phenomena, cutaneous pathologies, but also
and above all on its integrity and thickness, in addition to the temperature and hydration conditions
and eventual preliminary contact with various solvents. Particularly the thickness of the horny layer is
highly variable depending on the anatomical zone, exposure to ultraviolet radiation or physical
stresses and it is inversely proportional to the permeability. As to the hydration state resulting from
the absorption of water by the protein portion of the cutis, generally an increase of the pore size is
observed and the diffusion of the water through the human horny layer increases when the latter is
hydrated. The permeation of a few drugs appears to be enhanced by this hydration state whereas in
the case of compounds very soluble in lipids, on the contrary, a decrease of the cutaneous
permeation can occur (Blank I. H., The effect of hydration on the permeability of the skin, in
Percutaneous Absorption, Bronaugh R. L. and Maibach
H. I., Marcel Dekker, Inc, Ed., New York, pagg. 97-123, 1985). Chemical modifications can also
modify the permeability of the cutaneous layer: for example, it was detected that organic solvents
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and surface active agent solutions can result in the removal of lipids from the horny layer, increasing
the permeability thereof (Behl C. R., Kreuter J., Flynn G. L., Walters
K. A. and Higuchi W. I., Mechanism of solvent effects on percutaneous absorption. I: effects of
methanol and acetone on the permeation of n-alkanols through hairless mouse skin, A Ph. A. Abst.
10 (1), 98,1980).
If we consider that a successful transdermal administration depends on the capacity of the drugs to
permeate through the horny layer in amounts and at enough high rate to produce the desired
therapeutic effects, the importance of being able to increase the amount and rate of such a
permeation clearly appears.
The most drugs, the transdermal administration of which has been studied, could not penetrate
through the skin or do at not sufficient level for a therapeutic use, if they were not together with
special adjuvants known as "penetration enhancers"or"permeation enhancers"or also"absorption
promoters". These substances, acting by various and not always understood mechanisms, enhance
the active principle to overcome the barrier of the horny layer by increasing the transdermal flow, i. e.
the amount of drug which goes through the skin for surface and time unit.
The permeation enhancers, which generally can act at level both of polar penetration, associated
with the protein component of the horny layer, and not polar penetration, associated with the lipid
component, can be classified according to different criteria depending on their structure, action
mechanisms, and drug type against which the activity is experienced. According to one of the
classifications, for example, substantially three different groups of transdermal permeation enhancers
are identified: solvents, surface active agents and differently acting compounds (Walters K. A.,
Transdermal Drug Delivery, J. Hadgraft and R. H. Guy
Eds., Marcell Dekker, Inc, Ed., New York and Basilea, 1989).
Accordingly the first studies about the permeation enhancers, published in 1970, relate to two
solvents, dimethylsulfoxide and N, N-dimethylacetamide (U. S. patents No. 3 551 554, Crown
Zellerbach and No. 3 472 931, Forster Milburn). It was recognised that these compounds, together
with other solvents like dimethylformamide and ethyl alcohol, increase the penetration through the
skin by means of their capacity to dissolve the lipids of the horny layer.
Particularly, in 1983 (U. S. patents No. 4 379 454 et al., Alza) it was suggested ethyl alcohol to be
suitable for the transdermal release of estradiol, in dosage forms presently known as transdermal
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therapeutic systems (STT or TTS), constituted of patch structures which maintain the active principle,
together with the eventual enhancer and other excipients, if desiderd, firmly fixed on the cutis.
However the high permeation ability of ethyl alcohol, in addition to cutaneous tolerability problems,
exhibited the drawback in that a remarkable excess of enhancer was required, in order to avoid the
exhaustion in the transdermal system before the complete utilisation of the active principle. For such
a reason it was necessary to use a STT (of the type presently known as"reservoir", called also"of the
first generation") equipped with a reservoir wherein the drug and the enhancer are in the form of
solution, which reservoir is separated from the skin on which it is adherent by means of a membrane
able to control and limit suitably the flow of ethyl alcohol.
In addition to ethyl and isopropyl alcohol, subsequently other alcohols were suggested to be
suitable as enhancers, among which several aliphatic long chain alcohols (for example U. S. patents
No. 4 906 169, Rutgers Univ.; patent application PCT No. WO 90/04397, Schering Plough) and
polyfunctional alcohols as propylene glycol or glycerol, often associated with ethyl alcohol to
enhance the tolerability thereof (for example U. S. patent No. 4 855 294, Theratech). Also fatty acids
have been widely used, both alone and in association with other enhancers (for example U. S. patent
No. 4 626 539, Du Pont de Nemours; european patent No. 255 485, Warner Lambert, particularly
with reference to linoleic acid; U. S. patent No. 4 863 970,
Theratec, particularly with reference to oleic acid and corresponding alcohols, in combination with a
lower alcohol), as well the esters of fatty acids, preferably iso-propyl miristate, which already had
been successfully used in many pharmaceutical and cosmetic preparations (for example european
patent No. 436 203,
Nitto) and the esters of lauric acid (for example U. S. patent No. 4 568 343, to Alza, concerning
polyethylene glycol monolaurate, U. S. patent No. 4 746 515, again to
Alza, concerning glyceril monolaurate, U. S. paten No. 4 537 776, Procter & Gamble, concerning an
association of methyl laurate and N-2-hydroxypropyl pyrrolidone). Nmethyl-2-pyrrolidone and
derivatives thereof, as that just above mentioned, also received a successful consideration as
permeation enhancers, although the base molecule exhibits toxicity at some degree.
Other groups of compounds which showed activity in enhancing the transdermal penetration of
various active principles are Zonez (1dodecylazacycloeptan-2-one) and derivatives thereof (US
patents No. 3 989 816 and No. 4 316 893 and others, to
Nelson), the action mechanism of which is not yet clearly understood, alkanolamides (Nhydroxyalkyl-or N-di- (hydroxyalkyl) amides of fatty acids (for examples european patent No. 008
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3371, to Key Pharmaceuticals), phospholipids and derivatives of phosphates, as for example lecithin
(US patent No. 4 783 450, to Warner
Lambert) and sorbitan monoesters, diesters and triesters of fatty acids, in association with lower
aliphatic alcohols, if desired (for example U. S. patent
No. 5 122 383, to Theratech).
According to above, many essential oils and components thereof, principally terpenes, have been
studied as enhancers of transdermal permeation of various drugs, as, for example, 5-fluorouracil,
triamcinolone, indomethacin, ketoprofen and estradiol.
The effectiveness of these agents in enhancing the percutaneous penetration of the active principle
with which are in association would depend on an interaction with lipids of the horny layer resulting in
the destruction of the structural order thereof and an increase of the diffusing capacity of the active
principle by the lipid intercellular pathway. For example, in different patent documents (U. S. patents
No. 4 931 283 and No. 4 933 184, to American Home
Products, patent application PCT No. WO 91/115441, to
Morimoto) menthol has been suggested to be suitable as permeation enahncer of various drugs and
the cardamon essential oil (principally constituted of monocyclic terpenes) has been tested as
permeation enhancer of piroxicam through the rabbit skin, with the recognition that the pre-treatment
of the cutis by means of the enhancer during about one hour resulted in a strong increase of the
cutaneous permeation of the drug (Huang
Y. B., Wu P. C., Ko H. M. and Tsai Y. H., Effect of pretreatment by cardamon oil on in vitro
percutaneous penetration of piroxicam gel, Int. J. Pharm., 131-41, 1996).
One of the aspects which induced to study the use of the essential oils as possible permeation
enhancers was that their use is well documented both in the cosmetic and pharmaceutical field and
therefore it is less hazardous from the toxicity point of view. It is to be pointed out, indeed, that an
ideal enhancer should be not toxic, pharmaceutically inert, not irritating and not allergenic and
should allow the cutis to restore its usual integrity at the end of the application.
Among the first published documents about the use of terpenes as transdermal permeation
enhancers there is european patent No. 006 9385 (Merck & Co.), concerning eucalyptol or 1,8cineole, a terpene compound contained in various essential oils, the most important of which is the
eucalypt oil. This document suggests the use of 1,8-cineole as enhancer of the penetration of any
drug, designed to be active at systemic level and for dermatological use. Also in the latter case, in
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fact, it is necessary that the active substance overcomes the surface barrier represented by the
horny layer so that it is available in the derma and next lower tissues.
While the pharmaceutical compositions suggested in this document are in the form of topic
preparations, like lotion, cream, liniment or spray, the form of transdermal therapeutic system using
eucalyptol as enhancer has been the subject of subsequent patents of Ciba-Geigy, as for example U.
S. patent No. 5 079 008. This patent discloses a STT system of a type called"monolithic" (more
frequently known as"matrix"system) which does not contain the reservoir of the drug but the latter is
dispersed within an adhesive matrix, together with other adjuvants, if desired, and the whole
formulation is coated on a plastic support layer so that the assembly constitutes a patch much
thinner than those of the previous generation. In such a system 1,8-cineole is added to the matrix as
transdermal permeation enhancer.
According to the description, 1,8-cineole, which is present in the eucalyptus essential oil at
concentrations usually higher than 70 weight per cent, is included in the formulation preferably as
neat compound, but raw compounds (or not completely purified), with the provision they contain at
least 70 per cent 1,8-cineole, can also be used. Furthermore the document provides the association
of the suggested enancher with another permeation enhancer, which preferably is N-methyl-2pyrrolidone. Again in this case the drugs, the delivery of which can be enhanced by the enhancer,
are various and among these there are steroidal hormones.
Another patent document which suggests the use of components of essential oils in pharmaceutical
compositions to be administered by transdermal way is patent application PCT No. WO 91/05529 (to
Watson
Laboratories), according to which a not aromatic terpene alcohol or ester thereof, is included in the
matrix of a STT preparation in order to promote the release of the drug from said matrix. The tested
formulation, which preferably includes also an absorption enhancer selected among known ones, is
substantially based on alfa-terpineol as a not aromatic terpenic alcohol. The transdermal system is
suggested to be suitable for release of any drug, including steroids (among which, specifically, there
are 17-betaestradiol and dehydroepiandrosterone) and nonsteroidal anti-inflammatory drugs (among
which, specifically, there are piroxicam and ketoprofen).
Again the patent application PCT No. WO 98/37871 (3M) concerns the use of terpenes as
permeation adjuvants for transdermal systems, but with limitation to the testosterone release.
Although in the specification various terpenes are mentioned as being suitable for the designed
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purpose, the formulations reported in the experimental examples include testosterone associated
only with alfa-terpineol, with or without additional not terpenic permeation adjuvants.
Within the context of the research about essential oils or derivatives thereof having characteristics
suitable to be used as transdermal permeation enhancers it has been now found out that an essential
oil, already known and used in therapeutic field, namely niaouli, is particularly effective in enhancing
the penetration of pharmacologically active compounds through the skin. In addition to remarkable
enhancement of the passage of the drug with which is associated, niaouli essential oil is
characterised also by the absence of toxic and allergenic properties, which is peculiar for many of
such natural products.
As known, niaouli essence is an oil obtained by steam distillation from fresh leaves of Melaleuca
viridiflora Gaertn., a plant of the Myrtaceae family, principally frequent in Australia, New Caledonia,
Indonesia and Madagascar. This essence, being normally a colourless or green-yellow colour liquid,
smelling and tasting like camphor and peppermint, is commercially known as gomenolato oil or
oleogomenol, and it is used above all for its balsamic, expectorant and antiphlogistic properties,
usually in preparations to be administrated by nasal instillation and inhalation, for the therapy of the
upper respiratory infection.
Products based on niaouli oil are also administrated by external use in the form of creams and
liniments for stimulating massages or on fading skin, taking
advantage of the hyperemia inducing effects of the essence.
The composition of niaouli oil, as well as all natural essences, is somewhat variable depending on
the geographical origin, plant variety, harvesting and extraction techniques and various other factors,
but in any case it includes a remarkable amount of 1,8-cineole and significant amounts of alfaterpineol and alfapinene, in addition to various other components, among which limonene, linalol,
beta-pinene, sesquiterpene alcohols, valeraldehyde and benzaldehyde. According to
Official Italian Pharmacopeia, the characteristic features of niaouli essential oil are a concentration of
1,8-cineole in the range from 50,0 to 60,0 weight per cent and the presence of alfa-terpineol at
detectable concentrations. Based on what found out according to the present invention and as below
will be disclosed in more detail, niaouli essential oil exhibits such an activity as transdermal
penetration enhancer for drugs, steroidal and non steroidal, that it is significantly higher than that
exhibited, at the same concentration, by any one of its main components, particularly 1,8-cineole,
alfa-terpineol and alfapinene. Furthermore the transdermal flow obtained by using niaouli oil is
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surprisingly higher than the sum of the flows obtained using individually the three above mentioned
components, any one at the same concentration as it is contained in naiouli oil.
It is therefore an object of the present invention a composition for the transdermal and dermal
administration of pharmaceutically active principles including therapeutically effective amounts of
one or more of said active principles, one or more percutaneous permeation enhancers and other
pharmaceutically acceptable adjuvants and excipients, if desired, wherein said one ore more
percutaneous permeation enhancer include niaouli essential oil.
Depending on various possible sources derived from, niaouli oil can include amounts of the three
main components variable in the following ranges: from 40 to 65 weight per cent 1,8-cineole, from 6
to 30 weight per cent alfa-terpineol and from 1 to 20 weight per cent alfa-pinene, preferred
concentrations being from 50 to 55 per cent 1,8-cineole, from 7 to 14 per cent alfaterpineol and from
12 to 18 per cent alfa-pinene.
Drugs for which niaouli essence exerts an enhancing effect for the percutaneous permeation
includes firstly the class of steroidal compounds, including, specifically, estrogens (for example
estradiol and esters thereof, ethynyl-estradiol, estriol), androgens (for example testosterone, methyl
testosterone, fluoximesterone), progestins (for example progesterone, noretisterone or noretindrone,
norgestrel, gestodene), steroidal anti-progestins (for example mifepristone), steroidal anti-androgens
(for example cyproterone) and corticosteroids (for example cortisone, hydrocortisone,
betamethasone, prednisolone, triamcinolone and esters thereof). In addition to antiinflammatory
steroidal drugs (corticosteroids) niaouli essential oil exhibits a remarkable enhancing activity for the
percutaneous permeation also against FANS (non steroidal anti-inflammatory drugs), among which
are included, for example, diclofenac, piroxicam, ibuprofen, naproxen, ketoprofen, indomethacin
and nimesulide.
Particularly, estrogens are already widely used within formulations to be administered by
transdermal route, which proved to be advantageous for carrying out the so-called estrogenic
substituting therapy. As already known, the purpose of the estrogenic substituting therapy
substantially is to ameliorate various short and long term disorders, resulting from both physiologic
and surgically induced menopause, for example. Usually this therapy takes advantage of oral
administration of estrogens, in combination or subsequent to progestins, if desired.
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The hormonal substituting therapy carried out by using transdermal therapeutic systems proved an
efficiency comparable to that of oral systems, but providing the advantage resulting from avoiding
the interactions with other orally ingested drugs and a specific pharmacokinetic profile which can
results in better clinical results. Almost all the presently commercially available STT estradiol forms
(or estro-progestinic associations), a few of which make use of transdermal permeation enhancers,
are to be replaced every 3-4 days and it is therefore clear that the purposes of a better formulation of
these administration routes include the reduction of the active principle content in any patch, at the
same daily release or, at the same active principle content, a longer activity period.
In addition to the transdermal therapeutic systems there are various other pharmaceutical forms
wherein the compositions of the invention can be included, being possible, for example, to prepare
them as creams, pomades, ointments, gel, suspensions, emulsions, ecc., depending on the choice
and proportions of the excipients, making use of formulation techniques well known in the
pharmaceutical field. Particularly, a form designed to be administered by percutaneous way,
specifically for carrying out the substituting estro-progestinic therapy, which has been recently
suggested, is as gel, wherein the hormones containing products can be applied on a cutaneous
surface much larger than that allowed by the use of a patch. According to a recent study (Hirvonen
E.,
Cacciatore B., Wahlstrom T., Rita H., Wilten-Rosenquist
G., Effects of transdermal estrogen therapy in postmenopausal women: a comparative study of an
estradiol gel and an estradiol delivering patch, Br.,
J. Obstet. Gynaecol., 104 (Suppl. 16) 26-31,1997), the gel application forms proved, at the same
effectiveness for the substituting hormonal therapy, to be more complied by the patients (96,4 and
90,7 per cent for gel and STT, respectively) and a lower incidence with respect to the cutaneous
irritation.
Generally speaking, the compositions of the invention can include, in addition to one or more active
principles, for example steroids or FANS, and other permeation enhancers and conventional
ingredients, if desired, like, for example, pharmaceutically acceptable preservatives, antioxidants,
thickening agents, surface active agents, stabilisers and plasticizers, a concentration of niaouli
essential oil preferably within the range from 0,5 to 40 weight per cent based on the total weight of
the composition. Propylene glycol, exhibiting the double function as solvent and transdermal
permeation enhancer, proved to be a particularly advantageous ingredient. The synergistic activity of
propylene glycol together with a few terpenes probably results form its ability in increasing the
repartition of terpenes in the horny layer.
289/1651
In the case of a gel formulation, the product can be prepared, for example, using as starting
materials an aqueous dispersion containing carboxyvinyl polimers, like carboxypolymethylene (for
example Carbopol 1342) as gel forming and triethanol amine as neutralizing agents and an alcoholic
solution containing the drug and permeation enhancer of the invention, together with other enanchers
and/or excipients, if desired, mixing then the two solutions until the homogeneity is obtained. The
drug and niaouli oil can be metered at variable amounts depending on the desired therapeutic and
enhancing activity.
In accordance to various specific embodiments of the invention the suggested composition is
provided as a therapeutic transdermal system, which can have one of the different structures up to
now suggested for these administration forms, as for example those, already mentioned, known
as"drug reservoir"or first generation ones. Within these structures the drug and enhancer (as a
solution or colloidal dispersion, together with other excipients, if desired) are contained in a"reservoir",
from which the active principle spreads on the cutis through a polymeric membrane whose function
is to control the rate of the drug release. The membrane, which can be microporous or not and has a
well defined drug permeability, is kept in contact with the cutis by means of an adhesive, meanwhile
on the side opposite to the membrane the "reservoir"is closed by a impervious plastic laminate
protecting it from external environment. By way of example the external support layer can be made of
materials as poliethylene terephtalate, polypropylene, polyvinyl chloride or aluminum coupled
poliethylene; the drug reservoir can be constituted of ethanol hydroxypropyl cellulose gel containing
the active principle together with niaouli oil and other enanchers and adjuvants, if desired; the
membrane can be produced using ethylene-vinyl acetate copolymer or it can be a polypropylene or
polyethylene microporous membrane; the adhesive can be constituted of polyisobutylene and
mineral oil, acrylic or pressure silicon adhesives and, finally, the protective layer to be detached
before the use can be made of silicone treated polyethylene terephtalate or PVC.
However the presently preferred STT form is the so-called matrix type, already mentioned, wherein
the active principle is directly adsorbed within an adhesive solid matrix. In its more recent version the
matrix transdermal patch is constituted of a first support layer, a second layer, which is the matrix,
wherein the active principle, together with possible enhancers and excipients and a pressure
adhesive, is contained, and a third protective layer to be detached before the use. The use of this
STT form is more and more increasing by virtue of the easy and cheap industrial production and
small size thereof providing better compliance by the patient.
290/1651
Therefore, in accordance to a preferred embodiment thereof, the object of the invention is to provide
a system for the transdermal and dermal administration of pharmaceutical active principles
constituted of a laminate comprising:
-a support layer impervious for the components
of the adjacent layer;
-a matrix constituted of a solid mixture
containing a therapeutically effective amount
of one or more of said active principles, one
or more percutaneous permeation enhancers, one
thereof being said niaouli essential oil and
one or more pressure adhesives, as well as
other pharmaceutically acceptable adjuvants
and excipients, if desired;
-a protective layer easy detachable from said
matrix before the application.
Preferred compositions of the niaouli essence are as above already reported and the level of the
latter within the solid mixture constituting the matrix is preferably variable from 0,5 to 40 weight per
cent.
The support layer of the matrix transdermal system must fulfil the following requirements: to provide
such flexibility and softness characteristics to adjust itself suitably to the skin, be impervious and
chemically inert against both the active principle and other matrix components and, finally, adhere
firmly to the matrix after protective film detaching therefrom.
Examples of polymers suitable as support are polyethylene, polyesters, polyurethanes,
polypropylene and like. The adhesive must be selected among products suitable for a long contact
with the skin and providing, together with a stable adhesion, the continuity of administration;
furthermore it must be compatible with all the components of the matrix and maintain their own
adhesion and texture characteristics during the step of the STT production. Examples of suitable
adhesives are polysiloxanes, polyurethanes, polyacrylates, polyisobutylene; among these
polyacrilates with different cross-linking degrees, designed for this use and having Durotak (National
Starch Chemical Co.), Gelvat (Monsanto) and Ellastoide (Rohm Pharma) trade names are preferred.
Finally, as in the case of"drug reservoir"systems, the detachable protective layer is constituted of a
polymer, impervious and inert against the active principle and all other matrix components, which is
291/1651
made easy detachable from the matrix by means of a treatment using silicon and fluorine
compounds on one or both the sides of the protective polymer surface.
Above described transdermal systems can be produced according to standard methods, for
example producing on the support or protective layer a film resulting, by the solvent evaporation,
from a suitably concentrated solution containing the matrix ingredients. Then on the thus obtained
initial structure, the remaining layers are laminated. Again as an example, the pharmaceutical active
principle and niaouli oil can be dissolved, together with other ingredients, if desired, in an alcoholic
solution of polyaminomethacrylic polymer (Plastoidt E35L). The thus obtained solution, poured into a
die coated with a polyethylene film (support layer) can be evaporated at 40 C until the weight is
constant. At the end of the operation the protective layer is added.
Although the foregoing considerations are concerning more directly the transdermal administration
field, wherein a suitable formulation containing a pharmaceutically active principle is applied on a not
degraded skin area in order to perform the penetration of the active principle through the surface
tissues till it reaches the blood flow, it is clear that analogous problems and solutions characterise the
dermatological topic administration wherein it is necessary that the drug goes through the horny
layer and/or surface layers of a wound area in order to be available at optimum concentration in the
involved cutaneous tissues. In the field of the active principles considered according to the present
invention, for example, the corticosteroid drugs used as steroidal anti-inflammatory drugs, and non
steroidal anti-inflammatory drugs can be exemplary.
Some experimental results obtained within the scope of the present invention, including the data
concerning the characteristics and performances of niaouli essential oil and the comparison with
other essential oils and components thereof, are below reported by way of example, together with a
few diagrams represented in the enclosed drawings, wherein:
figure 1 shows the transdermal permeation profiles for estradiol from solutions containing niaouli oil
as enhancer, compared with solutions containing individually any one of its three main components ;
figure 2 shows profiles analogous to those in figure 1 relating to the transdermal permeation of
noretindrone acetate;
figure 3 shows the transdermal permeation profile for estradiol contained in gels together with niaouli
oil enhancer compared to formulations without the enhancer;
figure 4 shows the transdermal permeation profile for mifrepistone contained in solutions together
with niaouli oil enhancer compared to solutions without the enhancer ;
292/1651
figure 5 shows the transdermal permeation profile for diclofenac contained in solutions together with
niaouli oil enhancer compared to solutions without the enhancer;
figure 6 shows the transdermal permeation profile for ketoprofen contained in liquid formulations
together with niaouli oil enhancer compared to formulations without the enhancer;
figure 7 shows the transdermal permeation profile for piroxicam contained in liquid formulations
together with niaouli oil enhancer compared to formulations without the enhancer;
figure 8 shows the transdermal permeation profile for nimesulide contained in liquid formulations
together with niaouli oil enhancer compared to formulations without the enhancer;
figure 9 shows the transdermal permeation profile for diethyl ammonium diclofenac contained in
liquid formulations together with niaouli oil enhancer compared to formulations without the enhancer;
figure 10 shows the transdermal permeation profile for ketoprofen contained in semi-solid
formulations together with niaouli oil enhancer compared to formulations without the enhancer;
figure 11 shows the transdermal permeation profile for piroxicam contained in semi-solid
formulations together with niaouli oil enhancer compared to formulations without the enhancer;
figure 12 shows the transdermal permeation profile for nimesulide contained in semi-solid
formulations together with niaouli oil enhancer compared to formulations without the enhancer.
Characterization of the niaouli oil by gaschromatographic analysis
Niaouli essential oil used in the hereinafter reported permeation tests was characterised by
gaschromatographic (GC) analysis in order to exactly determine the precise contents of the different
components thereof. Essential oils from two different sources were analysed: niaouli o. e., available
from
A. C. E. F. S. p. A. of Piacenza (hereinafter called NIA) and niaouli o. e. available from by from Muller
& Koster (hereinafter called NIA*).
The analyses were performed by means of an HP 5890 Serie II gas-chromatograph equipped with
HP-Wax and HP-5 (30 m x 0,25 cm) capillary columns, and the following temperature schedule was
used: 10 minutes at 60 C, a 5 C/minute increase to 220 C, 20 minutes at 220 C; injector and
detector temperature: 250 C; carrier gas: nitrogen (5 ml/minute), dual FID detector; 1: 30 split ratio;
injection volume; 0,5 microliters.
The identification of the components was obtained by comparing the chromatograms from the two
columns taking advantage of the retention times of the pure compounds, while as per cent contents
the average value of the percentages obtained from the individual chromatograms was used. In the
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following Table 1 the contents of the three main components of NIA oil, both as determined using
each column and as average values, are reported.
Table 1-GC analysis of the NIA components
Essential oil Wax Column Sil Column Average
Component (%) (%) (%) 1,8-cineole 50,04 51,15 50,59 a-pinene 16,29 16,45 16,37 a-terpineol 8,32
8,31 8,32
In order to compare the compositions of niaouli essences from different sources in the following
Table 2 the average values, obtained as above, of the gas-chromatographic analysis of the NIA and
NIA* products are reported.
Table 2-GC analysis of the NIA and NIA* components
Essential oil NIA NIA*
Components (%) (%) 1,8-cineole 50,6 51,4 a-pinene 16,4 13,5 a-terpineol 8,3 12,7
It is to be pointed out that the analysis showed that at least other 20 components were present,
which represent about 20-25 per cent of the essential oil, among which there are beta-pinene (5 per
cent), limonene (6 per cent), linanol (2 per cent) and paracymene (4 per cent).
Transdermal permeation tests
In order to study the"in vitro"percutaneous permeation, hairless mouse skin, because of its easy
availability and simplicity in the experimental work, was used. The skin, both on the dorsal and
abdominal surface, does not adhere to the internal tissues and therefore it easily can be removed
maintaining an uniform thickness without the use of the microtome.
Male, hairless, 5-7 week old mice were used. Soon following their sacrifice by cervix dislocation of
the spina dorsalis, the intact cutis was cut and the derma was carefully freed of any adherence of
subcutaneous tissue and blood vessels. For the experiments portions having about a 3 cm side
length were cut and used.
The diffusion cell used for the study was of the horizontal type, as proposed by Chien and Valia
(Chien Y. W. and Valia K. H., Development of a dynamic skin permeation system for long-term
permeation studies, Drug. Dev. Ind. Pharm., 10,575-99,1984), the passage having an horizontal
direction through the vertically mounted skin lap. The assembly was constituted of two pyrex glass
symmetrical emi-cells having a relatively small capacity (8,5 ml), constituting the donor and the
recipient compartments, respectively. Each emi-cell had an upper opening for the filling and
294/1651
sampling and a glass or teflon closing to avoid the solvent evaporation. The mixing of the system was
carried out by means of a star type magnetic stirrer at a constant rate of 600 revolutions per minute.
The temperature is maintained constant by means of circulating water within cell double walls at 37 C.
Between the two emi-cells a cutis fragment with 2 cm2 of exposed area is mounted and the cell is
fixed on a platform containing the motors of the magnetic stirrers by means of a plexiglas support
equipped with a screw providing the assembly a perfect tightness.
The described horizontal cells have been selected to carry out suitable experiments concerning the
invention in order to study the mechanisms and kinetics of"in vitro"percutaneous permeation and the
screening of substances suitable to affect the barrier properties of said cutis.
In the below reported tests drug solutions in ethanol (J. T. Baker B. V., Deventer, The Netherlands)
or propylene glycol (Carlo Erba, S. p. A., Milan) solvents, containing the various products under
investigations as permeation enhancers, at the different concentrations considered, were tested as
donor phase. As recipient phase a 66,7 mM, pH = 7,4, phosphate buffer, made isotonic using
sodium chloride (0,44 g/100 ml) and containing sodium azide (0,003 per cent) as preservative, was
used. At suitable time intervals during each test 5,0 ml solution samples were withdrawn from the
recipient compartment, equal volumes of fresh buffer solutions being the replacement.
The drug content of the recipient phase was determined by HPLC analysis. The equipment used
included: Shimadzu LC-6A system, equipped with UV SPD6AV detector and C-R4A integrator; 20
microlitre capacity Rheodyne injection valve. Bondclone 300 x 3,0 inverted phase column, packed
with a 10 micrometer C18 (Phenomenox) phase and pre-column was Guard-PaK
Inserts, C18 micro-Bondapack (Waters). For the analysis of estradiol the mobile phase was an
acetonitrile: water: methanol mixture (45: 45: 10) (methanol and acetonitrile supplied by J. T. Baker
B. V.,
Deventer, The Netherlands). The flow was 1,0 ml/min, the detection was carried out at 280 nm
wavelength with a 6 minute retention time. For the analysis of noretindrone acetate the mobile phase
was an acetonitrile: water mixture (60: 40), the flow was 1,5 ml/min, the detection wavelength and the
retention time were 240 nm and about 5 minutes, respectively. For the analysis of mifepristone the
mobile phase was an methanol: water mixture (70: 30), the flow was 1,0 ml/min, the detection
wavelength and the retention time were 310 nm and about 5 minutes, respectively. For the analysis of
doclofenac the mobile phase was a methanol: acetonitrile: Sorensen pH 7,0 phosphate buffer
mixture (30: 17: 53), the flow was 0,8 ml/min, the detection wavelength and the retention time were
295/1651
275 nm and about 9 minutes, respectively. The quantitative analysis was carried out by comparison
using an external calibration curve.
For each formulation to be tested the following parameters were determined:
-steady state flow, J, expressed as microgram
of drug permeating the cutis over the time for
area unit (pg cm'h'); -apparent permability coefficient, Papp
obtained by the relationship Papp = J/Cv, where
Cv is the initial concentration of the drug
(expressed in cm h 1 103);
-lag-time, time taken by the drug to saturate
the cutis and reach the recipient compartment
(expressed in h);
permeated drug percentage at the end of the
experiment (which lasted five hours);
-enhancing factor, FP, measure of the enhancer
activity for propylene glycol (which was used
as solvent in most formulations to be
evaluated), calculated from the ratio between
obtained Papp using the enhancer to be
evaluated and that obtained using alone
propylene glycol.
Example 1
Percutaneous permeation of estradiol from essential oil containing solutions.
In a first step of the study of the enhancer of the invention, the activity of niaouli essential oil as
percutaneous penetration enhancer for estradiol was compared with that of other essential oils,
among which there are cardamon, melissa, sweet orange, myrtle and cajeput oils. It is to be pointed
out that the latter two essences are also extracted from plants of the
Myrtaceae family, namely Myrtus communis and Malaleuca leucadendron, respectively. The myrtle
oil includes, as main components, pinene, 1,8-cineole, dipentene and camphor, while the cajeput oil,
whose composition was more similar to that of niaouli, contains 1,8-cineole as the main component
and remarkable amounts of limonene and alfa-terpineol and minor amounts of alfapinene. Although
the presence of such components the mentioned essential oils showed a very different behaviour in
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the enhancing of percutaneous penetration of steroidal drugs, as it results from the data reported in
the following table.
In all the reported tests propylene glycol was used as solvent and the concentration of 17betaestradiol in the solution was 1 weight per cent.
Table 3
Transdermal permeation of estradiol from essential oil containing solutions
Enhancer J Papp Lag time Permeated
pg Cm~2h~1 cm h-1lO3 h drug, % cardamon o. e.- melissa o. e.- sweet orange o. e. 0,0520,01
myrtle o. e. 0,0450,01 cajeput o. e. 1,6C, 1 0,0260,008 niaouli o. e. 0,0730,004
Notes: a) the percutaneous permeation of beta-estradiol resulted null
Example 2
Percutaneous permeation of estradiol from solutions-Comparison between niaouli and the main
components thereof
In a second test group the activity of niaouli as percutenous penetration enhancer of estradiol was
compared with that of ethyl alcohol and propylene glycol individually used as solvent/enhancer and
with that of the three main components of niaouli, 1,8-cineole, alfa-terpineol, alfa-pinene, individually
used, again in propylene glycol solution and at concentration similar to that they are present in
niaouli essential oil. Specifically the concentrations used for the three comparison solutions were
those suggested by gas-chromatographic analysis of NIA oil (Tables 1 and 2):
1,8-cineole 50,59 per cent
alfa-pinene 16,37 per cent
alfa-terpineol 8,32 per cent
The tests were carried out according to the above reported protocol, using 17-beta-estradiol from
Sigma Chemical Co. (St. Louis, USA) at 1 weight per cent concentration, 1,8-cineole from A. C. E. F.
S. p. A.
(Piacenza, Italy), alfa-terpineol from Sigma Chemical and alfa-pinene from Fluka Chemie AG (Buchs,
Switzerland). The obtained results are reported hereinafter, in Table 4 (No. 1L-6L formulations).
As it is possible to see from the Table, both ethanol and propylene glycol, individually used as
solvent/enhancer (No. 1L and 2L formulations), proved to be little effective in the enhancing the
estradiol permeation through the hairless mouse skin. Differently from the remarkable activity
experienced by niaouli essential oil (No. 3L formulation, at 10 weight per cent concentration) each of
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the NIA individual components at the same concentrations they are present in equal amount of
niaouli oil (No. 4L, 5L and 6L) gave results surprisingly lower than niaouli oil. The most remarkable
aspect results from the consideration that the theoretical flow sum obtained using each of No. 4L, 5L
and 6L formulations micrograms cm 2 h 1) is equal to less than half of the flow obtained using the
essential oil.
Table 4 - Transdermal permeation of estradiol from solutions
Formulations Enhancer J Papp Lag time Permeate
No. 1) g cm-2h-1 cm h-1103 h drug, % 1L ethanol2) 0,32#0,05 0,04#0,006 0 0,007/0,@ 2L propylene
glycol2) 0,2#0,02 0,02#0,002 0 0,005#0,@ 3L NIA (10 %) 10,4#0,79 1,04#0,079 1,76#0,36 0,073#0,@
4L 1,8-cineole (5,06 %) 0,25#0,06 0,025#0,006 2,63#0,193 0,0016#0@ 5L ;-pinene (1,64%)
4,45#0,42 0,445#0,042 2,33#0,073 0,030#0,@ 6L ;-terpineol (0,83%) 0,202#0,06 0,0202#0,006
0,06#0,06 0,005#0,@ 7L 1,8-cineole (10%) 6,68#0,54 0,66730,054 2,13#0,14 0,053#0,@ 8L ;-pinene
(10%) 1,66#0,07 0,166#0,007 0,9030,199 0,017#0,@ 9L ;-terpineol (10%) 0,43#0,15 0,043#0,015 0 0
0,008#0,@ 10L "niaouli like" 9,00#0,70 0,863#0,067 2,54#0,06 0,052#0,@ mixture 11L NIA* (10%)
8,47#0,73 0,847#0,073 2,29#0,079 0,055#0,@
Notes: 1) In all the formulations except No. 1L the solvent was propylene gl@ 2) As olvent/enhancer
By means of a further test group, whose results are also showed in Table 4, the NIA oil activity (No.
3L formulation) was compared with the activity of individually used three main components thereof
(No. 7L, 8L and 9L formulations), at the same concentration (10 weight per cent). Again in this case
NIA proved to be the most effective enhancer for estradiol: the J flow again was notably higher (p <
0,001) than that obtained using same amount of 1,8-cineole, the main component thereof. On the
contrary, alfa-pinene and alfa-terpineol gave significantly low flow values. The permeation profiles
obtained in this test group are also showed in Figure 1.
By comparison the flow values obtained using the individual terpenes at different concentrations, it
is to be pointed out that No. 4L formulation, containing 5,06 per cent 1,8-cineole, provided a flow 27
times lower than the No. 7L formulation (containing 10 per cent 1,8-cineole), exhibiting therefore an
enhancing effect which increases with the agent concentration. On the contrary, alfa-pinene at 1,64
per cent concentration (No. 5L formulation) provided a flow about 2,7 times higher than that obtained
using an about 6 times higher amount of the same agent (No. 8L formulation, alfa-pinene at 10 per
cent concentration). In the case of alfa-terpineol at 0,83 per cent concentration (No. 6L formulation)
the flow is only half of that obtained using a formulation (No. 9L formulation at 10 per cent
concentration) containing 12 times higher amount.
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By means cf a further test group NIA essential oil was compared tc NIA* called oil (No.
11L formulation) from a different source and having a ternary in laboratory prepared composition
constituted of 1,8-cineole, alfa-terpineole and alfapinene combined at the predetermined per cent
ratio resulting from the gas-chromatographic analysis ("niaouli like"called mixture, No. 10L
formulation).
As it is possible to see in Table 4 the comparison with a niaouli essential oil from different source
(NIA*) did not point out statistically significant differences (p < 0,05) for the percutaneous permeation
of estradiol and also the"niaouli like"mixture provided a flow value not statistically different (p < 0,05)
from that obtained using NIA (and in any case about twice the theoretical flow value obtained from
the sum of the individually considered three components).
Although the use of the NIA is in any case advantageous with respect to the"niaouli like" mixture
because of the shorter"lag-time" (and statistically different, p < 0,05), at least as to the estradiol
permeation the thus formulated ternary mixture constituted of 1,8-cineole, alfa-pinene and alfaterpineol is anyway more advantageous than the use of the individually considered terpenes.
Therefore this"niaouli like"formulation represents a further object of the present invention.
Example 3
Percutaneous permeation of noretindrone acetate from solutions-Comparieon between niaouli and
the main components thereof
By means of a further test group the activity of niaouli essential oil as percutenous penetration
enhancer of another steroidal drug, the progestin known as noretindrone or noretisterone acetate.
Also in this case firstly the comparison was made with respect to alone used propylene glycol (as
solvent/enhancer) and each main component of niaouli, i. e. 1,8-cineole, alfa-terpineol, alfa-pinene,
again individually used and each at concentration similar to that they are present in niaouli essential
oil (according to the data ir. Tables 1 and 2). The test protocol were the same as already described
and noretindrone acetate (supplied from Sigma Chemical
Co., St. Louis, USA) was included in the propylene glicol solutions at 1 weight per cent concentration.
The obtained results are reported hereinafter in
Table 5 (No. 12L-16L formulations).
299/1651
The results reported in the table, although different from those obtained using estradiol, confirm
anyway that niaouli o. e. is clearly better than each individually used component. In this case the
theoretical sum of the flows obtained using each of No. 14L, 15L and 16L formulations (1,2630, 2736
igcm'h') is little more than half of the flow obtained using the essential oil.
In the subsequent test group, whose results again are reported in Table 5, the niaouli activity at 10
weight per cent concentration (No. 13L formulation) was compared with that of individual terpenes at
same concentrations (No. 17L, 18L and 19L formulations), demonstrating that the essential oil
according to the invention is the most effective enhancer also for noretindrone acetate. The
enhancing factor, calculated in comparison to the propylene glycol reference formulation (No. 12L),
is also higher than that obtained for estradiol. The graphic comparison of the profiles obtained using
niaouli, 1,8-cineole, alfa-pinene and alfa-terpineol, all at 10 weight per cent concentrations, is
reported in
Figure 2.
Table 5 - Transdermal permeation of noretindrone acetate from solutions
Formulations Enhancer J Papp Lag time Permeated
No. 1) g cm-2h-1 cm h-1103 h drug, % 12L propylene glycol2) 0,0307# 0,0041 0,031#0,0004 0
0,0005# 0,0@ 13L IA (10 %) 2,13#0,18 0,21#0,018 1,66#0,07 0,016#0,0@ 14L 1,8-cineole (5,06 %)
0,03#0,006 0,003#0,0006 1,26#0,64 0,0003#0,@ 15L ;-pinene (1,64%) 1,16#0,25 0,115#0,0025
1,86#0,62 0,008#0,@ 16L ;-terpineol (0,83%) 0,073# 0,0176 0,007#0,0018 0,41#0,06 0,0008# 17L
1,8-cineole (10%) 0,35#0,0815 0,035#0,0081 0,40#0,13 0,004#0@ 18 ;-pinene (10%) 0,418#0,115
0,041#0,0113 0 0,006#0@ 19L ;-terpineol (10%) 0,483#0,028 0,048#0,0028 0,15#0,15 0,007# 20L
"niaouli like" 0,168#0,024 0,016#0,0023 0,68#0,39 0,001@ mixture
Notes: 1) In all the formulations the solvent was propylene glycol 2) As solvent/enhancer
Again with reference to the data in Table 5, comparing the flow values obtained using individual
terpenes at different concentrations it is observed that No. 14L formulation, containing 5,06 per cent
1,8-cineole, gave a flow about 11 times lower than the No. 17L formulation (10 per cent 1,8-cineole)
and, analogously, 0,83 per cent alfa-terpineol (No.
16 L formulation) gave a flow about 7 times lower than that obtained with a concentration of the same
agent about 6 times higher (No. 19L formulation containing 10 per cent alfa-terpineol). Exhibiting an
opposite behaviour, 1,64 per cent alfa-pinene (No.
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15L formulation) gave a much higher (almost 3 times) flow than that obtained using a formulation (No.
19L at 10 per cent) containing a 12 times higher quantity.
The result obtained in the last test group relating to the"niaouli like"mixture (prepared according to
the previous example) is completely different from that obtained using estradiol: in this case the
value of transdermal flow obtained using the "niaouli like"mixture is definitely lower in comparison
both with that obtained using NIA (No. 13
L formulation) and the theoretical value obtained by the sum of the flows obtained using individually
said three terpenes (No. 14L, 15L and 16L formulations), i. e. 1,2510,2245 J.gcm'h'\ The fact that
the prepared in laboratory and called"niaouli like" mixture in this case did not exhibit analogous
results to those obtained using NIA suggests that the effectiveness of the essential oil results also
from its complex composition and does not depend only from the presence of the three considered
terpene compounds.
Example 4
Percutaneous permeation of estradiol form gel carriers
In order to verify the effectiveness of the niaouli essential oil as transdermal permeation enhancer of
17-beta-estradiol from gel formulations like those already described, the same experimental
procedure as in the previous examples has been applied pouring the gel (in spite of solution) in the
donor compartment of the described experimental apparatus. The estradiol gel containing niaouli
essential oil as enhancer has been prepared from the following ingredients:
Carbopol 1342 0,400 g
Water 40,000 g
Triethanolamine 0,720 g
95 % Ethanol 56,820 g
Estradiol 0,060 g
Niaouli o. e. 2,000 g
100,000 g
As already described the first three ingredients were mixed to form a gel inducing aqueous solution,
the three remaining ones were mixed to form an alcoholic solution, then the two mixtures were mixed
to obtain an homogenous semi-solid product.
For comparison, the above described gel has been prepared in the absence of the niaouli oil and
the permeation test results carried out using two different formulations are reported in the following
table. The corresponding permeation profiles are also illustrated in Figure 3.
301/1651
Table 6
Transdermal Permeation of estradiol from gel carriers
Enhancer J Papp Lag time Permeated pg gcm'h'cmh'10hDrug,% 1,4 2,3 2,0 5,0
Niaouli o. e. 2% 2,44 4,1 1,5 8,9
From the above data and more immediately from the permeation profiles compared in Figure 3 it
appears that the addition of niaouli essential oil to the formulation in form of gel remarkably benefits
the drug penetration through the skin.
Example 5
Percutaneous permeation of mifepristone from solutions
The enhancing effect of the niaouli essential oil was experienced with a steroidal drug different from
estrogens and progestins, i. e. mifeprostone. The latter, known also as RU 486, is a synthetic steroid
produced in 1980 (Roussel Uclaf) having an high bonding affinity with the progesterone receptor and
therefore exhibit activity as competitive receptor antagonist of progesterone.
Consequently the use of the product showed effectiveness as non surgical method for the
pregnancy interruption and as emergency contraceptive. More recently the application field of
mifepristone became wider being proved useful also in diseases like endometriosis, tumor of the
endometrium, uterine dysfunctions and premenstrual tension syndrome (Hodgen G. D., Williams R. F.,
Grow
D., Treatment of ovarian estrogen dependent conditions, Faming Zhuanli Shenquing Gonkai
Shuomingshu CN 1144486 AS March 1997,15 pages;
Kettel L. M., Treatment of endometriosis with mifepristone, Int. Congr. Symp. Semin. Ser., 13
(Endometriosis Today) 334-338,1997).
For the permeation tests two different solutions, one (No. 21L formulation) comprising 0,3 g
mifepristone and propylene glycol q. b. to 30,0 g and the other (No. 22L formulation) comprising 0,3
g mifepristone, 3,0 g niaouli essential oil and propylene glycol q. b. to 30,0 g were compared. The
results of permeation tests, carried out according to the same protocol as above, are reported in the
following table, while the corresponding permeation profiles are reported in Figure 4.
Table 7
Transdermal Permeation of mifepristone from solutions
Form. Enhancer J Papp Lag time Permeated FP
302/1651
No. jugcm'h'cmh'10 h Drug, % 21L propylene 0,101 0,0101 0 0,00294 1
glycol2) +0,0053 0,0005 0,0005 22L NIA (10%) 0,991 0,0991 0,928 0,00947 9,83
0,154 0,0154 0,606 0,0006 0,995
Notes: 1) In both formulations the solvent was propylene glycol
2) As solvent/enhancer
From above data it results that, also for mifepristone, the enhancing activity of NIA is appreciable: in
fact the enhancing factor (FP) obtained using the No. 22L formulation is over 9 times higher than
reference solution (No. 21L formulation, using propylene glycol as solvent/enhancer).
Example 6
Percutaneous permeation of diclofenac from propylene glycol solutions
The enhancing effect of the niaouli essential oil has been also experienced on an antiinflammatory
and analgesic non steroidal drug, i. e. diclofenac. This drug, included in the FANS group, is sodium
salt of o- [ (2,6-dichlorophenyl) amino] phenyl acetic acid, obtained by synthesis in 1966. It is used
by taking advantage of its remarkable antiphlogistic, analgesic and antipyretic activity, which is
electively exerted for the therapy of rheumatic affections with pronounced antiinflammatory
component, as well as in painful state resulting having extra-rheumatic or post-traumatic origin.
Diclofenac also exhibits activity as prostaglandin synthetase (cyclo-oxygenase) inhibitor (R.
Menasses et al., Scanf. J. Rheumatology, 22,5-16 (1978); P. D. Fowler et al., J. Clin. Pharmacol., 25,
389 (1983); P. A. Todd and E. M. Sorkin, Drugs, 35,244 (1988)).
In the permeation test were compared two different solutions, a first one (No. 23 formulation)
comprising diclofenac 0,3 g and propylene glycol q. b. to 30,0 g and the second one (No. 24L
formulation) comprising diclofenac 0,3 g, niaouli essential oil 3,0 g and propylene glycol q. b. to 30,0
g. The results of permeation tests, carried out in accordance to the same protocol as above, are
reported in Table 8, while the corresponding permeation profiles are showed in Figure 5.
Table 8
Transdermal Permeation of diclofenac from solutions
Form. Enhancer J Papp Lag time Permeated FP
No. 'gcm'h' cm h'10hDrug, % 23L propylene 0,153 0,15 1,19 0,007 1 glycol2) +0,03 0,004 0,26
0,0015 24L NIA (10%) 84,11 84,6 1,60 3,35 560
6,26 6,2 0,054 0,24 41,7
Notes: 1) In both formulations the solvent was propylene glycol
2) As solvent/enhancer
303/1651
From above data it results that the enhancing activity of NIA for diclofenac is remarkable: in fact the
enhancing factor (FP) obtained using the No. 24L formulation is 560 against the reference solution
(No. 23L formulation, containing propylene glycol as solvent/enhancer).
Example 7
Percutaneous permeation of FANS from liquid formulations
The enhancing effect of the niaouli essential oil has been also experienced on complete liquid
formulations containing FANS (Ketoprofen, piroxicam, nimesulide and diethyl ammonium diclofenac).
For the permeation tests two different formulations were compared for each FANS, containing and
not containing niaouli essential oil, respectively, the per cent compositions thereof being asbelow:
Drug **
Polyethylene glycol 400 50 per cent
Pluronic L64 10 per cent
NIA 10 per cent
Ethyl alcohol q. b. to 100 per cent Drug **
Polyethylene glycol 400 50 per cent
Pluronic L64 10 per cent
Ethyl alcohol q. b. to 100 per cent
**, 2 per cent nimesulide, 2,5 per cent ketoprofen, 1,0 per cent piroxicam, 1,16 per cent diethyl
ammonium diclofenac.
The results of permeation tests, carried out according to the same protocol as above, are reported in
Table 9, while the corresponding permeation profiles are showed in Figures 6-9.
Table 9
Percutaneous permeation data of anti-inflammatory drugs obtained from liquid form@
Drug Enhancer J P Lag time FP Pe@ g cm-2h-1 cm h-1103 h @ ketoprofen nothing 0,65#0,06
0,026#0,0019 0,76#0,24 " NIA 10 % 2,83#0,44 0,116#0,0176 0,49#0,085 4,41#0,67 piroxicam
nothing 0,17#0,025 0,018#0,0026 1,25#0,144 " NIA 10 % 0,78#0,185 0,082#0,019 0,87#0,37
4,46#1,06 nimesulide nothing 0,4#0,06 0,020#0,0029 " NIA 10 % 1,97#0,088 0,102#0,0044
0,76#0,05 4,92#0,22 diclofenac nothing 0,2 0,02 1,25#0,14 diethyl ammonium " NIA 10 % 2,82#0,47
0,285#0,047 14,12#2,34 14,12#2,34
304/1651
The foregoing data demonstrate a remarkable activity of NIA in enhancing the percutaneous
permeation of FANS: in fact, using the formulations containing NIA, a flow which is 4,4,5,2,4,9 and
14,1 times higher than that obtained in absence of
NIA, for ketoprofen, piroxicam, nimesulide and diethyl ammonium diclofenac, respectively, is
obtained.
Example 8
Percutaneous permeation of FANS from semisolid formulations
The enhancing effect of the niaouli essential oil was also verified for FANS (ketoprofen, piroxicam
and nimesulide) based semisolid (gels) formulations.
For the permeation tests two different formulations were compared for each FANS, only one of which
containing niaouli essential oil, the per cent compositions being as below:
Control formulation:
Drug **
Polyethylene glycol 600 40,0
Pluronic L64 20,0
Carbopol 1342 2,0
Distilled water 10,0
Propylene glycol q. b to 100,0
NIA containing formulation
Drug **
Polyethylene glycol 600 36,0
Pluronic L64 18,0
NIA 10,0
Carbopol 1342 2,0
Distilled water 8,0
Propylene glycol q. b to 100,0 **, 2 per cent nimesulide, 2,5 per cent ketoprofen, 1,0 per cent
piroxicam.
The results of permeation tests, carried out according to the same protocol as above, are reported in
Table 10, while the corresponding permeation profiles are showed in Figures 10-12.
Table 10
Percutaneous permeation data of anti-inflammatory drugs obtained from semi-solid
305/1651
Drug Enhancer J P Lag time FP Per@ aft@ ketoprofen nothing 1,7#0,36 0,058#0,012 5,62#0,61 " NIA
10 % 52,0#2,46 2,063#0,099 7,64#0,18 30,6#1,45 piroxicam nothing 1,23#0,09 0,123#0,009
4,09#0,96 " NIA 10 % 5,53#0,38 0,553#0,058 4,29#0,87 4,49#0,3 nimesulide nothing 0,2 0,0089
0,875#0,5 " NIA 10 % 5,23#0,75 0,288#0,042 6,86#0,21 29,5#4,25
The foregoing data prove a remarkable activity of NIA in enhancing the percutaneous permeation of
FANS: accordingly, using the formulations containing
NIA are obtained enhancing factors which are 30,6, 4,49, and 29,5, for ketoprofen, piroxicam,
nimesulide, respectively, in comparison to that of control formulation.
The present invention has been described with reference to specific embodiments thereof but it is
understood that variations and modifications can be carried out by those skilled in the field without
departing form the scope thereof.
Claims:
Claims
1. Composition for the dermal and transdermal administration of pharmaceutical active principles
comprising therapeutically effective amounts of one or more of said active principles, one or more
percutaneous permeation enhancers and other possible pharmacologically acceptable adjuvants
and excipients, characterised in that said one or more percutaneous permeation enhancers include
niaouli essential oil.
2. Composition according to claim 1 wherein said pharmaceutical active principles are steroids or
non steroidal anti-inflammatory drugs (FANS).
3. Composition according to claim 1 or 2 wherein said niaouli essential oil contains from 40 to 65
weight per cent of 1,8-cineole, from 6 to 30 weight per cent of alfa-terpineol and from 1 to 20 weight
per cent of alfa-pinene.
4. Composition according to claim 3 wherein said niaouli essential oil contains from 50 to 55 weight
per cent of 1,8-cineole, from 7 to 14 weight per cent of alfa-terpineol and from 12 to 18 weight per
cent of alfa-pinene.
306/1651
5. Composition according to any one of claims 2-4 wherein said steroids are selected from the
group consisting of estrogens, androgens, progestins, steroidal anti-progestins, anti-androgen
steroids and corticosteroids.
6. Composition according to anyone of claims 24 wherein said FANS are selected from the group
consisting of diclofenac, piroxicam, ibuprofen, naproxen, ketoprofen, indomethacin and nimesulide.
7. Composition for the dermal and transdermal administration of estrogens comprising
therapeutically effective amounts of one or more of said estrogens, one or more percutaneous
permeation enhancers and other pharmacologically acceptable possible adjuvants and excipients,
characterised in that said one or more percutaneous permeation enhancers include a ternary mixture
of terpenes containing from 55 to 85 weight per cent of 1,8-cineole, from 8 to 40 weight per cent of
alfa-terpineol and from 1,5 to 25 weight per cent of alfa-pinene.
8. Composition according to any one of claims 1-7 comprising in addition propylene glycol, as
solvent and additional permeation enhancer.
9. Composition according to any one of claims 1-8 comprising from 0,5 to 40 weight per cent of said
niaouli essential oil or mixture of terpenes.
10. Composition according to any one of claims 1-9 in the form of gel. 11.
Composition according to any one of claims 1-9 in the form of transdermal therapeutic system (STT
or TTS).
12. Composition according to claim 11 included in a solid matrix type STT, mixed with one or more
suitable pressure adhesives.
13. System for transdermal and dermal administration of pharmaceutical active principles
comprising a therapeutically effective amount of one or more of said active principles and the niaouli
essential oil as a percutaneous permeation enhancer.
14. System for transdermal administration according to claim 13 wherein said pharmaceutical active
principles are steroids or non steroidal antiinflammatory drugs (FANS).
307/1651
15. System for transdermal administration according to claims 13 or 14 constituted of a laminate
comprising:
-a support layer impervious for the components
of the adjacent layer;
-a matrix constituted of a solid mixture
containing a therapeutically effective amount
of one or more of said active principles, one
or more percutaneous permeation enhancers, one
thereof being said niaouli essential oil and
one or more pressure adhesives, as well as
other possible pharmaceutically acceptable
adjuvants and excipients;
-a protective layer easy detachable from said
matrix before the application.
16. System for transdermal administration according to claim 15 wherein said niaouli essential oil
contains from 40 to 65 weight per cent of 1,8cineole, from 6 to 30 weight per cent of alfa-terpineol
and from 1 to 20 weight per cent of alfa-pinene.
17. System for transdermal administration according to claim 16 wherein said niaouli essential oil
contains from 50 to 55 weight per cent of 1,8cineole, from 7 to 14 weight per cent of alfa-terpineol
and from 12 to 18 weight per cent of alfa-pinene.
18. System for transdermal administration according to any one of claims 14-17 wherein said
steroids are selected from the group consisting of estrogens, androgens, progestins, steroidal
antiprogestins, anti-androgen steroids and corticosteroids.
19. System for transdermal administration according to anyone of claims 14-17 wherein said FANS
are selected from the group consisting of diclofenac, diethyl ammonium diclofenac, piroxicam,
ibuprofen, naproxen, ketoprofen, indomethacin and nimesulide.
20. System for transdermal administration according to anyone of claims 15-18 wherein said matrix
solid mixture contains from 0,5 to 40 weight per cent of niaouli essential oil.
308/1651
21. System for transdermal administration of estrogens comprising therapeutically effective amounts
of one or more of said estrogens and, as percutaneous permeation enhancer, a ternary mixture of
terpenes containing from 55 to 85 weight per cent of 1,8cineole, from 8 to 40 weight per cent of alfaterpineol and from 1,5 to 25 weight per cent of alfa-pinene.
22. Composition for transdermal and dermal administration of pharmaceutical active principles and
corresponding system for transdermal administration according to claims 1-21, substantially as
above described.
309/1651
54. EP1365995 - 06.09.2002
PREPARATION OF ESSENTIAL OIL COMPOSITIONS FOR POTABLE LIQUID DISINFECTION
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=EP1365995
Inventor(s):
KULKARNI MANISHA (IN); PUROHIT HEMANT J (IN)
Applicant(s):
(IN)
COUNCIL SCIENT IND RES (IN); KULKARNI MANISHA (IN); PUROHIT HEMANT J
IP Class 4 Digits: C02F
IP Class:
C02F1/00
E Class: C02F1/50; A01N65/00
Application Number:
WO2002IN00002 (20020101)
Priority Number: US20010271678P (20010227)
Family: EP1365995
Cited Document(s):
US5403587; US4966754; CH688787; GB358865; EP0842606; JP1281193
Abstract:
THE PRESENT INVENTION PROVIDES COMPOSITIONS COMPRISING AN ESSENTIAL OIL,
METHODS FOR PREPARING THE COMPOSITIONS, AND METHODS OF DISINFECTING POTABLE
LIQUID WITH THE COMPOSITIONS. THE COMPOSITION COMPRISES: (A) AN EMULSIFIER
(TWEEN SURFACTANTS); (B) AN ESSENTIAL OIL (CLOVE OIL, EUCALYPTUS OIL, KAPURTULSI
OIL).Description:
PREPARATION OF ESSENTIAL OIL COMPOSITIONS FOR POTABLE LIQUID
DISINFECTION
310/1651
Field of the invention
This invention relates to a simple and natural method for disinfection of potable liquids, such as
drinking water, by using a formulation of an essential oil derived from an herbal material. More
particularly, this invention relates to a clove oil emulsion preparation, which finds application in
disinfection of drinking water contaminated with harmful pathogens to make it potable.
Background of the Invention
Water is life-the concept coined in ancient Indian civilization. The need for pure and safe water is
universal. The quest for pure water began in prehistoric times.
Criteria of purity have become more complex, more quantitative, perhaps even more rigid, but
principles, methods and materials for water purification remained remarkably similar from the earliest
recorded data of 2000 BC down to the present time.
The ancient Indian knowledge base on antimicrobial properties of herbs available in nature was the
first documented evidence on disinfection. It is true that there were no elaborate tools to establish the
validity of these claims. The quest for pure water prompted Rishis to search for suitable herbs in
nature and inspired us to check the validity of the concept in modern context. This is the best time to
search for such formulation as the whole world is back to nature for simple remedies with no side
effects.
In modern times, there are many techniques are available for disinfection of water, and yet rural
populations, such as in India, are unable to obtain pure water free from harmful pathogens like E. coli,
Salmonella, Vibrio, and Shigella. These harmful pathogens cause many deadly diseases such as
cholera, typhoid, paratyphoid, diarrhea, dysentery, jaundice, shigellosis, etc.
There is thus a need for a simple, inexpensive and widely available purification and disinfecting
system for potable liquids, especially water, that is: effective against range of Gram positive and
Gram negative bacteria, viruses and other microorganisms; safe and free from the side-effects
caused by chemical disinfectants; costeffective and affordable; simple to use and can be carried
anywhere; and requires no special assistance, equipment or training to use.
Essential oils are extensively used medicinally in Ayurveda and
Aromatherapy for their great variety of bio-dynamic actions. Besides antimicrobial and antiseptic
properties, they are reported to be antiviral and antitoxic.
311/1651
Essential oils are used as vital constituents of many cosmetic preparations, as spices, and in
medicines. In cosmetics essential oils are mainly responsible for fragrance; in spices, essential oils
are the principle ingredients which contribute to the flavor, easy digestibility and (sometimes) to the
durability of food.
Essential oils are complex mixtures of odorous, steam volatile or extractable organic compounds,
which are synthesized by many types of plants. Typically, the principle constituents of essential oils
are aromatic compounds. Essential oils are found various parts of the plant, such as the leaves,
stems, flowers, subcuticular space of glandular hairs, in cell organelles, in idioblasts, in excretory
cavities, canals, etc. Essential oils may also be found in heartwoods.
Chemically and biogenetically, the natural product class"Essential oils"is heterogenous. Mono-,
sesqui-and di-terpenoids (mevalonic acid-derived constituents); phenylpropanoids (cinnamic acidderived compounds) and alkane derivatives (alkanes, alkenes, alkynes, alkanols, alkanals, alkanoic
acids: mostly acetogenins) are by far the most ubiquitous components of essential oils.
Essential oils belong to the so-called"Natural Products"or secondary metabolites of plants. Usually
the secondary metabolites are not directly involved in growth and reproduction, but rather in fitness
for Life. In other words, secondary metabolites are more involved in the ecology than in the
physiology of plants.
Essential oils have long been used as medicines, and are now gaining increased acceptance as
aromatic therapies, and as dietary and nutritional supplements.
For example, certain names for the clove from India, like"Tikslma-pushpa","Ruchiram", "Girvana
Pushparna"suggest its use as an appetizer, digestive cordial, antitissusive and as mouth freshener.
Indications are toothache (local application), indigestion/flatulence, nausea, halitosis and
hyperacidity. It is also used as anesthetic and antiseptic in dentistry.
In the doses commonly used for the above-described indications, no adverse reactions have been
reported. In a recent study, clove oil used in large doses produced edema, congestion and necrosis
(see http ://Ayurvedwebline. com).
312/1651
Essential oils are also widely used in the food industry. For example, clove oil or clove bud oil is
used as a compounded oil for the flavouring of pastry, in special sauces and as a condiment. The
dried product is used directly in compounded infusions for liqueurs and bitters. The oil is typically
used in following proportions:
Non-alcoholic beverages 3.1 ppm
Alcoholic beverages 300 ppm
Ice-cream 13 ppm
Candy 320 ppm
Baked goods 37 ppm
Gelatins and puddings 0.3-5.0 ppm
Chewing gum 1800 ppm
Condiments 55 ppm
Meats 75 ppm
Spiced fruits 830 ppm
Jellies 7.3 ppm
Furthermore, clove oil preparations are commonly accepted in the Ayurvedic system, as a safe and
accepted medicine.
Antibacterial activity of clove oil has been reported against V. cholarae,
Gartner's Bacillus and Swine Erysipelas bacteria and Brucella and Mycobacterium,
Trichophyton, Achorion and Epidermophyton. Activity of clove oil volatile fractions is reported by S.
Agnihotri and A. D. B. Vaidya against E. coli, S. aureus, Bacillus subtilis, S. typhi, P. aeruginosa, S.
flexneri and P. vulgaris. (See The Wealth of India, Raw Materials,
Volume X, p. 93-99, a CSIR publication; World Economic Plants, A standard Reference, 1999, p. 487;
and Cultivation and Utilization of Aromatic Plants, edited by C. K. Atal and
B. M. Kapur, RRL Jammu Tawi, CSIR Laboratory, 1982.).
Brief Description of the Figures
FIG. 1A shows the disinfection activity of a 1: 20 dilution of clove oil emulsion E34.
FIG. 1B shows the disinfection activity of a 1: 50 dilution of clove oil emulsion E34.
313/1651
Brief Description of the Tables
Table 1 depicts the results of essential oil samples screened for antibacterial activity against test
organism E. coli. The oil samples tested were clove oil, eucalyptus oil, sandal oil, KapurTulsi oil and
ropan oil in various hydro-alcoholic dilutions by the bore well method.
Table 2 depicts the effect of clove oil on different organisms like E. coli, Salmonella typhi and Vibrio
cholarae in various hydro-alcoholic dilutions.
Table 2A depicts the comparison of activity of clove oil emulsions 1: 10,1: 20,1: 30,1: 40 and 1: 50
with the standard antibiotics available in the market. The activity was compared by Bore well method,
Zones of inhibition were compared for each emulsion with that of standard antibiotic.
Table 3 displays the results of inhibitory effect of clove oil 1: 100 hydro-alcoholic dilutions on log
phase and stationary phase cells of E. coli by serial dilution method at doses of 100tti, 501AI, 25pLI
and 12.5u1.
Table 4 depicts different percentages of detergent Tween 20 in clove oil emulsion preparations. The
detergent percentage was varied as 2,2.5,3.5 and 4.0 %.
Table 5 depicts the different time-periods for which the clove oil emulsion was sonicated (2,5,7,10
and 15 minutes).
Table 6 and Table 7 depict clove oil emulsion preparations with varying percentages of groundnut oil
(saturated oil). The different percentages of groundnut oil used were 50,20, 10,4,2,1 (Table 6) and
0.75,0.5,0.2 and 0. 1 (table 7) with a sonication time of 2 minutes and 2% of Tween 20.
Table 8 depicts the Clove oil emulsions with varying concentrations of unsaturated corn oil. The
different percentages were 1.0,0.75,0.5,0.2 and 0.1.
Table 9 depicts preparation of clove oil emulsion with 2% Tween 20 and 0.1% carrier
Saffola oil at pH 9.0 at different concentrations of an electrolyte NaCl solution. The concentrations of
NaCl used were 0. lppm, 0.05 ppm, 0.02 ppm and 0.01 ppm.
314/1651
Table 10 depicts the preparation of clove oil emulsion using an electrolyte Na2HPO4 solution in the
same conditions and concentration range as stated above for Table 9.
Table 11 depicts the preparation of clove oil emulsion using NaCl solution (O. lppm, 0.05 ppm, 0.02
ppm and 0.01 ppm) by diluting the emulsion with pH 9.0 water adjusted by using KOH solution.
Table 12 depicts the preparation of clove oil emulsion using Na2HP04 solution (0.1,0.05, 0.02,0.02
ppm) by diluting the emulsion with pH 9.0 water that was adjusted to pH 9.0 by using KOH solution.
Table 13 depicts the overall inhibitory effect of clove oil emulsions in sterile drinking water (D. W.)
innoculated with E. coli.
Table 14 depicts the inhibitory effect of clove oil emulsions prepared using NaCl and
Na2PH4 after standardizing conditions like emulsifying agent percentage, sonication time, carrier oil
percentage and dilutions in water.
Table 15 depicts the percentage removal of E. coli by different clove oil emulsions in 1L spiked water
Table 16 depicts the percentage removal of E. Coli by different clove oil emulsions in 1L spiked water.
Summary of the Invention
It has now been found that essential oils may be used as disinfectants for potable liquids, such as
water.
In one aspect, the invention provides a composition for the disinfection of a potable liquid,
comprising an essential oil; one or more emulsifiers ; optionally an electrolyte; and optionally a carrier
oil. In one embodiment of the invention, use of carrier oil is preferred, as it substantially favors a
stable emulsion preparation. An unsaturated carrier oil, such as Saffola oil (unsaturated corn oil) is
preferred.
In another aspect, the invention provides a method of disinfecting a potable liquid, namely water,
comprising providing a composition comprising an essential oil; one or more emulsifiers; optionally
an electrolyte; and optionally a carrier oil; and contacting the composition with the potable liquid for a
sufficient time to disinfect the potable liquid.
315/1651
As used herein, a"sufficient time to disinfect a potable liquid"means the length of time in which at
least about 60%, preferably at least about 80%, more preferably at least about 90% of the
microorganisms present in the potable liquid are killed, removed, or growthinhibited.
As used herein, potable liquid"is a liquid intended for consumption by a human being or animal, and
includes liquid that may be contaminated with one or more microorganisms.
As used herein,"disinfect"means the killing, removal or inhibition of growth of microorganisms found
in a potable liquid.
In a further aspect, the invention provides a method for preparing a composition for the disinfection
of potable liquids, comprising making an oil-in-water emulsion of (1) an essential oil; (2) one or more
emulsifiers; (3) optionally an electrolyte; and (4) optionally a carrier oil. Preferably, the potable liquid
is water.
In one embodiment, the invention provides a composition for disinfecting a potable liquid, said
composition comprising a emulsion of an essential oil, emulsifier, optional carrier oil, and electrolyte
and water where the emulsion is effective at a concentration at a composition: potable liquid ratio of
1: 10000 to 1: 100000.
In a still further aspect of the invention, the composition for disinfecting potable liquid is prepared by
mixing the essential oil, emulsifier, optional carrier oil, optional electrolyte and sterile water adjusted
to pH range 8.5 to 9.5, to obtain an oil-in water emulsion. Thus, in one embodiment of the invention,
the composition thus prepared has a shelf life of about one year.
In another embodiment, the invention provides a composition for the disinfection of up to 1L of
potable liquid, comprising an essential oil, an emulsifying agent and a carrier oil along with an
electrolyte.
In another embodiment of the invention, the composition comprises a clove oil emulsion comprising
Tween20 and Saffola oil with Na2BO4 at pH 9.0.
In another embodiment, the composition comprises a clove oil hydro alcoholic dilutions effective in
disinfecting drinking water contaminated with E. coli, Salmonella typhi and Vibj io cholarae, for
example at 1: 5000,1: 5000 and 1: 100 final dilutions respectively.
316/1651
Detailed Description of the Invention
It has now been found that essential oils may be used as disinfectants for potable liquids, such as
water. Potable liquids may be contaminated with any number of harmful microorgansims, including
bacteria, viruses, and parasites. It is desirable to remove these microorganisms before humans or
animals consume the liquid.
Thus in one aspect, the invention provides a composition for the disinfection of a potable liquid,
comprising an essential oil; one or more emulsifiers; optionally an electrolyte; and optionally a carrier
oil. The compositions of the invention are useful in removing, killing or inhibiting the growth of various
microorganisms in potable liquids, for example in drinking water, thus making the liquid safe for
human or animal consumption. For example, the compositions of the invention are useful in
disinfecting potable liquids contaminated with fecal coliform bacteria, (e. g., E. coli),
Salmonella, Vibrio, Shigella, S. aureus, Bacillus subtilis, S. typhi, P. aeruginosa, S. flexneri and P.
vulgaris.
Essential oils are available from a wide variety of plant species. Essential oils are typically mixtures
of organic aromatic and other compounds that are extractable from plant material by methods such
as steam distillation, cold pressing, C02 extracted, or extraction with organic solvents (e. g.,
hexanes), as are known to those of ordinary skill in the art.
Examples of essential oils useful in the present invention include, but are not limited to extracts from
Bergamot (citrus bergamia) ; Cedarwood (cedrus deodara and junipers virginiana) ; Cinnamon leaf
(cinnamomum zellanicum ceylon) ; Clove or clove bud (eugenia caryophyllata madagascar extra ;
Syzygium aromaticum l5./Eugenia aromatic L); Eucalyptus (eucalyptus globulus & radiata) ;
Geranium (pelargonium graveolens madagascar bourbon) ; Grapefruit (citrus paradisi) ; Lavender
(lavendula officinalis France) ; (organum marjorana) ; Patchouli (pogostemon cablin E. India dark),
Peppermint (mentha piperita) ; Rosemary (rosmarinus of'ficinalis) ; Sandalwood (aniba rosaeodora).
Other essential oils useful in the present invention include Sandal oil, KapurTulsi oil, and Ropan oil.
Clove oil (especially from Syzygium aromatic L. lEugenia aromaticum L), eucalyptus oil and
KapurTulsi oil are preferred.
A particularly preferred essential oil is clove or clove bud oil from
Syzygium aromaticum L./Eugenia aromaticum L, commonly known as Laung. Clove oil is mainly
comprised of eugenol, eugenol acetate and caryophyllene.
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Clove bud oil is obtained by water (e. g., steam) distillation of buds in yields ranging from 15-18%. It
is a clear, mobile liquid nearly colourless to yellow-brown. It tends to darken on ageing. The tinctures,
extracts and oleoresins are also useful in the present invention.
As mentioned above, essential oils contain a mixture of chemicals. For example, clove oil contains
free eugenol 70-90% (CloHI202, b. p. 251-254 C), eugenol acetate 2-17% and caryophyllene
(CloHi604 chiefly the Form) as main constituents. Both eugenol and eugenol acetate contribute to
commercial value of clove oil so the total phenol content is reported as eugenol. Eugenol is widely
used in pharmaceutical preparations, in perfumes for soaps and cosmetics and as a flavouring agent
in all kinds of foods, meats, sausages and sauces etc. Eugenol acetate is found in nature in clove
bud oil and is prepared by acetylation of eugenol. The compound, which is responsible for the
characteristic aroma of clove oil, is methyl-n-amyl ketone.
The structure of eugenol is given below:
Other common chemical constituents of essential oils are citral (geranial and neral isomers), limonen,
linalyl acetate and estragole (methyl chavicol), mono-, sesqui-and di-terpenoids (mevalonic acidderived constituents); phenylpropanoids (cinnamic acid-derived compounds) and alkane derivatives
(alkanes, alkenes, alkynes, alkanols, alkanals, alkanoic acids: mostly acetogenins). It is understood
that the term "essential oil"as used herein includes the naturally occurring extractable plant oils,
mixtures thereof, or one or more of the components found in extractable plant oils, whether naturally
or artificially synthesized. The term also includes derivatives and analogs of the components found in
extractable plant oils.
The compositions of the invention comprise an emulsifier or surfactant that allows the formation of
oil-in-water emulsions and that are regarded as safe for human consumption at the concentrations
used in the invention. The terms"emulsifier"and "surfactant"are used interchangeably throughout the
specification.
Any suitable emulsifier may be used, for example the Tween, Myrj and
Bryj surfactants, poloxamers and their derivatives, polyoxyethylene 50 stearate, polyoxyl 35 castor oil,
polyoxyl 10 oleyl ether, polyoxyl 20 cetostearyl ether, polyoxyl 40 stearate, polysorbate 20,
polysorbate 40, polysorbate 60, polysorbate 80, propylene glycol diacetate, propylene glycol
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monostearate, sodium lauryl sulfate, sodium stearate, sorbitan monolaurate, sorbitan mono-oleate,
sorbitan mono-palmitate, sorbitan monostearate, stearic acid, and emulsifying wax. The Tween
surfactants, in particular Tween20, are preferred.
The emulsifier may be present in any concentration sufficient to allow formation of a stable oil-inwater emulsion from the essential oil and optional carrier oil.
For example, the amount of emulsifier may be from. 5 to 10%, preferably from 2 to 4 % (w/w) of
essential oil in the composition. Preferred is a composition comprising 2% Tween20.
The compositions of the invention may optionally comprise a carrier oil. In some instances, carrier
oils allow the formation of finer and more stable emulsions than may be achievable with the essential
oil alone. Suitable carrier oils include vegetable and other plant oils; for example Sweet Almond Oil
(Prunus amygdalus var. dulcis) ; Apricot
Kernel Oil (Prunus armeniaca) ; Avocado Oil (Persea americana) ; Black Currant (Ribes nigrum) ;
Borage Seed Oil (Borago officirlalis) ; Canola Oil (Brassica napus/campestris) ;
Rapeseed Oil; Castor Oil (Ricinus common) ; Coconut, Copra (Cocos nucifera) ; Corn Oil (Zea mays)
Evening Primrose Oil (Oenothera biennis) ; Flax Seed Oil (Linum usitatissimum) ; Foraha Oil
(Calophyllum) (Calophyllum inophyllum) ; Grapeseed Oil (Vitis vinifera) ; Hazelnut Oil (Corylus
Avellana) ; Kikui Nut (Aleurites moluccana) ; Macadamia
Nut Oil (Macadami integrifolia, tetraphylla, or ternifolia) ; Olive Oil (Olea europaea) ;
Peanut Oil (Arachis hypogeae) ; Rose Hip Seed Oil (Rosa Mosqueta, R. Rubignosa, R. rubirosa) ;
Safflower Oil (Carthamus tinctorius) ; Sesame Oil (Sesamum indium) ; Soya
Bean Oil (Glycine max, G. soya) ; Sunflower Oil (Helianthus annuus) ; wheat germ oil, kardi oil, sun
flower oil or mixtures thereof. The carrier oil may be saturated, unsaturated, or a mixture of saturated
and unsaturated oils. Preferred are unsaturated oils, such as
Saffola (unsaturated corn oil), kardi oil and sun flower oil, and saturated oils such as groundnut oil.
Suitable amounts of carrier oil for use in the compositions of the invention may be determined by one
of ordinary skill in the art, for example by testing the composition according to the procedures
outlined in the General Methodologies below.
For example, the composition of the invention may comprise carrier oil in the range of about 0.01 to
50 % (w/w) of the composition, preferably from 2 and 20% or from about 0.1 to 1%. Particularly
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preferred are a carrier oil concentrations of 0.1,0.25,0.5,0.75,1 and 5.0%, for example Saffola oil at
0.1%.
The compositions of the invention may optionally comprise an electrolyte.
Suitable electrolytes include NaCl and Na2HP04, with Na2HP04 as the preferred electrolyte. Other
electrolytes are contemplated. Suitable electrolyte concentrations may be determined by one of
ordinary skill in the art, by testing compositions according to the procedures outlined in the General
Methodologies below.
In preferred compositions, the electrolyte is present in the composition in the range from 0.01 ppm
to 0.1 ppm. A preferred electrolyte concentration in the compositions of the invention is 0. lppm, for
example 0.1 ppm of Na2HP04.
The pH of the compositions of the invention may be any pH at which the essential oil emulsion
retains its disinfection activity. One of ordinary skill in the art may ascertain appropriate pH's by
testing compositions under the procedures outlined in the
General Methodologies below. The pH of the compositions of the invention may range, for example,
from about 6.0 to about 10, preferably from about 8.5 to about 9.5. Higher or lower pH's are
contemplated.
The compositions of the invention may be used to disinfect potable liquids without first being diluted,
or may be diluted before use. For example, dilutions of 1: 10,1: 100,1: 500 or 1: 5000 (with respect to
the original emulsion concentration) may be used.
Other dilutions are contemplated. One of ordinary skill in the art may ascertain appropriate dilutions
by testing compositions under the procedures outlined in the General
Methodologies below.
For example, the amount of emulsion used for disinfecting the potable liquid may be in the ratio 1:
1,000 to 1 : 200,000, preferable from about 1 : 10,000 to 1: 100, 000 with respect to the final volume
of the potable liquid to be disinfected.
In another aspect, the invention provides a method of disinfecting a potable liquid, comprising
providing one or more compositions of the invention (or dilutions thereof, as described above) and
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contacting the composition with the potable liquid for a sufficient time to disinfect the potable liquid.
As used herein, a"sufficient time to disinfect a potable liquid"means the length of time in which at
least about 60%, preferably at least about 80%, more preferably at least about 90% of the
microorganisms present in the potable liquid are killed, removed, or growth-inhibited. One of ordinary
skill may determine what is a sufficient length of time for contacting the composition with the potable
liquid by testing the potable liquid according to the procedures outlined in the
General Methodologies below. For example, the compositions of the invention may be contacted with
the potable liquid to be disinfected for about 3 to about 24 hours, preferably from about 6 to about 8
hours, particularly preferably for about 6 hours.
In a further aspect, the invention provides a method for preparing a composition for the disinfection
of potable liquids as described above, comprising making an oil-in-water emulsion of (1) an essential
oil; (2) one or more emulsifiers; (3) optionally an electrolyte; and (4) optionally a carrier oil. Any
suitable method for forming the emulsions may be used, as are familiar to those of ordinary skill in the
art; for example, sonicating, shaking, stirring, etc. Preferably, the compositions are prepared by
sonication.
In particular preferred embodiments, sonication time of about 2 minutes at each step is suitable.
The invention will be illustrated with the following non-limiting examples.
Examples
General Methodologies :
The general methodology adopted for the preparation of inocula of the test bacteria, E. coli and the
antibacterial assay methods mainly"bore-well"and serial dilution methods are explained below as
used in the present invention. Also explained herewith is the procedure for the preparation of
essential oil emulsions according to the invention; and the testing and detection methods of the water
samples after disinfection. The present invention in its most preferred aspect is the clove oil emulsion
preparation comprising the desired proportion of edible detergent, carrier oil and the electrolyte
solution with application in disinfection of drinking water.
In preparation of inocula for culturing E. coli, Luria-Bertani (LB, HiMedia) media was used. An
overnight culture of E. coli was grown in LB at 37 C at 150 rpm and was diluted to five times by LB;
the diluted culture was incubated in the same conditions until the optical density (OD) reached 0.5.
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Various compositions of essential oils (described below) were screened for antibacterial activity by
two methods; viz. bore-well method and serial dilution method.
In the bore-well method, a 1% culture of E. coli from log phase was inoculated into molten LB Agar
growth medium, and plates were poured. This gave final cell density of about 109 cells per ml. After
solidification of the medium, wells were made in the plate with the sterile borer. I OOPI of each
essential oil composition was placed in the wells. The plates were incubated at 37 C overnight. 50%
ethanol was placed in the control wells. The plate showed clear zone of inhibition surrounding the
wells where there was inhibition of the growth of E. coli, confirming the antibacterial effect.
In serial dilution method, E. coli culture in log phase growth was diluted in
LB broth to 103 cells/ml. One ml of this was taken in each tube, except the first tube in which 2ml
was taken. 100p1 of the essential oil compositions were added to the first tube.
One ml from the first tube was transferred to the second and similarly diluted into all the tubes so that
each tube contained half the concentration of the composition than the previous tube. Five dilutions
were likewise made. The last tube showing no turbidity ; i. e., growth in the tube was taken as the
Minimum Inhibitory Concentration (MIC) of the composition.
The common acceptance of clove oil by the general population, its safety as well as the potency to
kill the gram positive and gram negative bacteria makes the clove oil preferred antibacterial agent for
water disinfection.
The essential oils are not soluble in water and oil floats on the surface of water layer. To make the
clove oil miscible in water for its uniform dispersion throughout water, oil-in-water type emulsions
were prepared by using emulsifying agent, edible grade detergent.
Commercially available I. P. grade clove oil, manufactured by Dabur India
Ltd., was used in all the experiments. Five ml packages were procured for the experiments; for every
emulsion preparation 5ml constant volume was used.
To prepare the emulsion, clove oil I. P. 5ml setting was mixed with 2%
Tween 20 (1001l1) and 0. 1% saffola oil (5p1), sonicated for 2 mins between 2 and 3 of the
sonicator (make-Cole-Parmer, Torbeo, Ultrasonic Processor, 36800 Series) and diluted with sterile
distilled water to different dilutions as shown in Table 13.
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For better micelle preparation and subsequently stable emulsion it was believed that at pH 9.0 of
clove oil emulsion the molecule of eugenol will be in ionized form. With very low concentration of
electrolyte NaCl or Na2HP04 solution along with 2%
Tween 20 and carrier oil 0.1% Saffola oil forms better micelle. In these emulsions, the mixture of clove
oil, Tween 20 and saffola oil was first sonicated as above, diluted 1: 10 by sterile distilled water, and
the pH of the milky emulsion was adjusted to 9.0 by KOH solution. The concentrations of NaCl used
were O. lppm, 0.05 ppm, 0.02 ppm and 0.01 ppm
The method was then modified so that instead of changing the pH of diluted emulsion, dilutions were
made by pH 9.0 water. For 0.1,0.05,0.02 and O. Olppm each of NaCI and Na2HP04 solution
appropriate volumes were taken from lOppm stocks and sonicated for 2 minutes again.
As can be seen from the results in Table 13 and 14, the inhibitory effect of emulsions was
substantially enhanced with the use of low concentration of electrolytes at pH 9. 0.
To test the effect of the emulsions in contaminated water, lml, 100ml and 1L volumes drinking water
was sterilized by autoclaving and innoculated with E. coli. The cell concentrations used were: 103
cells/ml for lml ; 104 cells/100ml for 100ml ; and 105 cells/L for 1 liter.
As specified above, 2 ml E. coli culture in log phase growth at 0.5 OD was centrifuged and the pellet
suspended in lml of sterile distilled water in eppendorf tube by vortexing to give 109cells/ml. From
this appropriate dilutions were made in sterile distilled water to obtain 105 cells/ml (for 100ml
experiments) and 106 cells/ml for (1L experiments).
100p1 of the appropriate dilution was used for each flask to get final concentrations of 104
cells/100ml and 105 cells/L, respectively.
Disinfection activity was assayed by adding an aliquot from the reaction mixture in 2X LB medium
after a contact period of 3 hrs, and incubating the LB tubes at 37 C at 15rpm overnight. The tubes
were then checked for the presence of E. coli growth.
Disinfection activity was also assayed by the"Membrane Filter Technique", in which 100ml of the
reaction volume was filtered through sterile membrane filters (Millipore, size 0.451lm) and the filter
discs were placed on MEC agar (Hi-media) plates.
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The plates were kept at 44.5 C overnight, the colonies were treated with urea substrate for 15
minutes and the yellow-brown colonies were counted. (See Standard Methods of Water and Waste
water Analysis, 17th edition, Section 9213D the disclosure of which is herein incorporated by
reference.)
Example 1
Essential oil compositions were screened for antibacterial activity against the test organism E. coli
(Tablel). Clove oil, eucalyptus oil, sandal oil, KapurTulsi oil, and
Ropan oil compositions were tested by bore well method as described earlier. Clove oil showed very
good disinfection activity against the E. coli (Photographl) at all dilutions.
Eucalyptus oil showed activity in a neat sample, KapurTulsi oil showed activity up to a 1: 10 dilution,
while other compositions showed no activity in hydro-alcoholic dilutions against E. coli.
Table 1: Essential oil samples tested for antibacterial activity against test organism
E.coli
Oil Sample Effective Dose (HA dilution)
Neat 1: 10 1: 100 1: 200 1: 500
Clove + + + + +
OilEucalyptus oil +
KapurTulsi oil + +
Sandal oil
Neem oil - - - Ropan oil - - - Example 2
Clove oil hydro-alcoholic dilutions were tested against Salmonella typhi and
Vibrio cholarae along with E.coli, at different doses by the serial dilution method. Clove oil was found
to inhibit E. coli and Salmonella typhi growth at all dilutions, while Vibrio cholara growth was inhibited
up to dilutions of 1: 200 (see Table 2).
Table 2: Effect Clove oil hydro-alcoholic dilutions against E. coli, S. typhi & V. cholarae
Organism Effective Dose (HA dilution)
Neat 1: 10 1: 100 1: 200 1: 500 1 : 2000 1 : 5000
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E. coli + + + + + + +
Salmonella typhi + + + + + + +
Mibrio cholarae + + +
Example 3
The activity of clove oil emulsions 1: 10 (10%), 1: 20 (5%), 1: 30 (3.33%), 1: 40 (2.5%) and 1: 50 (2%)
was compared with the standard antibiotics available in the market. The activity was compared by
Bore well method by placing 100 ttl of each emulsion. Zones of inhibition were compared for each
emulsion with that of standard antibiotic.
Table 2A: Comparison of inhibitory activity of clove oil emulsions with the standard antibiotics
available in the market against E. Coli.
Zone of Inhibition (in mm)
Anti biotic
Antibiotic Clove oil emulsion
1: 10 1: 20 1: 30 1: 40 1: 50
Penicilin G - 16 14 12 10 8
Erythromycin 10 16 14 12 10 10
Ampicillin 14 16 14 12 10 10
Tetracycline 24 16 14 12 10 9
Gentamycin 24 16 14 12 11 10
Kanamycin 30 16 14 12 10 10
Chloromphen35181412118
icol
Example 4
As the bacterial cells in the drinking water will essentially be in stationary phase, the experiments
were performed to test if there was a different inhibitory dose requirement for log phase as opposed
to stationary phase cells. The experiment was carried out by serial dilution method. It was observed
that the dose required for both types of cells is the same, as shown in Table 3.
Table 3: Effect of Clove oil 1: 100 hydro-alcoholic dilutions on log phase and stationary phase cells
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E.coli Control 100 l 50 l 25 l 12.5 l
Log phase-+ +-cells
Stationary-+ +phase cells
Example 5
Five emulsions containing different percentages of Tween20 (E1 to E5; see
Table 4) were made and tested at different dilutions for the ability to disinfect 1 ml, 100 ml, or 1 L of
drinking water (D. W.) innoculated with E. coli (see General Methodologies, above).
After a 6 hr. contact period, 1 ml of each sample was transferred to a 2X LB tube and monitored for
growth as described in the General Methodologies above. Disinfection activity of the diluted
emulsions is given in Table 13.
Table 4: Clove Oil Emulsions with Different percentages of Tween 20
Emulsion Emulsion
Constituents El E2 E3 E4 E5
Clove 5ml 5ml 5ml 5ml 5ml
Oil neat
Tween 20
Percentage 2 2. 5 3.0 3.5 4.0
Emulsion E5 was also tested by varying the number of E. coli in the reaction volume (103 cells,
2x103 cells and 104 cells) with negative results.
Example 6
The dilutions of emulsion E2 1: 10,1: 100 and 1: 500 with 2.5% Tween 20 showed positive results in 1
ml while in 1L reaction volume at the doses of 100 ut, 500 ut and 1 ml gave negative results after
contact period of 3 hrs and 6 hrs.
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Similarly the emulsions E3 and E4 dilutions showed inhibition of E. coli in 1 ml volume and showed
negative results when tested in 1L water as shown in Table 13.
The emulsion E5 dilutions 1: 10,1: 100,1: 500 and 1: 5000 with 4% Tween 20 were tested in 1 ml, 100
ml and 1L volumes displayed positive results in 1 ml at 100 ml at 100 u. l and in 1L at 100 ul, 500 ul
and 1 ml displayed negative results as shown in Table 13.
Emulsions E5 were also tested by varying the cell number of E. coli in the reaction volume to 103
cells, 2x103 cells and 104 cells with negative results.
Example 7
Emulsions E6 to E10 were prepared by changing the sonication time (see Table 5).
The emulsions were tested in 100ml D. W. at a 1: 20 dilution test the effect of different sonication
times on the disinfection activity of the emulsions. As shown in Table 13, there was no difference in
the inhibitory effect with higher sonication time; therefore sonication time of 2 minutes at every step
was thought to be sufficient for emulsion preparation.
Table5 : Different sonication times in Clove Emulsion Preparation
Emulsion Emulsion
Constituents E6 E7 E8 E9 E10
Tween 20
Percentage 2 2.5 3.0 3.5 4.0
Sonication
Time 2 5 7 10 15
Example 8
Emulsions El l-E15 (Table 6) with 2% Tween 20 and different percentages of groundnut oil were
tested for the disinfection activity in 100ml. Disinfection activity of E12 was observed, but was nonreproducible, so"-"activity is indicated in Table 13 for this emulsion.
Table 6: Clove oil emulsion with varying concentrations of groundnut oil (saturated oil)
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Emulsion Stock Emulsion
Constituents
Ell E12 E13 E14 E15
Clove
Oil neat 5ml 5ml 5ml 5ml 5ml
Tween 20 100 l 100 l 100 l 100 l 100 l
(2%)
Groundnut250 l 200 l 150 l 100 l 50 l
Oil 5% 4% 3% 2% 1%
Disinfection activity of emulsions El l-E15 is shown in Table 13. Note that in 1L volume negative
results were observed for these emulsions even at 2 ml dose of emulsions E16-E20 with groundnut
oil concentrations below 1% (Table 7) when tested in the 100 ml reaction volume yielded positive
effect at the doses of 50 ul and 500 Ill after 6 hrs contact period.
Table 7: Clove oil emulsion with varying concentrations of groundnut oil (saturated oil)
Emulsion Stock Emulsion
Constituents E16 E17 E18 E19 E20
Clove
Oil neat 5ml 5ml 5ml 5ml 5ml
Tween 20 (2%) 100 l 100 l 100 l 100 l 100 l
Groundnut 50 l 33.5 l 25 l 12.5 l 5 l
Oil 1% 0.75% 0.5% 0.25% 0.1%
These results suggest that a lower percentage of carrier oil substantially enhanced the stability and
activity of the emulsion, while too high a percentage of carrier oil facilitates the growth of bacteria.
Example 9
Clove oil emulsion E20 (see Table 7) with 2% Tween 20, sonication time of 2 minutes, and 0.1%
groundnut oil were diluted 1: 20 and tested in 100ml water with 104 cells of E. coli with an overnight
contact time. These emulsions showed positive results by 2X
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LB method and the Membrane Filter Technique. As described above, the filter discs with the filtered
samples were placed on MEC agar plates at 44. 5 C overnight and the yellow colonies counted. In
100ml reaction volume, E20 at the doses of 50 u1, 100111, 200, u1 and 500 l gave positive results
(Table 13).
Example 10
Emulsions with 0.1% Saffola oil were found to be more fine and stable as compared to the groundnut
oil, so the emulsions with 0.1% Saffola oil are preferred.
Emulsion E21 with 0.1% unsaturated, Saffola oil (Table 8) displayed good disinfection activity results
in lml volume as shown in Table 13. In 100 ml reaction volume E21 yielded positive activity at doses
of 50 RI and 1001l1 while in 1L reaction volume zip and lml dilutions of 1: 10 completely inhibited
E.coli after 6 hrs contact period. Other dilutions were also effective to large extent.
Table 8: Clove oil emulsion with Saffola oil (unsaturated corn oil)
Emulsion Stock Emulsion
Constituents E21
Clove Oil neat 5ml
Tween 20 (2%) 100p1
Saffola oil 5, u1, 0.1%
Example 11
Clove oil emulsions E22-E26 were prepared using an electrolyte NaCl solution, along with 2% Tween
20 and 0.1% carrier Saffola oil at pH 9.0. Concentrations of NaCl used were O. lppm, 0.05 ppm,
0.02 ppm and 0.01 ppm (Table 9). Disinfection activities of emulsions E-22-E-26 are shown in Table
13.
Table 9: Preparation of Clove oil emulsion using NaCI solution
Emulsion Stock Emulsion
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Constituents E22 E23 E24 E25
Clove 5ml 5ml 5ml 5ml
Oil neat
Tween 20 (2%) 100 l 100 l 100 l 100 l
Saffola oil 0.1% 5 l 5 l 5 l 5 l
NaCI sol'n O. lppm 0.05 ppm 0.02 ppm 0. 01 ppm
(lOppm
stock)
Example 12
Clove oil emulsions E26-E29 were prepared using an electrolyte Na2HP04 solution (O. lppm, 0.
05ppm, 0.02 ppm and 0.01 ppm) (Table). Disinfection activity of these emulsions are shown in
Table 13.
It was observed that the better emulsions were obtained when using Na2HP04 solution rather than
NaCI. Antibacterial effect was substantially enhanced in 0.1 and 0. 05ppm of the electrolyte than
the lower concentrations.
The 0. lppm Na2HP04 solution in the clove oil emulsion at pH 9.0 is the desired electrolyte for the
stable and effective emulsion preparation.
Tab1e10 : Preparation of Clove oil emulsion using Na2HP04 solution
Emulsion Stock Emulsion
Constituents E26 E27 E28 E29
Clove 5ml 5ml 5ml 5ml
Oil neat
Tween 20 (2%) 1001 100 l 100 l 100 l
Saffola oil 5 l 5 l 5 l 5 l
0.1%
Na2HP04 soln O. lppm 0.05 ppm 0.02 ppm 0.01 ppm
Example 13
330/1651
Clove oil emulsions E30-E33 were prepared using O. lppm NaCI solution by diluting the emulsion
with pH 9.0 water instead of adjusting the pH of diluted emulsion (Table 11). These emulsions were
tested for their disinfecting effect. The emulsions at a 1: 10 dilution were observed to disinfect 100ml
and 1L D. W. water after 6 hrs contact period as shown in Table 13.
Similar results were observed in 1: 20,1: 50 and 1: 100 dilutions of these emulsions, which inhibit
growth above 90% of the E. coli cells in the given contact period.
Table 11 : Preparation of Clove oil emulsion using NaCl solution dilution by pH 9.0 water
Emulsion Stock Emulsion
Constituents
E30 E31 E32 E33
Clove 5ml 5ml 5ml 5ml
Oilneat
Tween 20 100 l 100 l 100 l 100 l
(2%)
Saffola oil 5 l 5 l 5 l 5 l
0.1%
NaCI soln
(10ppm stock) 0. lppm 0.05 ppm 0. 02 ppm 0. 01 ppm
Example 14
Clove oil emulsions E34-E37 were prepared using 0. lppm Na2HP04 solution by diluting the
emulsion with pH 9.0 water instead of adjusting the pH of diluted emulsion (Table 12). These
emulsions were tested for their disinfecting activity in 100ml and 1L
D. W. Disinfection activity of emulsions E34-E37 are shown in Table 13.
It was observed that these emulsions with 2% Tween20,0.1% Saffola oil, 2 minutes sonication time at
each step and O. lppm of Na2HP04 at pH 9.0 performed well in disinfection of drinking water, as
shown in Table 14.
Tablel2: Preparation of Clove oil emulsion using Na2HP04 solution, dilution by pH 9.0 water
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Stock Emulsion
Emulsion
Constituents E34 E35 E36 E37
Clove Oil 5ml 5ml 5ml 5ml
Neat
Tween 20 (2%) 100 l 100 l 100 l 100 l
Saffola oil 0. 1% 5 l 5 l 5 l 5 l
Na2HP04 soln 0. 1 ppm 0. 05 ppm 0.02 ppm 0.01 ppm
The results in 1: 20 and 1: 50 dilutions shown that the lower dose of emulsion also reduces the
bacterial population to considerable extent and in the safe limits as shown in Fig. 1A (Photograph 7)
and Fig. 1B (Photograph 8).
Table 13 : Disinfection Activity of Clove oil Emulsion on sterile D. W. Inoculated with E. co
Stock Inhibitory Effect of Emulsions
Emulsi Working (Contact time 6h)
on No. Diluted Reaction volume
emulsions
DW 1ml DW 100ml DW 1000ml
10 l 50 l 10 l 50 l 100 l 500 l 1ml
100 l 100 l
El 1: 10 - ++ ++ ++ ++ - - 1:100 - ++ ++ + ++ - 1:500 - - ++ - + - - 1:5000 - - - - - - E2 1: 10 - ++ ++
1: 100 - ++ ++ 1:500 - - ++
E3 1: 10 - ++ ++
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1:100 - ++ ++ 1:500-++
E4 1: 10-++ ++
1: 100 - ++ ++ ++
1:500 - - ++
E5 1: 10 ++ ++
1: 100 ++
1: 500 - ++ ++ 1:5000 - +
++
E6 1: 20--+ +
E7 1: 20 +
E8 1: 20 +
E9 1 : 20 +
E10 1:20 +
Ell 1 : 20
E12 1 : 20 +
E13 1 : 20 - + ++ - - - - 1:20 - ++ ++ - - - - E15 1:20 - +
E16 1:20 ++
E17 1:20- ++ ++
E18 1:20 ++ ++
E19 1:20 ++ ++
1:20 ++ ++
E20
1:10 ++ ++ ++ - ++ ++
E21 1: 50 + + +
1: 100 ++ ++ ++ + + +
1: 200 ++ ++ ++--+
1: 500 + ++1 : 10 ++ + +
E22 1: 100 + + + +
1: 10 ++ + +
333/1651
E23 1: 100--+ + +
1: 10 ++ ++ ++ + +
E24 1 : 100 + +
1 : 10 ++ ++ ++ + +
E25 1: 100 + +
++ ++ ++
1: 10 ++ +
E26 1: 100 ++ ++ ++ + +
1: 10 ++ +
E27 1: 100 + +
1: 10 ++ ++ ++ ++ +
E28 1 : 100 + +
1: 10 ++ ++ ++ ++ +
E29 1: 100 + +
1 : 10 ++ ++ ++ + ++
E30 1 : 20 + +
1: 50 ++ ++ ++ + +
1: 100 + +
1: 10 ++ ++ ++ + ++
E31 1: 10 + +
E32 1: 10 + +
E33 1: 10 ++ ++
E34 1: 20 ++ ++ ++ + ++
1:50 ++ ++ ++ + +
1: 100 ++ ++ ++ + +
1: 10 ++ ++ ++ ++ ++
E35 1: 10 ++ ++
E36 1: 10 ++ ++
E37
++ ++ ++
++ ++ ++
++ ++ ++
'++'100 % removal, +'above 60% removal,'-'no effect
Table 14: Percentage removal of E. coli in 100ml and 1L D. W. by Indicated Clove oil emulsions
334/1651
Stock Working % Removal of E. coli
Emulsions Dilutions
(100 1 dose (lml dose)
E22 1: 10 96 92
E23 1: 10 98 90
E24 1: 10 95 89
E25 1: 10 99 89
E26 1: 10 100 92
E27 1: 10 100 94
E28 1: 10 100 95
E29 1: 10 100 96
E30 1: 10 100 100
E31 1: 10 100 98
E32 1: 10 97 97
E33 1: 10 95 97
E34 1: 10 100 100
1: 20 94
1: 50 91
E35 1: 10 100 100
E36 1: 10 100 100
E37 1: 10 100 100
Example 15
After getting 100% inhibition of E. coli with 1: 10 emulsion in spiked 1L water 1: 20,1: 30, 1: 40 and 1:
50 oil-in-water emulsions of clove oil were prepared. The emulsions when tested in 1L spiked water
at the fixed dose of 1 ml showed complete inhibition of 105 and 103 E. coli after 6hrs contact period
with 1: 20 emulsion. 1: 30,1: 4,1: 50 emulsions also showed appreciable inhibition as shown in Table
15.
The result in 1: 50 dilution shows that the lower dose of emulsion also reduces the bacterial
population to considerable extent.
335/1651
Emulsion Percentage
(Oil:Water) Inhibition of E.coli
1:10 100
1: 20 100
1 : 30 96
1:40 95
1 : 50 91
Example 16-Well water experiments:
Well water experiments were performed in 1L-water samples from various areas of
Nagpur City, India. The well water samples were in use for household purposes. Control as well as
test samples were given 6 hrs and overnight contact period with a standardized dose of lml of 1: 10
dilution of clove oil emulsion. After the specific contact period, 25ml of the aliquot was filtered
through sterile 0.45um size membrane filters. The filters were placed on MEC media and incubated
at 44.5 C overnight as described in the general methods above. The membranes were treated with
the urea solution and the yellow colonies counted in control as well as experimental samples. The
results are shown below in Table 16.
Table 16
Area % Removal % Removal Colony
6 hrs contact Overnight Characteristics
period contact period
Ramdaspeth 70 80 Blue
Bharatnagar 40 75 Bright yellow
Mankapur 70 90 Yellow blue
Samarthnagar 75 90 Yellow blue
Bazargaon/
Murli 50 65 Dark blue
Dharampeth 50 80 Dirty yellow
Kachipura 70 90 Yellow blue
336/1651
Snehnagar 50 70 Yellow blue
All references discussed herein are incorporated by reference. One skilled in the art would readily
appreciate the present invention is well adapted to carry out the stated objects and obtain the
disclosed ends and advantages, as well as those inherent herein. The present invention may be
embodied in other specific forms without departing from the spirit or essential attributes thereof.
Therefore, any descriptions of specific embodiments in the foregoing disclosure is not to be
construed as limiting the scope of the present invention.Claims:
We claim: 1. An emulsion composition used for disinfecting pathogenic micro-organisms present in
water enabling the water to be potable, the said composition comprising (a) an emulsifier, (b) an
essential oil, and (c) optionally an electrolyte and a carrier oil.
2. The composition as claimed in claim 1, wherein the essential oil is selected from the group
consisting of clove oil, eucalyptus oil and KapurTulsi oil, preferably clove oil.
3. The composition as claimed in claim 1, wherein the emulsifier is selected from the group
consisting of Tween, Myrj and Bryj surfactants, poloxamers and their derivatives, polyoxyethylene 50
stearate, polyoxyl 35 castor oil, polyoxyl 10 oleyl ether, polyoxyl 20 cetostearyl ether, polyoxyl 40
stearate, polysorbate 20, polysorbate 40, polysorbate 60, polysorbate 80, propylene glycol diacetate,
propylene glycol monostearate, sodium lauryl sulfate, sodium stearate, sorbitan mono-laurate,
sorbitan mono-oleate, sorbitan mono-palmitate, sorbitan monostearate, stearic acid, or emulsifying
wax.
4. The composition as claimed in claim 1, wherein the emulsifier used is selected from group
consisting of Tween surfactants, preferably Tween 20.
5. The composition as claimed in claim 1, wherein the amount of emulsifier used is in the range of
about 0.5 to 4.0 % of total essential oil, preferably is in the range of about 1.5 to 3.0 % of total
essential oil.
6. The composition as claimed in claim 1, wherein the carrier oil used is selected from a group
consisting of unsaturated vegetable oils.
337/1651
7. The composition as claimed in claim 1, wherein the amount of carrier oil used is in the range of
about 0. 01 to 5.0 % of total essential oil, preferably is in the range of about 0.01 to 0.5% of total
essential oil.
8. The composition as claimed in claim 1, wherein the electrolyte is selected from NaCl or Na2HP04.
9. The composition as claimed in claim 1, wherein the amount of electrolyte used is in the range of
about 0.01 to 0.1 PPM of essential oil.
10. The composition as claimed in claim 1, wherein the amount of composition used for disinfecting
pathogen contaminated water is in the ratio of 1: 10000 to 1: 200000.
11. The composition as claimed in claim 1, wherein the ratio of composition used to disinfect 100 %
pathogens, present in the contaminated water is in the ratio between 1: 10000 and 1: 20000.
12. The composition as claimed in claim 1, wherein the ratio of composition used to disinfect 60 %
pathogens, present in the contaminated water is in the ratio between
1: 20000 and 1: 200000.
13. A method of disinfecting water contaminated with pathogenic micro organism, the said method
comprising: (i) obtaining a composition as defined in claim 1 comprising an essential oil, a emulsifier
and optionally an electrolyte and a carrier oil, and (ii) treating the contaminated water with the
composition of step (i) for a period ranging up to 24 hours, preferably between 6-8 hours to disinfect
the water.
14. The method as claimed in claim 13, wherein the pathogenic microorganisms treated are selected
from group consisting of E. Coli, Salmonella thphi and Vibro cholarae.
15. The method as claimed in claim 13, wherein the amount of composition used for disinfecting the
pathogen contaminated water is in the range of about 1: 10000 to
1: 200000.
16. The method as claimed in claim 15, wherein 100 % pathogens are removed by the composition
at a ratio between 1: 10000 and 1: 20000 of the contaminated water.
338/1651
17. The method as claimed in claim 15, wherein 60 % pathogens are removed by the composition at
a ratio between 1: 20000 and 1: 200000 of the contaminated water.
18. The method as claimed in claim 13, wherein the essential oil used is selected from the group
consisting of clove oil, eucalyptus oil and KapurTulsi oil, preferably clove oil.
19. The method as claimed in claim 13, wherein the emulsifier used is selected from the group
consisting of Tween, Myrj and Bryj surfactants, poloxamers and their derivatives, polyoxyethylene 50
stearate, polyoxyl 35 castor oil, polyoxyl 10 oleyl ether, polyoxyl 20 cetostearyl ether, polyoxyl 40
stearate, polysorbate 20, polysorbate 40, polysorbate 60, polysorbate 80, propylene glycol diacetate,
propylene glycol monostearate, sodium lauryl sulfate, sodium stearate, sorbitan mono-laurate,
sorbitan mono-oleate, sorbitan mono-palmitate, sorbitan monostearate, stearic acid, or emulsifying
wax.
20. The method as claimed in claim 13, wherein the emulsifier used is selected from the group
consisting of Tween surfactants, preferably Tween 20.
21. The method as claimed in claim 13, wherein the amount of emulsifier used in step (i) is in the
range of about 0.5 to 4.0 % of essential oil, preferably is in the range of about 1.5 to 3.0 % of
essential oil.
22. The method as claimed in claim 13, wherein the carrier oil used is selected from group consisting
of unsaturated vegetable oils.
23. The method as claimed in claim 13, wherein the amount of carrier oil used is in the range of about
0.01 to 5.0 % of essential oil, preferably is in the range of about 0.01 to 0.5 %.
24. The method as claimed in claim 13, wherein the electrolyte used is selected from the group
consisting of NaCl or Na2HP04.
25. The method as claimed in claim 13, wherein the amount of electrolyte used is in the range
between 0.01 to 0.1 PPM of essential oil.
26. The method as claimed in claim 13, wherein-alternatively hydro-alcoholic preparation of essential
oil may also be used to kill the pathogenic microorganisms contaminating the water.
339/1651
27. The method as claimed in claim 26, wherein the ratio of contaminated water: hydro alcoholic
solution of essential oil is in the range between 10: 1 to 5000: 1.
28. A process of preparing a emulsiable composition for the disinfection of water, the said process
comprising steps of : a) mixing an essential oil, an emulsifier, optionally an electrolyte, and optionally
carrier oil; b) shaking, stirring or sonicating the mixture of step (a) to obtain an emulsion of essential
oil; and c) adjusting the pH of solution of step (b) up to 11 using KOH solution to obtain a
composition for disinfecting contaminated water.
29. A method as claimed in claim 28, wherein the preferred pH is between 8.5 to 9.50.
30. The method as claimed in claim 28, wherein the essential oil used is selected from the group
consisting of clove oil, eucalyptus oil and KapurTulsi oil preferably clover oil.
31. The method as claimed in claim 28, wherein the electrolyte is selected from the group consisting
of NaCI or Na2HP04, 32. The method as claimed in claim 28, wherein the carrier oil used is selected
from group consisting of unsaturated vegetable oils.
340/1651
55. ES2165296 - 01.03.2002
PROCESS FOR OBTAINING FUNGICIDAL EXTRACT FROM ESSENTIAL OIL OF LEMON SUBMITS
ESSENTIAL OIL TO HEXANE TO ELIMINATE TERPENES AND CAROTENOIDS AND THEN WITH
BENZENE TO EXTRACT FUNGICIDAL POLYMETHOXYLATE FLAVONES
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=ES2165296
Inventor(s):
DEL RIO CONESA JOSE ANTONIO (ES); ARCAS MINARRO MARIA CRUZ (ES);
BOTIA ARANDA JUANA MARIA (ES); ORTUNO TOMAS ANA MARIA (ES)
Applicant(s):
UNIV MURCIA (ES)
IP Class 4 Digits: A01N; A23B
IP Class:
A01N65/00; A23B7/16
Application Number:
ES20000000124 (20000121)
Priority Number: ES20000000124 (20000121)
Family: ES2165296
Abstract:
PROCESS FOR OBTAINING A FUNGICIDAL EXTRACT FROM ESSENTIAL OIL OF LEMON SUBMITS
THE ESSENTIAL OIL TO HEXANE TO ELIMINATE TERPENES AN CAROTENOIDS. IT IS THEN
TREATED WITH BENZENE TO EXTRACT FUNGICIDAL POLYMETHOXYLATE FLAVONES. BOTH
STAGES OF THE PROCESS ARE EFFECTED IN THE PRESENCE OF WATER.
341/1651
56. ES8507442 - 16.12.1985
PROCESS FOR PREPARING ALCOHOLIC EXTRACTS OF CAMOMILE OR THE ESSENTIAL OIL OF
CAMOMILE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=ES8507442
Applicant(s):
DEGUSSA (DE)
IP Class 4 Digits: C11B; C07C
IP Class:
C11B9/02; C07C13/52
Application Number:
ES19840538073 (19841129)
Priority Number: ES19840538073 (19841129)
Family: ES8507442
Abstract:
PROCESS FOR PREPARING IMPROVED ALCOHOLIC EXTRACTS OF CAMOMILE OR IMPROVED
ESSENTIAL OIL OF CAMOMILE FROM THE SPECIES OF CAMOMILE, MANZANA.
342/1651
57. FR2533197 - 23.03.1984
DEVICE FOR PACKAGING A LIQUID SUBSTANCE, PARTICULARLY AN ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2533197
Inventor(s):
MAIRE NEE (--); SENS-OLIVE DANIELE (--)
Applicant(s):
EXPANSION AROMATIQUE FSE SA (FR)
IP Class 4 Digits: B01L; B65D
IP Class:
B65D17/28; B65D1/00; B65D41/40; B01L3/00; B65D81/18; B65D81/20
E Class: A61J1/06C
Application Number:
FR19820015882 (19820921)
Priority Number: FR19820015882 (19820921)
Family: FR2533197
Equivalent:
BE894598
Abstract:
THE PRESENT INVENTION IS CONCERNED WITH A NEW PACKAGING FOR A LIQUID SUBSTANCE,
PARTICULARLY AN ESSENTIAL OIL CAPABLE OF BEING MODIFIED IN AIR, COMPRISING A PHIAL
WITH TWO SELF-BREAKING POINTS, A FLEXIBLE END PIECE ADAPTABLE AT ONE OF THE ENDS
OF THE PHIAL ONTO THE BODY OF THE SAID PHIAL, AND A STOPPING MEANS ADAPTABLE TO
THE OTHER END, THE END PIECE MOUNTED IN A SEALED MANNER ON THE BODY OF THE
PHIAL FORMING WITH THE LATTER A DROPPER WHEN THE POINTS HAVE BEEN BROKEN.
Description:
343/1651
Dispositif pour le conditionnement d'une substance liquide > notamment une huile essentielle.
La prйsente invention a trait а un nouveau dispositif pour le conditionnement d'une substance
liquide, notamment une huile essentielle susceptible d'кtre altйrйe par contact frequent avec leair.
On sait que les huiles essentielles sont des extraits vйgйtaux liquides susceptibles d'йtire altйrйs,
modifiйs ou detruits par l'oxygиne ou l'humiditй de l'air. Il se trouve que les conditionnements
actuels des huiles essentielles dans des bouteilles en verre ou des bidons mйtalliques de grand
volume (notamment de l'ordre de 100 и 1000 ml), qui sont livrйs notamment aux pharmaciens
d'officine pour leurs preparations magistrales, ne conviennent pas en raison de la mise en contact
avec l'air quand ils sont ouverts frequomment pour prйlиvements de l'ordre du millilitre.~
Selon l'inventions on propose un nouveau dispositif pour le conditionnement sous un faible volume
pour des doses unitaires susceptibles d'кtre fractionnйes.Ce nouveau dispositif, qui est,trиs
pratique pour les huiles essentielles, convient d'une maniиre gйnйrale pour tous les liquides
pouvant кtre altйrйs par contact frйquent avec l'air.
Le dispositif selon l'invention qui est du type ampoule auto-cassable et qui est susceptible de
permettre une utilisation d'une partie du contenu de ladite ampoule est caractйrisй en ce qu'il
comprend
a) une ampoule а deux pointes auto-cassables remplie
d'un volume d'une substance liquide,
b) un embout souple adaptable а l'une des deux
extrйmitйs de l'ampoule sur le corps de celle-ci
au-delа de l'affaiblissement de matiиre permettant
de sйparer la pointe auto-cassable et formant un
rйservoir de propulsion quand il est montй de
faзon йtanche sur le corps de ladite ampoule, et
c) un moyen d'obturation susceptible d'entre adaptй
а l'autre extrйmitй de l'ampoule, quand la pointe
auto-cassable de ladite extrйmitй a йtй sйparйe
de l'ampoule,
le moyen b) montй de faзon йtanche sur le corps de l'ampoule
constituant avec ladite ampoule un compte-gouttes quand les deux
pointes auto-cassables ont йtй sйparйes de ladite ampoule.
344/1651
De faзon avantageuse, l'ampoule а deux pointes
auto-cassables sera remplie sous gaz inerte tel que l'azote, et
le contenu de l'ampoule correspondra а une dose ou un volume
unitaire, notamment 1 ml d'huile essentielle.
D'autres avantages et caractйristiques de l'invention seront mieux cpmpris а la lecture de la
description dйtaillйe
qui suit et а l'examen du dessin annexй qui reprйsente а titre d'illustration un exemple de
rйalisation nullement limitatif.
La figure unique montre un dispositif selon l'invention comprenant une ampoule en verre 1 а deux
pointes 4 et 5 auto-cassables selon les lignes ou traits 6 et 7 du type а affaiblissement de matiere, et
contenant une huile essentielle non reprйsentйe ici ; un embout souple 2 susceptible d'кtre adaptй,
au moment de l'emploi, de faзon йtanche au corps de l'ampoule 1 au-delа de la ligne ou trait de
cassage 6 ; et, un moyen d'obturation ou capuchon souple 3 pouvant titre adaptй de faзon
йtanche l'ampoule au-delа de la ligne ou trait de cassage 7, le moyen 3 йtant reprйsentй ici
sйparй dc I'anpoulc, d'une part, et montй sur ladite ampoule, d'autre part.
Le meilleur mode de mise en oeuvre consiste а monter de faзon йtanche l'embout souple 2 а
l'ampoule 1, а casser l'extrйmitй 4 selon 6, puis а casser l'extrйmitй 5 selon 7 pour obtenir un
compte-gouttes. De faзon avantageuse, l'embout 2 sera adaptй а l'ampoule de telle faзon que
l'espace compris entre 2 et 1 soit sensiblement plus grand que le volume d'huile essentielle contenu
dans 1. Aprиs utilisation de la quantitй requise d'huile essentielle, le capuchon 3 pourra etre
adaptй а l'ampoule de faзon йtanche autour de la cassure 7 pour conserver la quantitй d'huile
essentielle pouvant encore кtre contenue dans l'ampoule.
Selon ce mode de mise en oeuvre, l'embout souple 2
permet de sйparer la pointe auto-cassable 4 en protйgeant les
doigts du manipulateur, ceux-ci n'йtant pas en contact direct avec
ladite pointe. De mкmeg le capuchon 3 peut кtre utilisй pour la
sйparation de la pointe 5 sans risque pour le manipulateur, il
suffit ensuite d'enlever ledit capuchon pour libйrer l'ouverture
de l'ampoule situйe au voisinage de 7.
D'une maniиre gйnйrale, l'embout 2 et le capuchon 3
345/1651
peuvent кtre rйalisйs en matiиre inerte vis-а-vis du contenu
de l'ampoule9 par exemple en caoutchouc naturel ou synthйtique,
notamment en polytйtrafluoroйthylиne. L'embout et le capuchon peuvent кtre avantageusement
emballйs sous vide а cфtй d'un lot
d'ampoules I.
Avec le dispositif de l'invention, on propose des
ampoules renfermant de faibles quantitйs d'huile essentielle,
le contenu de chaque ampoule d'un volume de l'ordre de I ml pouvant
кtre fractionnй au moment de l'emploi. Claims:
REVENDICATIONS
1. Dispositif pour le conditionnement d'une substance liquide, notamment une huile essentielle
pouvant кtre altйrйe par contact frйquent avec l'air, ledit dispositif, qui est du type ampoule autocassable et qui est susceptible de permettre l'utilisation dsune partie du contenu de ladite ampoule,
йtant caractйrisй en ce qu'il comprend
a) une ampoule а deux pointes auto-cassables remplie
d'un volume d'une substance liquide,
b) un embout souple adaptable а l'une des deux
extrйmitйs de l'ampoule sur le corps de celle-ci
au-dell de l'affaiblissement ae matiиre permettant
de sйparer la pointe auto-cassable et formant un
rйservoir de propulsion quand il est montй de
faзon йtanche sur le corps de ladite ampoule, et
c) un moyen d'obturation susceptible d'кtre adaptй
а l'autre extrйmitй de l'ampoule, quand la pointe
auto-cassable de ladite extrйmitй a -йtй sйparйe
de l'ampoule, le moyen b) monte de faзon йtanche sur le corps de l'ampoule constituant avec
ladite ampoule un compte-gouttes quand les deux pointes auto-cassables ont йte sйparйes de
ladite ampoule.
346/1651
2. Dispositif selon la revendication 1, caractйrise en ce que la'espace interieur compris entre
l'embout adapte au corps de l'ampoule et ladite ampoule est sensiblement supйrieur au volume du
contenu de ladite ampoule.
3. Dispositif selon l'une quelconque des revendications 1 et 2, caractйrisй en ce que l'ampoule а
deux pointes autocassables renferme 1 ml d'huile essentielle sous gaz inerte.
347/1651
58. FR2574087 - 06.06.1986
PREPARATION OF EXTRACTS OF CAMOMILE AND OF ESSENTIAL OIL FROM TETRAPLOID
CAMOMILES
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2574087
Inventor(s):
ISAAC OTTO (--); CHLODWIG FRANZ (--)
Applicant(s):
DEGUSSA (DE)
IP Class 4 Digits: A61K; C11B
IP Class:
A61K35/78; C11B9/00
E Class: C11B9/02; A61K35/78; C11B9/02E; A01H1/04; A01H5/02B; A01H5/02F
Application Number:
FR19840018279 (19841130)
Priority Number: FR19840018279 (19841130); DD19840270119 (19841130); DE19833323411
(19830629)
Family: FR2574087
Abstract:
PROCESS FOR THE PREPARATION OF IMPROVED ALCOHOL EXTRACTS OF CAMOMILE OR OF
IMPROVED CAMOMILE ESSENTIAL OIL, FROM THE CAMOMILE SPECIES MANZANA.Description:
Ia demande de brevet franзais nO 8409855 du 22.6.84 au nom de la Demanderesse concerne une
nouvelle espиce de camomille tйtraplolde (dйnomination MANZANA) qui se caractйrise par une
teneur йlevйe, а la fois en chamazulиne et en (-)-9-bisabolole, les fleurs de cette espиce de
camomille MANZANA, sйchйes а 400C, contenant au moins (par rapport а la substance sиche)
348/1651
150 mg a de chamazulиne, au moins 300 mg % de (-)-o(-bisabolole et moins de 50 mg % d'autres
bisaboloides.
Or, il s'zest rйvйlй que les extraits obtenus а partir des fleurs de cette espиce MANZANA
prйsentent йgalement des teneurs йlevйes, а la fois en chamazulиne et en (-)-o(-bisabolo. Il en
va de meme pour une huile essentielle obtenue а partir de cette espиce de camomille.
le sйchage des fleurs de camomille et la prйparation des drogues s'effectuent de la maniиre
indiquйe dans la demandй de brevet franзais nO 8409855 du 22.6.84 au nom de la
Demanderesse.
C'est ainsi que des extraits alcooliques d'une drogue obtenue а partir de l'espиce de camomille
MANZANA ou de fleurs sйchйes de l'espиce de camomille MANZANA contiennent au moins 5
mg %, de prйfйrence 5,6 mg % de chamazulиne et au moins 15 mg %, de prйfйrence au moins
15,5 mg % de (-)-ebisabolole dans l'extrait alcoolique de la drogue et moins de 8 mg % d'autres
bisabololdes.
La prйparation de tels extraits s'effectue de la maniиre habituelle а cet effet. Pour l'extraction, on
peut utiliser par exemple des dispositifs de mйlange, notamment des machines dites malaxeurs а
deux fonds, des percolateurs et d'autres appareils d'extraction appropriйs. Ia tempйrature pendant
l'extraction est par exemple de 10 а 500C. Un refroidissement n' est pas nйcessaire.
En cas d'extraction au moyen de machines mйlangeuses, la vitesse de rotation du mйlangeur sera
rйglйe en particulier de telle maniиre que la vitesse pйriphйrique d'un point situй а la pйriphйrie
du mйlangeur soit comprise entre 1,7 et 2,7 m/s, la durйe de l'extraction se situant de prйfйrence
entre 15 minutes et 3 heures, en particulier entre 30 et 120 minutes.
Pour un mйlangeur ayant un rayon de 55 cm, une vitesse de rotation de 50 а 250 tr/mn est par
exemple appropriйe, la durйe de l'extraction йtant alors comprise par exemple entre 15 minutes et
3 heures. De prйfйrence, avec un mйlangeur de cette taille, on choisit une vitesse de rotation de 50
а 250 tr/mn,uae durйe de l'extraction de 15 а 120 minutes йtant suffisante.
Entrent en particulier en ligne due compte, en tant que solvants, des mono- ou polyalcools
aliphatiques linйaires ou ramifiйs а 1-6 atomes de carbone eut le sol-cйtal (2-dimйthyl-4-oxy
349/1651
mйthyl-1,3-dioxolanne), comme par exemple le mйthanol, l'йthanol, le propanol-(2), le butanol, le
glycйrol ou similaires, ainsi que des mйlanges de ces solvants avec l'eau.
On peut aussi utiliser des mйlanges de ces solvants. La quantitй minimale de solvant est de 2
parties de solvant pour 1 partie de drogue. En gйnйral, on utilise 2 а 20 parties de solvant pour 1
partie de drogue, en particulier 3 а 10 parties de solvant pour 1 partie de drogue.
Une huile essentielle, obtenue а partir de l'espиce de camomille MANZANA, contient au moins 5 %
de chamazulиne et au moins 15 % de (-)-o(-bisabolole et moins de 10 % d'autres bisabolofdes.
Pour la prйparation de l'huile essentielle, on procиde en gйnйral en chauffant а l'йbullition des
fleurs. sйchйes de camomille avec de l'eau, par exemple en prйsence d'acide ascorbique (par
exemple sous forme de sel, notamment sous forme de sel sodique) а un pH compris entre 4 et 6, de
prйfйrence entre 5 et 5,5. Le pH est rйglй par exemple au moyen d'un acide tel que l'acide
chlorhydrique.
Pour une partie en poids de fleurs sйchйes de camomille on emploie par exemple de lO а 50
parties en poids a d'eau et йventuel- lement 0,1 а l partie en poids d'acide ascorbique.
On chauffe en gйnйral pendant 2 а 8 heures.
Le distillat aqueux obtenu est йpuisй а plusieurs reprises avec un hydrocarbure aliphatique
infйrieur liquiae < par exemple un йther de pйtrole (de point d'йbullition compris par exemple
entre 35 et 60oC), le pentane, le xylиne, la dйcaline), la phase organique est sйchйe (par
exemple au moyen de sulfate de sodium) et le solvant organique est йliminй avec mйnagement
(par exemple par distillation dans ltйvaporateur rotatif ou par distillation а 40 - 700C, de
prйfйrence а 50 - 600C). Avec des solvants de point d'йbullition plus йlevй, cette йlimination par
distillation est effectuйe sous vide.
La dйtermination de la teneur en chamazulиne et en q-bisabolole, ainsi qu'en autres bisabololdes
dans les extraits ou dans l'huile essentielle est effectuйe de la maniиre indiquйe dans la demande
de brevet franзais nO 8409855- du 22.6.84 au nom de la Demanderesse.
Exemple
350/1651
200 g de fleurs sйchйes de camomille suivant la demande de brevet franзais nO 8409855 du
22.6.84 au nom de la Demanderesse (sйchage effectuй а une tempйrature de l'air de 500C а l'abri
de la lumiиre solaire) sont mйlangйs, dans un ballon а fond rond de 5 litres, avec 3,6 litres d'eau et
2 g d'ascorbate de sodium et le pH est rйglй а 5,0 avec HOl 1N. Aprиs addition de perles
facilitant l'йbullition, on chauffe а l'йbullition. En l'espace de 3 heures environ, on recueille а peu
prиs 1,2 litres de distillat.
Aprиs l'achиvement de la distillation, le distillat est йpuisй а trois reprises avec 100 ml d'йther
de pйtrole chaque fois et sйchй sur du sulfate de sodium anhydre. Ia solution sйchйe est filtrйe
et le solvant est ensuite йliminй par distillation dans l'йvaporateur rotatif. Le rendement s'йlиve а
1,44 g d'huile essentielle.
Dans l'huile essentielle obtenue, la teneur en chamazulиne et en (-)-c{-bisabolole est ensuite
dйterminйe. Claims:
- REVENDICATIONS
1.- Extraits alcooliques de camomille, qui sont obtenus par emploi de fleurs sйchйes de l'espиce
des camomilles tйtraploldes suivant la revendication 3 de la demande NQ 84 09855, caractйrisйes
en ce qu'ils contiennent au moins 5mg% de chamazulиne et au moins 15 mg% de (-)- -bisabolole
et moins de 8 mg % d'au- tres bisabololdes.
2.- Huile essentielle qui est obtenue par l'emploi de fleurs sйchйes de l'espиce des camomilles
tйtraploldes suivant la revendication 10 de la demande nQ 84 09855, caractйrisйe en ce qu'elle
contient au moins 5% de chamazulиne et au moins 15% de (-)- -bisabolole йt moins de 108
d'autres bisabololdes.
3.- Procйdй pour l'obtention d'extraits alcooliques de camomille ou -d'huiles essentielles de
camomille par l'emploi de l'espиce des camomilles tйtraploldes suivant les revendications 3 et 10
de la demande n2 84 09855, et particuliиrement par l'emploi de fleurs sйchйes de cette espиce
de camomilles tйtraploldes, caractйrisй en ce que les extraits obtenus par extraction avec alcools
contiennent au moins 5 mg % de chamazulиne et au moins 15 mg % de (-)-c(-bisabolole et moins
351/1651
de 8 mg % d'autres bisabolosdes, et en ce que l'huile essentielle obtenue par distillation en
prйsence d'eau, contient au moins 5% de chamazulиne et au moins 15% de (-) -d- bisabolole et
moins de 10% d'autres bisabololdes.
4.- Emploi de l'espиce des camomilles tйtraploldes suivant la revendication 1 de la demande N2
84 09855, en particulier de leurs fleurs sйchйes pour l'obtention d'extraits alcooliques de
camomilles ou pour l'obtention d'huile essentielle de camomille.
352/1651
59. FR2581311 - 07.11.1986
PHARMACEUTICAL COMPOSITIONS FOR THE TREATMENT OF COLITES AND COLOPATHIES,
BASED ON THYME OIL AND CADE ESSENTIAL OIL.
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2581311
Applicant(s):
BENTCHIKOU ABDELHAMID (FR)
IP Class 4 Digits: A61K
IP Class:
A61K35/78; A61K35/04
E Class: A61K35/78
Application Number:
FR19860001950 (19860213)
Priority Number: LU19850085877 (19850506)
Family: FR2581311
Equivalent:
CH667391; DE3615031; LU85877
Abstract:
PHARMACEUTICAL COMPOSITION FOR THE TREATMENT OF COLITES AND COLOPATHIES. THIS
COMPOSITION CONTAINS THYME OIL AND CADE ESSENTIAL OIL AS ACTIVE INGREDIENTS. THE
PROPORTIONS MAY BE 0.1 TO 70% THYME OIL AND 0.1 TO 40% CADE ESSENTIAL OIL,
RELATIVE TO THE TOTAL WEIGHT OF A DOSAGE UNIT OF THE COMPOSITION, FOR WHICH THE
EXCIPIENT MAY BE AQUEOUS.Description:
La prйsente invention est relative а une composition pharmaceutique pour le traitement de colites
et colopathies.
353/1651
On sait que le systиme digestif, en particulier l'intestion grкle et le cфlon, est le siиge d'une sйrie
d'affections, souvent chroniques, que l'on qualifie, en gйnйral, de grкlites, colites ou colopathies.
I1 s'- agit de maladies infectieuses, parasitaires ou fonctionnelles, dues souvent а divers
microorganismes tels que colibacilles, ascaris, amibes, etc... ou а un disfonctionnement qui se
manifestent principalement par de la constipation et/ou de la diarrhйe accompagnйes de douleurs
abdominales et d'autres troubles, tels que cйphalйe, insomnie, voire mкme troubles psychiques.
I1 est connu de traiter les colites et colopathies а l'aide de divers mйdicaments, notamment des
antibiotiques comme la rovamycine, l'йmйtine et divers dйrivйs halogйnйs ou arsйnicaux de la
quinolйine, de mкme qu'au moyen de pansements а base de composйs de bismuth. Ces
mйdicaments connus ont, en gйnйral, des effets secondaires indйsirables. Ils provoquent souvent
un dйsйquilibre de la flore intestinale et parfois d'autres troubles notamment au niveau oculaire.
La prйsente invention concerne une composition pharmaceutique dйpourvue de ces effets
secondaires, convenant spйcialement pour le traitement de diverses formes de colites et
colopathies.
La composition pharmaceutique suivant la prйsente invention se caractйrise essentiellement par le
fait qu'elle contient, comme principes actifs, de l'essence de thym et de l'huile essentielle de cade.
L'essence de thym est une essence aromatique contenant du thymol obtenue par traitement de la
plante Thymus vulgaris, par distillation avec de l'eau, par chauffage а la vapeur d'eau et
condensation.
Quant а l'huile essentielle de cade, il s'agit d'un mйlange de produits de distillation du bois de
gйnйvrier oxycиdre (Juniperus oxycedrus), dont l'emploi est connu dans le traitement d'affections
cutanйes, telles que le psoriasis et certains eczйmas.
Conformйment а la prйsente invention, la composition pharmaceutique contient, а titre
d'ingrйdients actifs, de l'essence de thym а raison d'environ 0,1 а 70 % en poids, ainsi que de
l'huile essentielle de cade а environ 0,1 а 40 % en poids, par rapport au poids total de la
composition.
La proportion d'essence de thym est, de prйfйrence, comprise entre environ 2 et 20 * du poids de
la composition totale, tandis que la proportion d'huile essentielle de cade est avantageusement
354/1651
comprise entre 0,2 et 10 % du poids de la composition totale, cette derniиre contenant de
prйfйrence une quantitй d'essence de thym supйrieure а celle d'huile de cade.
Pour une unitй posologique de 0,5 g, la composition pharmaceutique contient de 0,5 а 350 mg, de
prйfйrence de 2 а 100 mg d'essence de thym et de 0,5 а 200 mg, de prйfйrence, de 1 а 75 mg
d'huile essentielle de cade.
La composition pharmaceutique suivant l'invention peut йvidemment contenir des excipients
classiques.
Elle peut se prйsenter sous diverses formes galйniques а administrer par la bouche.
La composition pharmaceutique se prйsente, de prйfйrence, sous forme de capsules molles ou
dures, telles que des capsules de gйlatine, contenant les deux ingrйdients actifs. Cependant, elle
peut aussi se prйsenter sous forme de sirop, de suspensions aqueuses, voire mкme sous forme de
prйparations solides, telles que des comprimйs ou dragйes entйriques.
Les exemples non limitatifs suivants illustrent des compositions pharmaceutiques suivant l'invention.
EXEMPLE 1
Dans une capsule de gйlatine molle, on introduit, en plus d'un excipient aqueux, de l'essence de
thym et de l'huile essentielle de cade dans les proportions suivantes essence de thym : 65 mg huile
essentielle de cade : 7 mg excipient q.s. ad 0,5 mg
EXEMPLE 2 essence de thym : 25 mg huile essentielle de cade : 1 mg excipient aqueux q.s. ad 0,5
g pour une capsule de gйlatine molle.
Des essais ont rйvйlй que l'administration de 1 a 4 capsules par jour permet de faire disparaоtre
en quelques jours les symptфmes et effets douloureux de divers types de colites ou colopathies, en
particulier les colites dues a des bactйries ou parasites pathogиnes, ainsi que les colites
spasmodiques.
Ces essais ont dйmontrй que la composition pharmaceutique suivant l'invention respecte
l'йquilibre de la flore intestinale et possиde une remarquable activitй antispasmodique. Claims:
355/1651
REVENDICATIONS
1. Composition pharmaceutique pour le
traitement de colites et de colopathies,
caractйrisйe en ce qu'elle contient, а titre
d'ingrйdients actifs, de l'essence de thym et de
l'huile essentielle de cade.
2. Composition pharmaceutique suivant la
revendication 1, caractйrisйe en ce qu'elle
contient de 0,1 а 70 % environ d'essence de thym
et de 0,1 а 40 % d'huile essentielle de cade, ces
pourcentages йtant basйs sur le poids total d'une
unitй posologique de la composition.
3. Composition pharmaceutique suivant la
revendication 2, caractйrisйe en ce qu'elle
contient de 2 а 20 % environ d'essence de thym et
de 0,2 а 10 e environ d'huile essentielle de cade.
4. Composition pharmaceutique suivant l'une
quelconque des revendications prйcйdentes,
caractйrisйe en ce qu'elle contient une proportion
pondйrale d'essence de thym supйrieure а celle
d'huile essentielle de cade.
5. Composition pharmaceutique suivant l'une
quelconque des revendications prйcйdentes, carac
tйrisйe en ce qu'elle est constituйe d'une capsule
molle ou dure, telle qu'une capsule de gйlatine
contenant les ingrйdients actifs, ainsi qu'йven
tuellement un excipient pharmacologiquement accep
table.
356/1651
60. FR2598620 - 20.11.1987
AROMATIC HYDROSOL OF ESSENTIAL OIL OF MELISSA OFFICINALIS USED IN AEROSOL FORM
AS A STIMULANT OF MALE SEXUAL ACTIVITY, AND COMPOSITION OF ESSENTIAL OIL OF
MELALEUCA QUINQUENERVIA NEROLIDOLIFERA AND BORAGE POWDER INTENDED TO BE
TAKEN IN ORDER TO COMBINE ITS EFFECTS WITH THOSE OF THE HYDROSOL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2598620
Applicant(s):
DESCHLER CHRISTOPHE (FR); CHIKAR MAURICE (FR); RIOUX JEAN (FR)
IP Class 4 Digits: A61K
IP Class:
A61K35/78
E Class: A61K35/78
Application Number:
FR19860006891 (19860514)
Priority Number: FR19860006891 (19860514)
Family: FR2598620
Abstract:
AROMATIC HYDROSOL OF ESSENTIAL OIL OF MELISSA OFFICINALIS USED IN AEROSOL FORM
AS A STIMULANT OF MALE SEXUAL ACTIVITY.Description:
HYDROSOL AROMATIQUE D'HUILE ESSENTIELLE DE MELISSE OFFICI
NALE UTILISE EN AEROSOL COMME STIMULANT DE L'ACTIVITE
SEXUELLE MASCULINE ET COMPOSITION D'HUILE ESSENTIELLE DE
MELALEUCA QUINQUENERVIA NEROLIDOLIFERA ET DE POUDRE DE
BOURRACHE DESTINEE A ETRE INGEREE POUR CONJUGUER SES EFFETS
A CEUX DE L'HYDROSOL.
357/1651
L'invention a pour objet un hydrosol aromatique d'huile essentielle de mйlisse officinale utilisй en
aйrosol comme stimulant de l'activitй sexuelle masculine et une composition d'huile essentielle de
melaleuca quinquenervia nerolidolifera et de poudre de bourrache destinйe а кtre ingйrйe pour
conjuguer ses effets а ceux de l'hydrosol.
L'huile essentielle de melaleuca quinquenervia nerolidolifera a un effet de stimulation hypophysotesticulaire tandis que la bourrache est un dйtoxifiant et augmente les йchanges cellulaires tout en
tonifiant l'organisme et que la mйlisse officinale agit par effet vasodilatateur chez l'homme.
L'huile essentielle de melaleuca quinquenervia nerolidolifera diminue en outre les risques cardiovasculaires.
L'invention sera mieux comprise а l'aide de la description ci-apres.
Des gйlules de taille No 1 sont remplies de 120 mg de poudre de bourrache provenant des
sommitйs de la plante et deux gouttes d'huile essentielle de melaleuca quinquenervia nerolidolifera
sont ajoutйes dans la gйlule, qui est immйdiatement fermйe.
On prйpare un hydrosol aromatique avec une phase acqueuse imprйgnйe d'huile essentielle de
mйlisse officinale et on en remplit des vaporisateurs pour l'utiliser en aйrosol.
L'ingestion de la gйlule est immйdiatement suivie de vaporisation de l'aйrosol in situ.
L'huile essentielle de melaleuca quinquenervia nerolidolifera contient principalement un alcool
diterpйnique, le nйrolidol, tandis que l'hydrosol contient des aldйhydes du type citraldйhyde et
que la bourrache a pour composants principaux des mucilages, de l'allantoine et une saponine.
Claims:
Revendications
358/1651
1. Hydrosol aromatique d'huile essentielle de Mйlisse officinale utilisй en aйrosol comme stimulant
de l'activitй sexuelle masculine.
2. Composition d'huile essentielle de melaleuca quinquenervia nerolidolifera et de poudre de
bourrache destinйe а кtre ingйrйe pour conjuguer ses effets а ceux de l'hydrosol selon la
revendication 1.
3. Composition selon la revendication 2, caractйrisйe par sa prйsentation en gйlules de taille No 1
contenant 120 mg de poudre de bourrache et deux gouttes d'huile essentielle de melaleuca
quinquenervia nerolidolifera.
359/1651
61. FR2717492 - 22.09.1995
EXTRACTION OF ESSENTIAL OIL FROM PLANT MATERIAL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2717492
Inventor(s):
MICHEL SILHOL (--); PIERRE MONDAN (--); PIERRE DENIS (--)
Applicant(s):
COMMISSARIAT ENERGIE ATOMIQUE (FR)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
E Class: C11B9/02H; B01D5/00H
Application Number:
FR19940002984 (19940315)
Priority Number: FR19940002984 (19940315)
Family: FR2717492
Abstract:
EXTRACTION OF AN ESSENTIAL OIL FROM PLANT MATERIAL COMPRISES; (I) CONTACTING THE
PLANT MATERIAL WITH WATER VAPOUR AT A TEMP. BELOW 100 DEG C AND A PRESSURE
BELOW ATMOSPHERE; AND (II) SEPG. THE EXTRACTED OIL FROM THE WATER VAPOUR. ALSO
CLAIMED IS THE APPTS. FOR EXTRACTING AN ESSENTIAL OIL FROM PLANT MATERIAL. THE
PROCESS IS USEFUL FOR PRODUCING AROMATIC OR MEDICINAL ESSENCES FOR USE IN THE
FOOD, TOBACCO, PERFUME AND PHARMACEUTICAL INDUSTRIES. DEGRADATION OF THE
QUALITIES OF THE ESSENTIAL OIL IS LESS THAN WITH CONVENTIONAL STEAM
DISTN.Description:
360/1651
PROCEDE ET INSTALLATION D'EXTRACTION D'UNE HUILE ESSENTIETTw- A PARTIR DE vu
VEGETAUX
La prйsente invention a pour objet un procйdй d'extraction d'une huile essentielle а partir de
vйgйtaux, utilisable notamment pour l'extraction а basse tempйrature d'essences aromatiques et
mйdicinales.
De nombreux vйgйtaux, en particulier les plantes aromatiques ou mйdicinales, contiennent des
huiles essentielles qui peuvent trouver de nombreuses applications dans l'industrie de l'agroalimentaire, dans l'industrie du tabac et de la parfumerie, ainsi que dans l'industrie pharmaceutique.
Les procйdйs couramment employйs pour l'obtention d'huiles essentielles а partir de vйgйtaux
sont l'hydrodistillation et l'extraction par la vapeur d'eau. Une installation d'hydrodistillation d'huile а
partir d'herbes aromatiques est dйcrite par exemple dans Perfumer & Flavorist, vol. 14, 1989, p. 57
а 63.
Ces techniques d'hydrodistillation et d'extraction par la vapeur d'eau ont pour inconvйnient d'exiger
des tempйratures йgales ou supйrieures а 1000C, qui peuvent dйtruire ou diminuer les qualitйs
propres de l'huile essentielle.
Ainsi, l'huile essentielle issue du fruit de coriandre comprend une trиs forte proportion (60 а 80 %)
de dextrolinalol (isomиre droit), et d'autres composйs terpйniques en plus faible proportion qui
contribuent aussi а la note olfactive de l'huile essentielle tant apprйciйe des aromaticiens et des
parfumeurs du monde entier.
Or, le linalol est dйgradй а une tempйrature de 100"C en produits tels que le myrcиne, l'a terpinйol et le gйraniol qui sont nuisibles а la qualitй de l'huile essentielle.
Pour surmonter cette difficultй, on peut envisager de rйaliser l'extraction de l'huile essentielle par
solvant, mais ce procйdй ne peut кtre dйveloppй а grande йchelle en raison d'une mise en
oeuvre peu commode et plus coыteuse.
La prйsente invention a prйcisйment pour objet un procйdй d'extraction d'une huile essentielle а
partir de vйgйtaux tels que des plantes aromatiques ou mйdicinales, qui permet d'йviter la
destruction ou la diminution des qualitйs propres а chaque plante, en rйalisant l'extraction а des
tempйratures infйrieures а 1000C.
361/1651
Selon l'invention, le procйdй d'extraction d'une huile essentielle а partir de vйgйtaux, consiste а
mettre en contact les vйgйtaux avec de la vapeur d'eau а une tempйrature T infйrieure а 1000C,
sous une pression P infйrieure а la pression atmosphйrique, pour extraire l'huile essentielle dans la
vapeur d'eau, puis а sйparer de la vapeur d'eau l'huile ainsi extraite.
Pour mettre en oeuvre ce procйdй, on peut introduire les vйgйtaux dans une enceinte, faire
circuler dans l'enceinte de la vapeur d'eau а la tempйrature T sous la pression P, et condenser la
vapeur d'eau sortant de l'enceinte pour sйparer de celle-ci l'huile extraite.
La mise en circulation de la vapeur d'eau dans l'enceinte est avantageusement rйalisйe par
pompage sous vide relatif de l'air et de la vapeur d'eau.
L'extraction de l'huile essentielle se fait ainsi а une tempйrature limitйe, ce qui permet
- d'amйliorer la qualitй de l'huile essentielle extraite,
- d'augmenter le rendement d'extraction, et
- de diminuer la consommation d'йnergie par rйduction du temps d'extraction.
De prйfйrence, pour amйliorer le rendement d'extraction, on effectue un pompage discontinu car
la mise en dйpression brutale favorise l'йclatement des cellules du vйgйtal et l'extraction de l'huile
essentielle.
La tempйrature T et la pression P utilisйes pour l'extraction sont choisies en fonction des vйgйtaux
traitйs. Gйnйralement, la tempйrature T est situйe dans la gamme de 60 а 800C et la pression P
est dans la gamme de 20 а 50kPa. De bons rйsultats peuvent кtre obtenus avec la plupart des
vйgйtaux а une tempйrature T de 75"C et une pression P de 38 kPa (285 mm de mercure).
L'invention concerne йgalement une installation d'extraction d'une huile essentielle а partir de
vйgйtaux, qui comprend
- une enceinte de traitement apte а contenir les vйgйtaux а traiter,
- un gйnйrateur de vapeur d'eau,
- un condenseur,
- un sйparateur huile essentielle-eau,
- un circuit reliant l'enceinte d'une part au gйnйrateur de vapeur et d'autre part au condenseur et
au sйparateur huile-eau,
362/1651
- des moyens de pompage sous vide relatif pour rйgler la pression de la vapeur d'eau provenant du
gйnйrateur au point de fonctionnement optimum,
- des moyens de rйgulation pour maintenir la tempйrature du gйnйrateur de vapeur а la valeur T
et la pression dans l'enceinte а une valeur P infйrieure а la pression atmosphйrique.
L'invention s'applique а de nombreux vйgйtaux, en particulier aux plantes mйdicinales et
aromatiques dont les huiles essentielles sont recherchйes. A titre d'exemple de telles plantes, on
peut citer la menthe, le romarin, la lavande, le lavandin, le tilleul, le geniиvre et la coriandre.
D'autres caractйristiques et avantages de l'invention apparaltront mieux е la lecture des exemples
suivants, donnйs bien entendu а titre illustratif et non limitatif en rйfйrence aux figures 1 et 2
annexйes.
La figure 1 reprйsente schйmatiquement en coupe verticale une installation d'extraction conforme
а l'invention et
La figure 2 reprйsente schйmatiquement en vue de dessus l'utilisation de quatre bacs а vйgйtaux
mobiles pour faciliter la mise en oeuvre du procйdй dans l'installation d'extraction.
Sur la figure 1, on voit que l'installation d'extraction conforme а l'invention comprend un gйnйrateur
de vapeur 1, une enceinte de traitement des vйgйtaux 3, un condenseur 5, un sйparateur eau-huile
essentielle 7 et une pompe а vide 9.
Le gйnйrateur de vapeur 1 comprend un rйservoir d'eau 11 disposй dans un bain-marie d'eau
chaude 13 qui est maintenu а la tempйrature voulue par circulation d'eau chaude provenant d'une
chaudiиre 15 par l'intermйdiaire de la conduite 17, une conduite 19 de vidange ou de recyclage
йtant prйvue а l'extrйmitй infйrieure du bain-marie 13.
La vapeur sortant du rйservoir 11 est amenйe par la conduite 21 dans l'enceinte de traitement 3
qui comporte а sa partie infйrieure une grille de retenue 22 pour les vйgйtaux а traiter. La vapeur
sortant de l'enceinte par la conduite 23 est amenйe dans le condenseur 5 oщ elle est refroidie par
une circulation d'eau froide par les conduites 24 et 26. On rйcupиre а la sortie du condenseur par
la conduite 25 le condensat comportant l'eau et l'huile essentielle qui est sйparй par dйcantation
dans le sйparateur eau-huile 7. L'eau et l'huile ainsi sйparйs peuvent кtre extraits par la conduite
27.
363/1651
La pression dans le circuit de vapeur est rйglйe par la pompe а vide 9 raccordйe sur la conduite
25 par l'intermйdiaire d'un ballon tampon 35.
Conformйment а l'invention, on peut faire fonctionner cette pompe en discontinu en fermant la
vanne 29 de faзon cyclique.
L'installation comporte de plus des moyens de rйgulation de la tempйrature 31 qui permettent de
rйgler la tempйrature de la vapeur sortant du rйservoir 11 а la valeur T voulue en agissant sur la
chaudiиre 15 en fonction de la tempйrature dйtectйe dans la conduite 21. Des moyens de
rйgulation de la pression 33 sont йgalement prйvus pour actionner la vanne 34 afin de rйgler le
vide en fonction de la pression dйtectйe dans l'enceinte de traitement 3.
Dans l'installation reprйsentйe sur la figure 1, on fait circuler la vapeur depuis le sommet jusqu'а la
base de l'enceinte de traitement 3, mais on pourrait йgalement adopter une disposition diffйrente
reprйsentйe en traits mixtes sur la figure 1 en faisant circuler la vapeur depuis le bas jusqu'au
sommet de l'enceinte de traitement comme reprйsentй en 3'.
Dans l'installation reprйsentйe sur la figure 1, on utilise une seule enceinte de traitement, mais
selon un mode prйfйrй de rйalisation reprйsentй sur la figure 2, l'installation comporte quatre
enceintes de traitement 3 identiques 31 32, 33 et 34 montйes sur un barillet 4 qui permet а chaque
enceinte d'кtre solidarisйe avec la conduite 21 et la conduite 23, tandis qu'on rйalise sur les autres
enceintes des opйrations de remplissage, de vidange et de nettoyage.
Ainsi, dans la position reprйsentйe sur la figure 2, l'enceinte 31 est associйe а un quai de
chargement de vйgйtaux qui permet d'assurer son remplissage, alors que l'enceinte 32 est en
cours de traitement en йtant reliйe au gйnйrateur de vapeur 1 et au condenseur 5, l'enceinte 33 en
cours de vidange des vйgйtaux qui ont йtй soumis prйcйdemment au traitement, et l'enceinte 34
en cours de nettoyage. Cette disposition permet ainsi d'utiliser l'installation en continu sans кtre
gкnйe par les opйrations prйalables de remplissage et les opйrations ultйrieures de vidange et
de nettoyage de l'enceinte de traitement.
On dйcrit ci-aprиs des exemples de traitement de vйgйtaux conformes а l'invention.
ExesRle 1 : Extraction d'huile essentielle de coriandre.
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On charge 200 g de graines de coriandre dans l'enceinte de traitement 3, puis on fixe cette
enceinte sur le circuit de vapeur en chauffant l'eau dans le rйservoir 11 а 75"C et en mettant en
service la pompe а vide 9 jusqu'а la valeur de pression dйsirйe de 285 mm de mercure, soit 38
kPa. On fonctionne dans ces conditions de pompage pendant 5 minutes, puis on effectue un
pompage discontinu pendant les 10 minutes qui suivent en rйalisant cycliquement 30 secondes de
pompage, suivies de 30 secondes sans pompage dans les mкmes conditions de pression. Pendant
les 5 minutes qui suivent, on rйalise le pompage en continu, puis pendant 10 minutes on reprend le
pompage en discontinu comme prйcйdemment, et on termine par 5 minutes de pompage en
continu. Ces conditions de pompage sont rйsumйes dans le tableau 1 ci-dessous.
TABLEAU 1
Temps d'extraction Type de pompage
de t = 0 а 5 min en continu
de t = 5 а 15 min en discontinu : 30" pompage
suivi de 30" sans pompage
de t = 15 а 20 min en continu
de t = 20 а 30 min en discontinu : (30"/30")
de t = 30 а 35 min en continu
Pour sйparer l'huile extraite, on rиgle la tempйrature dans le condenseur а 16C et on rйcupиre
l'huile essentielle dans le sйparateur 7.
On analyse ensuite l'huile extraite. Les rйsultats obtenus sont donnйs dans le tableau 2 qui suit.
TABLEAU 2
Composition de composition de
Composйs terpeniquer l'extrait de l'Ex. 1
l'extrait de l'Es.
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(en %) Comparatif (en %)
Alpha pinиne 1,3 9,9
Camphиne 0,1 0,9
Sabinиne 0,1 0,4
Bйta pinиne 0,1 0,5
Myrcиne 0,2 0,7
Para cymиne 2,3 4,2
Limonиne 0,9 1,9
Gamma terpinиne 6,5 10,0
Terpinolиne 0,3 0,4
Linalol 80,0 63,6
Camphre 3,5 2,9
Bornйol 0,1 0,1
Terpin-l-иne 4-ol 0,1 0,2
Alpha terpinйol 0,1 0,3
Gйraniol 0,8 1,6
Acйtate de linalyle 0,25 Tr
Acйtate de gйranyle 3,0 2,4
Exemple Comparatif 1
Dans cet exemple, on traite des graines de coriandre par un procйdй d'hydrodistillation en
utilisant de la vapeur d'eau а une tempйrature de 100"C et plus sous la pression atmosphйrique.
On analyse de la mкme faзon l'huile extraite. Les rйsultats obtenus sont donnйs йgalement dans le
tableau 1.
Au vu de ces rйsultats, on remarque que les terpиnes non fonctionnalisйs apparaissent en moins
grande quantitй par le procйdй de l'invention que dans une hydrodistillation traditionnelle. En
revanche, la proportion de linalol est plus importante dans le procйdй de l'invention (80 %), alors
qu'elle n'est que de 63,6 % dans le procйdй d'hydrodistillation. En effet, on йvite la dйgradation du
linalol en myrcиne, a-terpinйol et gйraniol dont les quantitйs sont plus importantes avec le
procйdй d'hydrodistillation.
On remarque de plus la prйsence d'acйtate de linalyle alors que celui-ci n'est prйsent qu'а l'йtat
de trace dans l'huile obtenue par hydrodistillation.
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Ainsi, l'extraction par le procйdй de l'invention donne une bonne qualitй d'huile essentielle et
constitue une vйritable amйlioration par rapport au procйdй d'hydrodistillation sous pression
atmosphйrique.
En effet, on limite la proportion des produits de dйgradation et on peut ainsi se rapprocher de la
qualitй olfactive de la graine broyйe.
Exemples 2 а 6 : Extraction d'huile essentielle de lavande.
Dans ces exemples, on suit le mкme mode opйratoire que dans l'exemple 1, mais on opиre а des
tempйratures et des pressions diffйrentes. On dйtermine en fin d'opйration le rendement
d'extraction, c'est-а-dire le poids d'huile sur le poids de lavande traitйe.
Les conditions d'extraction et les rendements obtenus sont donnйs dans le tableau 3.
TABLEAU 3
Ex T(0c > P(kPa) Rendement
2 < 60 < 20 0
3 60 20 trace d'huile
4 68 29 2,5 а 3,3
5 73 35 3
6 75 38 6
Au vu des rйsultats du tableau 3, on remarque que les meilleurs rйsultats sont obtenus lorsque la
tempйrature T est de 75 C et la pression P de 38 kPa (285 mm de mercure). Claims:
REVENDICATIONS
1. Procйdй d'extraction d'une huile essentielle а partir de vйgйtaux, caractйrisй en ce qu'il
consiste а mettre en contact les vйgйtaux avec de la vapeur d'eau а une tempйrature T infйrieure
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а 100"C, sous une pression P infйrieure а la pression atmosphйrique, pour extraire l'huile
essentielle dans la vapeur d'eau, puis а sйparer de la vapeur d'eau l'huile ainsi extraite.
2. Procйdй selon la revendication 1, caractйrisй en ce que l'on introduit les vйgйtaux dans une
enceinte, on fait circuler dans l'enceinte de la vapeur d'eau а la tempйrature T et on condense la
vapeur d'eau sortant du rйcipient pour sйparer de celle-ci l'huile extraite.
3. Procйdй selon la revendication 2, caractйrisй en ce que le rйglage de la pression de la vapeur
d'eau dans l'enceinte est obtenu par pompage sous vide relatif.
4. Procйdй selon la revendication 3, caractйrisй en ce que le pompage est discontinu ou non.
5. Procйdй selon l'une quelconque des revendications 1 а 4, caractйrisй en ce que T est de 60 а
80"C et P est de 150 а 350 mm de mercure (20 kPa а 50kPa.
6. Procйdй selon la revendication 5, caractйrisй en ce que la tempйrature T est de 75"C et la
pression P est de 38 kPa.
7. Procйdй selon l'une quelconque des revendications 1 а 6, caractйrisй en ce que les vйgйtaux
sont choisis parmi les plantes mйdicinales et aromatiques.
8. Procйdй selon l'une quelconque des revendications 1 а 7, caractйrisй en ce que les vйgйtaux
sont choisis parmi la menthe, le romarin, la lavande, le lavandin, le tilleul, le geniиvre et la coriandre.
9. Installation d'extraction d'une huile essentielle а partir de vйgйtaux, caractйrisйe en ce qu'elle
comprend
- une enceinte de traitement (3) apte а contenir les vйgйtaux а traiter,
- un gйnйrateur de vapeur d'eau (1),
- un condenseur (5),
- un sйparateur huile essentielle-eau (7),
- un circuit reliant l'enceinte d'une part au gйnйrateur de vapeur (1) et d'autre part au condenseur
(5) et au sйparateur huile-eau (7),
- des moyens de pompage (9, 34) sous vide relatif pour rйgler la pression de la vapeur d'eau
provenant du gйnйrateur (1) au point de fonctionnement optimum, et
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- des moyens (31, 33) de rйgulation pour maintenir la tempйrature du gйnйrateur de vapeur а la
valeur T et la pression dans l'enceinte а une valeur P infйrieure а la pression atmosphйrique.
369/1651
62. FR2721519 - 29.12.1995
DIFFUSER FOR VOLATILE SUBSTANCES E.G PERFUMES, ESSENTIAL OIL ETC.
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2721519
Inventor(s):
HISPA ROGER (--)
Applicant(s):
HISPA ROGER (FR)
IP Class 4 Digits: A61L
IP Class:
A61L9/03
E Class: A61L9/03
Application Number:
FR19940008235 (19940627)
Priority Number: FR19940008235 (19940627)
Family: FR2721519
Abstract:
DIFFUSER E.G. FOR A PERFUME, ESSENTIAL OIL, DEODORISING SUBSTANCE OR INSECTICIDE,
USES HEAT PRODUCED BY A LIGHT BULB (L) AND CONSISTS OF A BODY (1) IN THE SHAPE OF
A CROWN, HAVING A CENTRAL APERTURE (2) AND ONE OR MORE CAVITIES (3) FOR THE
VOLATILE SUBSTANCES (6). THE INNER SURFACE OF THE BODY HAS A SERIES OF
INDENTATIONS FORMING PROJECTIONS OR TEETH (4) POINTING TOWARDS THE CENTRE OF
ITS APERTURE (2). THE DIFFUSER IS MADE FROM A ZINC ALLOY, PREFERABLY 'ZAMAC' (RTM);
ITS CAVITIES (3) ARE IN THE SHAPE OF SCOOPS WITH DIVERGING WALLS AND FLAT BASES,
AND THE VOLATILE SUBSTANCES CAN BE CONTAINED IN PASTILLES OF POROUS
MATERIAL.Description:
370/1651
Diffuseur de substances йvaporables.
La prйsente invention concerne un diffuseur de substances йvaporables telles que, par exempLe,
parfums, essences de parfums, huiles essentielles, desodorisants, insecticides, etc., utilisant la
chaleur produite par une lampe d'йclairage qui peut кtre avantageusement constituйe par une
lampe а incandescence, une lampe hallogиne ou autre source de chaleur.
Il est connu d'utiliser la chaleur produite par une lampe а incandescence ou par une rйsistance
pour accйlйrer l'йvaporation de substances йvaporables telles que des essences de parfum
contenues dans un diffuseur.
Il existe, par exemple, dans le commerce, des diffuseurs annulaires rйalisйs en terre cuite et se
positionnant sur le sommet d'une ampoule а incandescance de la-pe d'йclairage classique qui
fournit une chaleur suffisante pour favoriser l'йvaporation du produit liquide dont ils sont
prйalablement imprйgnйs.
Toutefois, il s'avиre que la mise en oeuvre pratique d'un teL diffuseur prйsente plusieurs
inconvйnients non nйgligeables.
L'un de ces inconvйnients rйsulte du fait qu'en position d'utilisation, l'anneau de terre cuite se
trouve en contact etroit avec la totalitй de la pйriphйrie de la lape йlectrique, de sorte que ce
contact entraоne une surchauffe du filament et de l'ampoule de la lampe, laquelle est susceptible de
rйduire de faзon sensible la duree de fonctionnement des lampes et/ou de provoquer l'йclatement
des ampoules.
Un premier objectif de L'invention, est donc de remйdier а cet inconvйnient.
Pour cela, le diffuseur selon l'invention est rйalise sous forme de couronne dйlimitant une ouverture
centrale, et il est principalement remarquable par le fait qu'il comporte une indentation interne
constituйe par une pluralitй de saillies ou de dents d'appui dirigйes en direction du centre de cette
ouverture et dont les sommets sont disposйs sur un cercle, ces saillies ou dents d'appui йtant, de
prйfйrence, rйguliиrement rйparties autour de ladite ouverture centrale.
Grвce а cette disposition, lorsque le diffuseur selon l'invention est en position d'utilisation sur une
lampe, il se trouve en contact ponctuel avec L'ampoule seulement par l'intermйdiaire du sommet
371/1651
des saillies ou dents d'appui, de sorte que l'air peut circuler autour de ladite ampoule, ce qui evite
une йlйvation excessive de temperature susceptible d'entratner une mise hors d'usage
prйmaturйe de la lampe.
Les diffuseurs en terre cuite connus prйsentent en outre les autres inconvйnients ci-apres : - leur
structure en terre cuite ne permet pas leur chauffage rйgulier, d'oщ une йvaporation irrйguliиre
des produits ; - le chauffage de la terre cuite entraine, dans un premier temps, une diffusion des
substances dans la structure des diffuseurs, ce qui retarde L'йvaporation desdites substances ; - en
cas de changement de parfum ou autres substances йvaporables, des molйcules du produit
prйcйdemment utilisй restent dans les pores de la structure de terre cuite et peuvent reagir avec
celles du nouveau produit en entrainant une alteration de l'odeur ou, selon le cas, de L'action de ce
dernier.
Un autre objet de l'invention est donc de remйdier йgalement а ces inconvйnients.
Selon une autre disposition caractйristique de l'invention, cet objectif est atteint grвce а la
rйalisation du diffuseur en alliage de zinc et, plus prйcisйment, en alliage de zinc connu sous le
nom de "Zamac" (Marque deposйe).
Cette disposition caractйristique permet une diffusion rйguliиre de la chaleur dans la structure
cristalline du diffuseur et, par consйquent, une йvaporation rйguliиre des parfums ou autres
produits. En outre, la substance parfumante ou active, n'est pas absorbйe ou dйnaturйe par la
structure non poreuse du diffuseur, avant son йvaporation, mais diffusйe dans l'environnement avec
toutes ses qualitйs.
D'autre part, Le "Zamac" (Marque dйposйe), par sa masse molaire йlevйe donne au diffuseur un
poids qui participe а sa stabilitй lorsqu'il est posй sur le sommet d'une Lampe.
Un autre inconvйnient des diffuseurs en terre cuite connus, rйside dans le fait qu'ils ne permettent
pas d'intervenir sur la rapiditй du processus d'йvaporation, ni sur les quantitйs de produits
souhaitables. En outre, ils ne permettent pas la diffusion simultanйe de plusieurs produits
йvaporables prйsentant des senteurs ou caractйristiques diffйrentes.
Un autre objet de l'invention est de remйdier aussi а ces inconvйnients.
372/1651
Pour cela, le diffuseur selon l'invention comporte une pluralitй de cavitйs ou godets rйpartis autour
de son ouverture centrale.
La quantitй de produit а diffuser peut donc кtre aisйment adaptee en fonction du volume des
piиces ou locaux, en utilisant tous les godets disponibles ou une partie d'entre eux seulement.
D'autre part, il est possible d'utiliser un ou plusieurs godets pour diffuser un parfum choisi et un ou
plusieurs godets pour diffuser un autre parfum ou un produit ayant une action diffйrente tel qu'un
insecticide par exemple.
En outre, on peut intervenir sur la vitesse de l'йvaporation des produits. En effet, si l'on souhaite
obtenir une йvaporation rapide, les produits sont versйs ou dйposйs directement dans les cavitйs
ou godets du diffuseur, tandis que si l'on souhaite une йvaporation lente, les produits liquides sont
versйs sur une pastille de matйriau poreux que l'on dispose dans lesdits godets.
On conзoit aussi, comme indiquй prйcйdemment, que L'on peut deposer des produits de senteur
ou de nature diffйrente dans les godets du diffuseur, de sorte qu'il n'y a aucun risque de mйlange
ou de rйaction entre les produits avant leur йvaporation.
Les buts, caractйristiques et avantages ci-dessus, et d'autres encore, ressortiront mieux de la
description qui suit et des dessins annexйs dans lesquels
La figure 1 est une vue en plan d'un exemple de rйalisation du diffuseur selon L'invention.
La figure 2 est une vue en coupe selon la ligne 2-2 de la figure 1.
La figure 3 est une vue de dйtail, а plus grande йchelle et en coupe, de l'un des godets ou
cavitйs rйceptrices du diffuseur.
La figure 4 est une vue en coupe verticale montrant le diffuseur selon l'invention en position
d'utilisation sur le sommet d'une Lampe йlectrique du type ampoule а incandescence.
On se reporte auxdits dessins pour dйcrire un exemple de rйalisation intйressant, quoique
nullement Limitatif, du diffuseur de substances йvaporables selon l'invention.
Ce diffuseur comprend un corps 1 en forme de couronne dйlimitant une ouverture centrale 2 et
comportant au moins une cavitй 3 pour la rйception des produits йvaporables а diffuser.
373/1651
Selon une premiиre disposition caractйristique de l'invention, ce corps comporte une indentation
interne constituйe par une pluralitй de saillies ou dents d'appui 4 dirigйes en direction du centre de
L'ouverture 2 et, de prйfйrence, rйguliиrement rйparties autour de cette derniиre.
Ces dents d'appui 4 ont avantageusement un sommet pointu 4a et leurs deux cфtйs forment, par
exemple, un angle de l'ordre de 130 degrйs. Le corps 1 prйsente ainsi, interieurement, une
conformation йtoilйe ou en dents de scie dont les parties saillantes ou dents 4 ont leurs sommets 4a
rйguliиrement rйpartis sur un cercle. En outre, comme le montre plus particuliиrement la figure 3,
les sommets 4a des dents d'appui peuvent prйsenter au moins une portion oblique 4b orientee de
maniиre а s'йloigner de l'axe du corps 1 dans la direction haut-bas.
Le bord extйrieur du corps 1 peut йgalement prйsenter une conformation йtoilйe dont les parties
rentrantes permettent une meilleure prise en main du diffuseur.
Le diffuseur йtant appelй а кtre positionnй sur et autour de la partie supйrieure d'une ampoule de
Lampe а incandescance ou autre, il peut кtre exйcutй en diffйrentes dimensions et notamment
avec une ouverture centrale 2 adaptee а des ampoules de diffйrentes grosseurs disponibles dans
le commerce, le cercle sur lequel se trouvent disposйs les sommets 4a des saillies ou dents d'appui
4 devant avoir un diamиtre plus rйduit que le plus grand diamиtre de la partie renflee desdites
ampoules.
Selon une autre disposition caractйristique de l'invention, le diffuseur est exйcutй en alliage de
zinc dont la structure cristalline permet d'obtenir une tempйrature rйguliиre sur l'ensemble du
diffuseur, et, plus prйcisйment, en un alliage de zinc du type Zn-Al-Cu, ou
Zn-Al-Mg, ou Zn-Al-Cu-Mg, connu sous le nom de "Zamac" (Marque dйposйe).
Selon une autre disposition caractйristique de l'invention, le diffuseur comporte une pluralitй de
cavitйs ou godets 3 rйpartis autour de son ouverture centrale 2.
Selon L'exemple illustrй, les cavitйs ou godets 3 sont au nombre de quatre et ont une forme
circulaire, mais il est йvident qu'ils pourraient кtre en nombre diffйrent ou avoir toute autre forme.
Ces cavitйs ou godets 3 sont dimensionnйes pour recevoir quelques gouttes d'un produit
йvaporable 5 (godet gauche de la figure 2), ou une pastille 6 imprйgnйe de substances volatiles
374/1651
(godet droit de la figure 2), ou une pastille de matйriau spongieux ou poreux que L'on peut imbiber
d'un produit liquide йvaporable.
Les cavites ou godets 3 sont rйpartis rйguliиrement ou non autour de L'ouverture centrale 2, mais
dans le second des cas, ils sont disposйs symйtriquement, de sorte que le diffuseur puisse rester
parfaitement stable lorsqu'il se trouve disposй horizontalement sur et autour de la partie supйrieure
d'une ampoule йlectrique.
Les cavitйs ou godets 3 ont, de maniиre prйfйrйe un fond plat 3a et une paroi latйrale 3b
s'йvasant en direction du haut, pour favoriser L'йvaporation et la diffusion des substances volatiles.
Le diffuseur peut кtre complйtй par des pastilles 6 de matйriaux spongieux ou poreux
imprйgnйes de produit evaporable ou apte а кtre imprйgnйes de tels produits.
Dans ce cas, ces pastilles sont conformйes et dimensionnйes pour pouvoir se loger, sans jeu
excessif, dans les cavitйs 3. Elles ont, notamment lorsqu'il s'agit de pastilles spongieuses ou
poreuses rechargeables, une hauteur lйgиrement supйrieure а la hauteur des cavitйs 3 (figure 2),
de faзon а pouvoir en кtre retirйes facilement.
La figure 4 montre le diffuseur en position d'utilisation sur le sommet d'une lampe L du type lampe
а incandescence.
On comprend que la chaleur produite par la Lampe est recupйree par le diffuseur 1 dont
L'йchauffement favorise l'йvaporation ou volatilisation du produit йvaporable imprйgnant les
pastilles 6 logйes dans les godets 3. Dans ce cas, on obtient une йvaporation lente du produit.
Pour obtenir une diffusion plus rapide, il suffit de verser le produit directement dans les cavites
rйceptrices ou godets 3 du diffuseur. Claims:
REVENDICATIONS
375/1651
1. - Diffuseur de substances йvaporables telles que, par exemple, parfums, essences de parfums,
huiles essentielles, desodorisants, insecticides, utilisant une source de chaleur produite par une
lampe et comprenant un corps (1) en forme de couronne dйlimitant une ouverture centrale (2) et
pourvu d'au moins une cavitй (3) pour la rйception desdites substances (5, 6), caractйrisй en ce
que le bord interne dudit corps dйlimitant cette ouverture centrale, comporte une indentation
constituйe d'une pluralitй de saillies ou dents (4) orientйes en direction du centre de ladite
ouverture centrale (2).
2. - Diffuseur de substances йvaporables selon la revendication 1, caractйrisй en ce qu'il est
executй en alliage de zinc et, de prйfйrence, en alliage de zinc connu sous le nom de "Zamac"
(Marque dйposйe).
3. - Diffuseur de substances йvaporables suivant L'une des revendications 1 ou 2, caractйrisй en
ce qu'il est pourvu d'une pluralitй de cavitйs ou godets (3) rйpartis autour de
L'ouverture centrale (2).
4. - Diffuseur de substances йvaporables selon la revendication 1, caractйrisй en ce que les dents
(4) ont un sommet pointu (4a).
5. - Diffuseur de substances йvaporables suivant l'une des revendications 1 ou 4, caractйrisй en ce
que les sommets (4a) des saillies ou dents (4) sont disposйs sur un cercle.
6. - Diffuseur de substances йvaporables selon l'une quelconque des revendications 1, 4 ou 5,
caractйrise en ce que les saillies ou dents (4) sont rйguliиrement espacйes, de sorte que le bord
interne du corps (1) a une conformation en dents de scie.
7. - Diffuseur de substances йvaporables selon L'une quelconque des revendications 1, 4, 5 ou 6,
caractйrisй en ce que les sommets (4a) des dents (4) comportent au moins une portion pentee (4b)
dont l'inclinaison tend а s'йloigner de l'axe du corps (1) dans la direction haut-bas.
8. - Diffuseur de substances йvaporables selon la revendication 3, caractйrisй en ce que les
cavitйs ou godets (3) ont une paroi latйrale (3b) s'йvasant en direction de l'extйrieur et, de
prйfйrence, un fond plat (3a).
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9. - Diffuseur de substances йvaporables suivant L'une des revendications 3 ou 8, caractйrisй en
ce que les cavitйs ou godets (3) sont disposйs symйtriquement.
10. - Diffuseur de substances йvaporables selon l'une des revendications 3, 8 ou 9, caractйrisй en
ce qu'il comprend des pastilles spongieuses ou poreuses (6) imprйgnйes de substances
йvaporables ou aptes а кtre imprйgnйes de telles substances, ces pastilles йtant dimensionnйes
et conformes pour pouvoir se loger dans les cavitйs ou godets (3), et ayant, de prйfйrence, une
hauteur lйgиrement supйrieure а la profondeur de ces derniers.
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63. FR2734157 - 22.11.1996
HOT OLEOHYDROSALINE AEROSOL USES SPA OR SEA WATER AND ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2734157
Applicant(s):
NIAUDET PATRICE YVES GUY (FR)
IP Class 4 Digits: A61K
IP Class:
A61K35/78; A61K9/72; A61K35/08
E Class: A61K9/00M20B
Application Number:
FR19950005904 (19950518)
Priority Number: FR19950005904 (19950518)
Family: FR2734157
Abstract:
NEW HOT OLEOHYDROSALINE AEROSOL HAS MEDICAL USE PARTIC. AGAINST DAMAGE TO
THE ATMOSPHERE. IT COMPRISES A MIXT. OF SEAWATER OR SPA WATER AND ESSENTIAL OIL
WHICH IS HEATED AND NEBULIZED BY A GENERATOR COMPRESSOR (PROTOTYPE AZ41)
USING THE "HOT AEROSOL SOLUTION" TECHNIQUE. EXAMPLES OF ESSENTIAL OILS ARE
OREGANO, MARJORAM AND CITRONELLA OILS AND ESSENTIAL OLIVE OIL.Description:
DESCRIPTION
En temps qu'inventeur et premier dйposant,la prйsente invvention concerne l'utilisation d'un
aйrosol chaud olйohydrosalin,produit par un gйnйrateur coipresseur nйbuliseur proto type.L'йtat
actuel de cette tйchnique nйcessitant des normes de standa"disation pour une fiabilitй aux
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applications multiples privйes,coilectives ou publiques.Seul le champ d'investigations mйdicales
sera envisagй et dйveloppй ici.
DEMONINATION: Tйchnique d'aйrosol chaud olйohydrosalin.
COMPOSITION: Eau de mer standardisйe en ampoules de dix milli- litres;huile essentielle
standardisйe en flacon compte gouttes selon l'indication mйdicale;eaux thermales.
DC INDICATIONS: Tout l'arbre respiratoire,et les voies oto -rhino-laryngologiques;la surface cutanйe
dans son ensemble ; sitфt qu'un prйjudice ambiant atmosphйrique peut кtre dйtectй.
La simple amйlioration de confort physiologique et les travaux en cours dans le domaine de la
mйdecine du Sport en йlargiront les indications aussitфt les preuves йtablies.L'utilisation de ce
support comme vйhiculant d'une molйcule ou d'un produit thйrapeutique voir gйnйtique ou
vaccinal parant Outre rйalisй.L'origen, la marjolaine,la citronnelle et l'huile essentielle d'olive seront
retenues а titre d'exemple,pour les diffйrentes propriйtйes pharmacologiques qu'elles prйsentent.
DC POSOLOGIE ET MODE D'ADMINISTRATION:Une goutte d'huile essentielle pour dix millilitres
d'eau thermale ou de mer.Sйan- ces de dix а vingt minutes d'aйrosol prйchauffй selon les
indications mйdicales retenues.Applications individuelles ou а groupe de sujets dans des locaux
adйquates et adaptйs.
DC CONTRE INDICATION: Aucune retenue а ce jour.
DC MISE EN GARDE ET PRECAUTIONS: Durйe d'exposition limitйe, propretй du matйriel
utilisй,controlй avant chaque utilisation et nettoyage pour йviter tout corps йtranger, tous produits
contaminйs,toxiques ou dangereux.
DC INTERACTIONS MEDICAMENTEUSES: Aucune retenues а ce jour.
DC GROSSESSE ET ALLAITELENT; aucun travaux n'йtant publiйs а ce jour,les prйcautions et le
recul resteront observйs.
DO CONDUITE ET UTILISATION DE MACHINE: Aйrosol rйalisй avec un prototype AZ 41 de la
DIFFUSION TECHNIQUE FRANCISE ATOMISOR - HERCENDOR KITET, pouvant кtre alimentй
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sur le secteur ou а un groupe йlectrogиne en ambulatoire et nйcessitant une auto risation de
L'utilisation dans les diffйrents moyens de transports nйssecitant l'accord des constructeurs pour
rйpondre aux normes de sйcuritй.
DC EFFETS INDESIRABLES: Risque d'hyperhydratation intracellulaire en cas d'utilisation
prolongйe.Une а deux sйances par jour durant quinze jour+aiimum0 Aucune dйpendance ou
accoutumance n'ont йtй relevйes а ce jour. Produits testйs rйguliиrement depuis le 18 octobre
1984.
DC SURDOSAGEtL'aйrosol йtant limitй}!au dйbit du nйbuliseur; il n'existe pas de risque de
surdosage avec les produits utilisйs,
Seules des quantitйs anormalement concentrйes d'huiles essentielles et mйlangйes seraient
toxiques.
PP PHASTMACODYNAMINE:Production de micelles d'un demi micron, ayant un fort pouvoir de
pйnйtration et amйliorant les йchanges alvйolo-capillaires au niveau de l'arbre
respiratoire.L'aйrosol chauffй а 38 au maximum йvite toute rйaction anormale locale.
L'apport d'oligoйlйments catalysant toutes les rйactions m6ta- boliques;activant la cascade de
dйgradation de l'acide arachidonique,et la stimulation de la guanylate cyclase . Ce procйdй peut
donc кtre considйrй comme un puissant dйtoxiquant а la lumiиre des travaux а venir.
PP PHARMACOCINETIQUE: Les diffйrent produits utilisйs restent des produits physiologiques aux
normes prйconisйes. La prise en charge dans l'organisme respectant l'homйostasie.
PP SECURITE PRECLINIQUE:Tous les statstathologiques doivent e n tout йtat de cause pris en
considйration et ne reprйsentent а ce jour aucune contre indication.
INCOMPATIBILLITE: Matйrial d'aйrosol adaptй aux produits utilisйs#
DP CONDITIONS DE CONSERVATION: Les produits utilisйs rйpondent а des normes prйcises,et
les prйparations sont extemporannйes.
Les huiles essentielles conservйes а l'abri de la lumiиre.
cette
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DP MODALITES DE MANIPULATION: Achat ou location de l'appareil dйlivrant l'aйroSOl;nйtessitant
une dйclaration d'utilisation et le rиglement d'une redevance annuelle rйvisible chaque annйe et
non cessible.Un contrфle de vйrification de fonctionnement et du respect d'utilisation pouvant кtre
effectuй par le service des fraudes et usage de faux et sanctionnй en cas d'anomalie .Tous
renseignement administratifs йtant dйlivrйs par la firme productrice du matйriel йmettant
l'aйrosols La
DIFFUSION TECHNIQUE FRANCAISE, 114-120 rue Bergson, BP 132, 42003 SAINTETIENNE.EDEXI.T 77.74.51.11.Fax 77.79.67.72.
Tx 300772 DTF.
RENSEIGNEMENTS ADMINISTRATIFS:Condition de dйlivrance:Liste I.
Visa ou AMt:
Titulaire de l'autorisation de mise sur le marchй:Le fabriquant et l'inventeur de la tйchnologie
d'utilisation pour les indications retenues.
Quatre photographies sont Jointes en annexe la description de l'appareil et le montage pour son
utilisation sont Jointe tu matйriel au moment de la livraison et indйpendante de la description du
brevetla dйnomination H.A.S (Hot Aerosol Solutio n) est proposйe pour cette technique moderne qui
peut elle uOme кtre baptisйe OY.
Les applications industrielles dans le domaine des transports, de l'agriculture et de l'aйrospacial
sont а envisager. Claims:
REVENDICATIONS
1) L'aйrosol chaud olйohydrosalin rйpond а des nйcessitйs mйdicales, pour des indications
prйcises contre les prйjudices atmosphйriques ambiants et leurs rйpercussions chez l'кtre
humain;il est caractйrisй par le mйlange d'eau thermale ou marine et d'huile essentielle, le tout
йtant rйchauff t nйbulisй par un gйnйrateur compresseur : prototype AZ 41 dйnommй H.A.S
381/1651
( Hot Aerosol Solution ); mйthode OY 2) L'aйrosol selon la revendication 1) se fait avec un mйlange
hydrique, huileux et salin chauffй.
382/1651
64. FR2748204 - 07.11.1997
ANTISEPTIC USE OF DISTILLED MELALEUCA ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2748204
Applicant(s):
INTEREXPORT SERVICES (FR)
IP Class 4 Digits: A61K
IP Class:
A61K35/78; A61K7/48; A61K31/01
E Class: A61K8/31; A61K8/92C; A61Q19/00; C11B9/02B; A61Q5/00; A61K35/78; A61Q5/02;
A61K8/34
Application Number:
FR19960005612 (19960506)
Priority Number: FR19960005612 (19960506)
Family: FR2748204
Abstract:
COSMETIC OR PHARMACEUTICAL COMPOSITIONS, PARTICULARLY FOR USE IN SKIN CARE OR
FOOD, COMPRISE A RECTIFIED MELALEUCA TERPINEN-4-OL ESSENTIAL OIL, CONTAINING
LESS THAN 0.5% LIMONENE, ALPHA -PINENE, BETA -PINENE AND 1,8-CINEOL.Description:
Le genre Melaleuca appartient а une famille botanique, les Myrtaceae, aux nombreuses plantes
fortement aromatiques (Myrtes, Eucalyptus, Giroflier...). I1 comprend plus de 100 espиces
originaires d'Ocйanie. Trois d'entre elles sont trиs exploitйes pour leur intйrкt thйrapeutique: Le
Niaouli (Melaleuca viridiflora Gaertn.), le Cajput (Melaleuca leucadendron L.) et l'Arbre а thй
(Melaleuca alternifolia Cheel)
La dйcouverte initiale de l'йtonnant pouvoir antiseptique de l'huile essentielle des feuilles du
383/1651
Melaleuca alternifolia appelй dans les pays anglo-saxons "Tea Tree Oil" remonte а 1925.
Depuis, bien des йtudes scientifiques ont confirmй les effets antibactйriens et antifongiques de
cette huile essentielle. Une synthиse de ces travaux permet d'йtablir la liste des principaux microorganismes sensibles а cette huile essentielle
Staphylococcus aureus, Streptococcus sp., Enterococcus sp., Propionibacterium acnes,
Escherichia coli, Pseudomonas aeruginosa, Proteus vulgaris, Legionella sp., Enterobacter sp.,
Salmonella typhi, Candida albicans, Aspergillus niger, Trichophyton mentagrophytes,
Trichophyton gypseum, Trychophvlon rubrum.
La premiиre norme de qualitй portant sur l'huile essentielle de Melaleuca alternifolia a йtй publiйe
en 1967 par "the Standard Association ofAustralia" Cette norme n'йtant pas assez fiable pour
assurer une activitй antimicrobienne reproductible de l'huile essentielle, une nouvelle norme a йtй
йtablie en 1985 par l'Australian Standard (AS 2782). Cette seconde norme, а la diffйrence de la
premiиre, n'est pas spйcifique а Melaleuca alternifoha mais s'applique aux Melaleuca riches en
terpinиne-4-ol. Ainsi, la norme AS 2782 prйcise que les huiles essentielles de Melaleuca type
"terpinиne-4-ol" doivent contenir - un taux minimum de 30 % de terpinиne-4-ol - un taux de 1,8cinйole qui ne doit pas excйder 15 %
En 1991, une norme AFNOR NF T-75-358 a repris les exigences de la norme australienne
AS 2782 en y ajoutant des limites portant sur 11 constituants (en plus des limites du terpinиne-4-ol
et du 1,8-cinйole) gamma-terpinиne 10,0 а 28,0 % I aromadendrиne : traces а 7,0 % alphaterpinиne . 5,0 а 13,0 % l sabinиne : traces а 3,5 % alpha-terpinйol 1,5 а 8,0 % I delta-cadinиne:
0 а 8,0 % alpha-terpinolиne: 1,5 а 5,0 % l globulol 0 а 3,0 % p-cymиne : 0,5 а 12,0 % I viridifiorol
0 а 1,5 % d-limonиne . 0,5 а 4,0 % I
Une norme internationale ISO 4730 est parue en 1992. Elle reprend йgalement les exigences de la
norme australienne AS 2782, en y ajoutant des limites relatives а 7 constituants. Ces limites sont les
memes que celles de la norme AFNOR NF T-75-358 (cidessus) sauf pour les composйs suivants:
Absence de limites pour: aromadendrиnes, sabinиne, delta-cadinиne, globulol et viridifiorol.
Par contre, une limite supplйmentaire: alpha-pinиne 1,0 а 6,0 %
Toutes ces normes en vigueur ont permis de bien caractйriser l'huile essentielle, d'йviter
d'йventuelles falsifications, d'assurer ainsi un pouvoir antiseptique satisfaisant, en prenant des
prйcautions а l'йgard du 1,8-cinйole considйrй par certains comme irritant pour la peau.
384/1651
Cependant, l'huile essentielle de Melaleuca type terpinиne-4-ol usuelle prйsente malgrй ces
normes, deux inconvйnients majeurs pour des applications cosmйtiques, pharmaceutiques ou
alimentaires: son odeur et sa tolйrance au niveau cutanй.
L'odeur des huiles essentielles de Melaleuca type terpinиne-4-ol est fortement aromatique
rappelant un mйlange d'eucalyptus, de rйsine fraоche de pin, et de tйrйbenthine. Trois notes trop
prononcйes rendent cette odeur gкnante : une note de tкte dйsagrйable due aux "terpиnes"
(pinиnes, myrcиne, limonиne...); une note dure provenant du 1,8-cinйole; une note due au
gamma-terpinиne qui persiste sur la peau aprиs йvaporation des composйs les plus volatils. Cette
odeur s'avиre donc peu compatible avec nombre de formulations cosmйtiques, dermatologiques,
ou alimentaires.
Les huiles essentielles usuelles d'Arbre а thй ne prйsentent pas une tolйrance cutanйe
suffisamment satisfaisante. En effet, des cas d'irritations suite а l'application prolongйe et rйpйtйe
d'huiles essentielles de Melaleuca type terpinиne-4-ol sur la peau ont йtй signalйs а plusieurs
reprises dans la littйrature. CARSON C.F., RILEY V. (Clinical Toxicol., 1995, 33, 2, pp. 193-194).
Plusieurs auteurs ont mis en cause certaines substances -Pour Knight T.E. et collaborateurs (J. Am.
Acad. Dermatol., 1994, 30, 3, pp. 423-427), le limonиne serait l'agent le plus frйquemment
allergisant chez des sujets traitйs localement par l'huile essentielle d'Arbre а thй.
-Pour VAN DER VALK P.G. et collaborateurs (Ned. Tijdschr Geneeskd, 1994, 138, 16, pp.
823-825), LASSEK E.V. et collaborateurs (Austr. Med. Plants, 1983, p. 97), BARNES B.
(Modern Phytotherapy, The clinical significance ofTea Tree and other essential oils, pp. 3542), les
soupзons se porteraient sur le 1-8-cinйole.
Parmi les composants naturels les plus frйquemment citйs dans la littйrature pour leurs effets
allergisants on trouve l'alpha-pinиne et le limonиne.
L'objet du prйsent brevet repose sur la mise au point d'un produit nouveau et naturel prйparй а
partir d'une huile essentielle de Melaleuca type terpinиne-4-ol et ne prйsentant plus les deux
inconvйnients йvoquйs prйcйdemment. Cette huile essentielle particuliиre se distingue de l'huile
essentielle courante (dйfinie par la norme AFNOR NF T-75-358) par sa composition diffйrente et son
385/1651
procйdй de purification (rectification) qui permet d'йliminer ou de fortement diminuer la prйsence
de plusieurs groupes de composйs prйsents dans l'huile essentielle courante: - des composйs
responsables de l'odeur gкnante - des composйs mal tolйrйs par la peau - des substances de
faible intйret antiseptique.
Le procйdй permet aussi d'augmenter l'activitй antiseptique de l'huile essentielle rectifiйe
comparйe а une huile essentielle de Melaleuca type terpinиne-4-ol usuelle.
Les huiles essentielles de Melaleuca type terpinиne-4-ol sont obtenues selon la mйthode
traditionnelle par hydrodistillation ou entraоnement а la vapeur d'eau а pression atmosphйrique
des feuilles fraоches et des jeunes rameaux du Melaleuca.
Pour la prйparation d'une huile essentielle rectifiйe de Melaleuca type terpinиne-4-ol quatre
mйthodes de fractionnement (ou rectification) ont йtй examinйes:
Fractionnement au moyen d'йthanol а 60 % v/v
Fractionnement par chromatographie sur colonne
Fractionnement en йtuve sous pression rйduite
Rectification par distillation sous pression rйduite
Exemple 1: Fractionnement au moyen d'йthanol а 60 % v/v 1 ml d'huile essentielle de Melaleuca
type terpinиne-4-ol est extrait par 4 ml d'йthanol а 60 % v/v sous agitation а tempйrature de 20"C
pendant 10 minutes. Le mйlange est ensuite centrifugй. La fraction surnageante est analysйe par
chromatographie en phase gazeuse.
Le rйsultat du chromatogramme montre que le terpinиne-4-ol reprйsente 35,7 % de la fraction
surnageante et 39,4 % de la fraction hydroalcoolique. Cette mйthode manque donc de sйlectivitй
vis а vis du terpinиne-4-ol.
Exemple 2 : Fractionnement par chromatographie sur colonne 0,1 ml d'huile essentielle de
Melaleuca type terpinиne-4-ol est mйlangй avec du gel de silice, puis le mйlange est placй sur
une colonne de gel de silice G 60. L'huile essentielle est йluйe successivement par de l'hexane, de
l'йther diйthylique puis du mйthanol.
Une analyse des 3 fractions par Chromatographie en phase gazeuse montre que l'on retrouve dans
chacune des fractions du terpinиne-4-ol. Ce dernier reprйsente 24 % de la fraction йluйe par
l'hexane, 67 % de la fraction йluйe par йther et 12 % de la fraction йluйe par le mйthanol.
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Cette technique permet de sйparer plus finement les catйgories de molйcules en fonction de leurs
polaritй comparйe а celle dйcrite а l'exemple 1. Cependant, le terpinкne-4-ol reste prйsent en
quantitй notable dans les diffйrentes fractions. D'autre part, cette mйthode prйsente l'inconvйnient
de mettre en oeuvre plusieurs solvants organiques.
Exemple 3 : Fractionnement en йtuve sous pression rйduite
0,5 ml d'huile essentielle de Melaleuca type terpinиne-4-ol sont placйs dans une йtuve
chauffйe а 450C pendant 18 heures sous pression rйduite. L'opйration achevйe, il s'avиre que
40 % de l'huile essentielle s'est йvaporйe.
L'analyse par chromatographie en phase gazeuse montre que l'huile essentielle rйsiduelle
contient 56 % de terpinиne-4-ol, contre 40 % initialement. Un fractionnement dans des
conditions identiques pendant 4 heures (au lieu de 18 heures) fournit une composition de
l'huile essentielle identique а la composition initiale avant traitement. Une durйe intermйdiaire
serait а examiner.
Exemple 4 : Fractionnement par distillation sous pression rйduite
50 litres d'huile essentielle de Melaleuca alternifolia sont placйs dans une cuve йquipйe d'une
colonne de distillation dont le nombre de plateaux thйoriques est voisin de 30. La colonne
comprend un garnissage ordonnй, inox, de marque Sulzer. Un vide de 4-7 mm de mercure
accompagnй d'un reflux а tempйrature variable a permis d'aboutir а l'obtention d'une huile
essentielle rectifiйe particuliиrement intйressante.
D'aprиs les rйsultats d'analyse par chromatographie en phase gazeuse, il apparaоt que l'huile
essentielle prйparйe par distillation sous pression rйduite est trиs fortement "dйterpйnйe". Elle
est dйbarrassйe de la note de tкte dйsagrйable, de la note "dure" et de la note due au gamma
terpinиne, ainsi que des principales substances considйrйes comme irritantes pour la peau.
Le tableau, ci-aprиs, prйsente d'une part la composition d'huiles essentielles type terpinиne-4ol usuelles (non rectifiйes), et, d'autre part, la composition de l'huile essentielle rectifiйe par
distillation sous pression rйduite d'une huile essentielle usuelle.
-------Composants majeurs---lHuile essentielle usuelle l Huile -------(*)------------------------l valeurs
extrкmes ¦ essentielle ------- ---------------------------l (mini. et maxi.)(*) rectifiйe 1-terpinиne-4-ol--------¦
387/1651
28,6 а 59,9 % l 67,3 % -------gamma-terpinиne-------l 9,5 а 28,3 % 1,8 % ------- 1,8-cinйole -------------l 0,5 а 17,7 % 1 0,09 % -------alpha-terpinиne ---------l 4,6 а 12,8 % l 0,06 % -------p-cymиne---------------l 0,4 а 12,4 % 0,2 % -------alpha-terpinйol----------l 1,5 а 7,6 % l 7,4 % -------delta-cadinиne ---------l 0,1 а 7,5 % 1 3,6 % ------- aromadendrйne ---------I 0,1 а 6,6 % ? ------- vindinorиne ------------1 0,3 а 6,1 % l
terpinolиne j 1,6а 5,4% 1 1,9% -- alpha-pinйne ------------1 0,8 а 3,6 % 1 0,01 % -------globulol-----------------l 0,оа 3,0% 1 0,6% -------limonиne-----------------l 0,4 а 2,7 % 1 0,02 % -------alphaphellandrиne-----l 0,1 а 1,9 % 0 -------myrcиne-----------------¦ 0,1 а 1,8 % l 0 -------beta-pinиne-------------l 0,1 а 1,6% I 0
(*) Selon BROPHY J.J. et collaborateurs (J. Agric. Food Chem., 1989, 37, pp. 1330-5).
Le tableau ci-dessus montre que le procйdй par distillation sous pression rйduite a permis de
rйduire а l'йtat de traces les composйs indйsirables suivants : 1,8-cinйole (trиs odorant et mal
tolйrй), limonиne, alpha-pinиne et beta-pinиne (sensibilisants).
Le nouveau produit naturel selon la prйsente invention correspond а une huile essentielle rectifiйe
de Melaleuca type terpinиne4-ol dйfinie par la composition chimique suivante: - la somme des taux
de limonиne, d'alpha-pinиne, de beta-pinиne et de 1,8-cinйole dans l'huile essentielle rectifiйe
n'excиde pas 0,5 % en poids.
- le taux de terpinиne-4-ol contenu dans l'huile essentielle rectifiйe n'est pas infйrieur а 60 % en
poids - la somme des taux d'alpha-terpinиne et gamma-terpinиne contenus dans l'huile essentielle
rectifйe revendiquйe n'excиde pas 5,0 % en poids - l'huile essentielle rectifйe revendiquйe
contient en particulier de l'alpha-terpinйol, du cadinиne et du terpinolиne
Parmi les diffйrentes espиces de Melaleuca type terpinиne4-ol utilisйes pour la prйparation du
nouveau produit selon l'invention, on peut citer : Melaleuca alternifolia, Melaleuca linarfifolia
Melaleucadisirifolia
Activitй antiseptique des composants de l'huile essentielle rectifiйe
Les activitйs antimicrobiennes des 7 composants principaux de l'huile essentielle de
Melaleuca alternifolia ont йtй comparйes et rapportйes par CARSON C.F. et RILEY V. (J.
Appl. Bacteriol., 1995, 78, pp. 264-269).
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Parmi ces composants, le pouvoir antiseptique du terpinиne4-ol apparaоt comme le plus large,
suivi de l'alpha-terpinйol, puis du terpinolиne, de l'alpha-terpinиne, et du cinйole. Le gammaterpinиne et le p-cymиne prйsentent de faibles pouvoirs antiseptiques.
En rйexaminant le tableau prйcйdent relatif а la composition d'huiles essentielles type terp:mиne4ol usuelles (non rectifiйes) et la composition d'une huile essentielle aprиs rectification on peut
remarquer ceci - Parmi ces composйs quantitativement "majeurs", les deux dont les pouvoirs
antiseptiques sont les plus faibles ont йtй fortement rйduits (gamma-terpinene et p-cymиne) dans
l'essence rectifiйe.
- L'antiseptique le plus intйressant (le terpinиne4-ol) atteint les 213 de la composition totale de
Ibuile essentielle rectifiйe.
- L'alpha-terpinйol, antiseptique le plus intйressant aprиs le terpinиne4-ol, devient quantitativement
le deuxiиme composant de l'huile essentielle rectifiйe.
Exemple 5 : Activitй antiseptique de l'huile essentielle rectifiйe
Etude comparative des activitйs bactйricides et fongicides d'huiles essentielles de Melaleuca
alrernlfolia non rectifiйes et rectifiйes selon la mйthode par dilution-neutralisation (note technique
propharmacopoea ne288).
Conditions expйrimentales
Milieux de subculture : Brain heart agar (Marque Difco) -Souches microbiennes Issues de la
Collection Nationale de 'Institut Pasteur Pseudomonas aenrginosa, Eschscherichia coli,
Siaphyloccocus aureus, Enrerococcus faecium. Candida albicans, Propionibaclerium acnes
-Neutralisant : neutralisant-diluant Pharmacopйe franзaise
Tween 80
Lйcithine
Histidine, HCI
Peptone de Casйine
NaCI
Phosphate monopotassique
Phosphate disodique dihydratй
389/1651
Eau distillйe -Temps et tempйratures de contact: 5 et 30 min; 32 +/- 10C -Tempйrature d'incubation
des cultures: 37 C pour toutes les souches sauf Propionibacteflum acnes (30 C en atmosphиre
anaйrobie)
Rйsultats:
La validitй du neutralisant a йtй vйrifiйe pour la concentration de 5 % en produit pour les 6
souches.
Souches Temps de Activitй bactйricide
contact (rйduction de 5 Log)
(minutes) CMB (*)
huiles essentielles
Non rectifiйe Rectifiйe
Pseudomonas aeruginosa 5 > 5,0 % < 0,5 %
30 2,5 %( ) < 0,5 %
Eschscherichia coli 5 0,5 % 1,0 %
30 0,5 % < 0,5%
Staphyloccocus aureus 5 2,5 %( ) 1,0 %
30 2,5 % 0,5 %
Enterococcusfaecium 5 > 5,0 % > 5,0 %
30 > 5,0 % 2,5 %( )
Candida albicans 5 > 5,0 % > 5,0 %
30 2,5 % 2,5 %(0)
Propionibacterium acnes 5 > 5,0 %
30 1,0 %( ) (*): Concentration Minimum Bactйricide (C) : Rйduction proche de 5 Log
L'huile essentielle rectifiйe possиde un pouvoir bactйricide а l'йgard de Pseudomnas aeruginosa,
Staphylococcus aureus, et Enterococcus faecium supйrieur а l'huile essentielle non rectifiйe.
Les effets fongicides а l'йgard de Candida albicans et bactйricides vis а vis d'Escherichia coli des
deux types d'huile essentielle йtant assez proches.
L'huile essentielle rectifiйe de Melaleuca type terpinиne-4-ol peut кtre utilisйe comme ingrйdient
actif, seul ou en association avec d'autres ingrйdients actifs, dans la prйvention ou le traitement de
troubles d'origines microbiennes variйes : plaies, brыlures, infections cutanйes bactйriennes ou
fongiques telles que l'acnй, les dermatoses, les furonculoses, l'onycomycose, le pied d'athlиte7
390/1651
infections du cuir chevelu, infections bucco-dentaires, infections oto-rhinolaryngologiques, infections
urinaires, infections vaginales.
Cette huile essentielle rectifiйe peut aussi кtre utilisйe en tant qu'agent conservateur antibactйrien
et antifongique seul ou associй а d'autres agents conservateurs naturels ou d'origine synthйtique.
L'huile essentielle rectifiйe de Melaleuca peut кtre incorporйe dans toutes les formes galйniques
employйes en cosmйtique ou dermopharmacie а savoir: йmulsions, laits, lotions, gels, pommades,
huiles, lotions capillaires, shampooings, savons, sticks, crayons, sprays. Il en est de mкme pour
toutes les formes galйniques employйes en pharmacie, а savoir : solutйs, йmulsions, sirops,
mйlanges liquides pour inhalations, huiles essentielles pures ou diluйes, gйlules, suppositoires,
patchs.
La concentration de l'huile essentielle rectifiйe dans les formules cosmйtiques, dermatologiques,
pharmaceutiques ou alimentaires est comprise entre 0,01 et 99 % prйfйrentiellement 0,5 а 10 % en
poids de la composition totale. Claims:
REVENDICATIONS
1/Composition cosmйtique ou pharmaceutique, notamment dermatologique, ou alimentaire
caractйrisйe en ce qu'elle contient une huile essentielle rectifiйe de Melaleuca type terpinиne- 4-ol;
la somme des taux de limonиne, d'alpha-pinиne, de beta-pinиne et de 1,8-cinйole dans l'huile
essentielle rectifiйe n'excйdant pas 0,5 % 2/Composition selon la revendication 1 caractйrisйe en
ce que le taux de terpinиne-4-ol contenu dans l'huile essentielle rectifiйe revendiquйe n'est pas
infйrieur а 60,0 % de l'huile essentielle.
3/Composition selon la revendication 1 а 2 caractйrisйe en ce que la somme des taux
d'alphaterpinиne et gamma-terpinиne contenus dans l'huile essentielle rectifiйe revendiquйe
n'excиde pas 5,0 % de l'huile essentielle.
4/Composition selon la revendication 1 а 3 caractйrisйe en ce que l'huile essentielle rectifiйe
revendiquйe contient en particulier de l'alpha-terpinйol, du delta-cadinиne et du terpinolиne.
391/1651
5/Composition selon la revendication 1 а 4 caractйrisйe en ce que le Melaleuca type terpinиne-4-ol
prйcitй est choisi parmi les espиces : Melaleuca alternifolia, Melaleuca linarXifolia, Melaleuca
disitiflora.
6/Composition selon les revendications 1 а 5 caractйrisйe en ce que l'huile essentielle rectifiйe
revendiquйe est obtenue par distillation sous pression trиs rйduite а partir d'une huile essentielle
de Melaleuca type terpinиne 4-ol prйparйe par hydrodistillation ou par distillationа la vapeur d'eau
du feuillage et des branches terminales du Melaleuca.
7/Composition selon les revendications 1 а 6 caractйrisйe en ce que la concentration de l'huile
essentielle rectifiйe revendiquйe est comprise entre 0,01 et 99 % prйfйrentiellement 0,5 а 10 % en
poids de la composition totale.
8/ Composition selon les revendications 1 а 7 caractйrisйe en ce que l'huile essentielle rectifiйe
revendiquйe est utilisйe dans toute forme galйnique employйe en cosmйtique ou
dermopharmacie а savoir: йmulsions, laits, lotions, gels, pommades, huiles, lotions capillaires,
shampooings, savons, sticks, crayons, sprays.
9/Composition selon les revendications 1 а 7 caractйrisйe en ce que l'huile essentielle revendiquйe
est utilisйe dans toute forme galйnique employйe en pharmacie, а savoir: solutйs, йmulsions,
sirops, mйlanges liquides pour inhalations, huiles essentielles pures ou diluйes, gйlules,
suppositoires, patchs.
10/Composition selon les revendications 1 а 9 caractйrisйe en ce que l'huile essentielle rectifiйe
revendiquйe est utilisйe comme ingrйdient actif, seul ou en association avec d'autres ingrйdients
actifs, dans la prйvention ou le traitements de troubles d'origine microbienne plaies, brыlures,
infections cutanйes bactйriennes ou fongiques telles que l'acnй, les dermatoses, les furonculoses,
l'onycomycose, le pied d'athlиte, infections du cuir chevelu, infections bucco-dentaires, infections
oto-rhino-laryngologiques, infections urinaires, infections vaginales.
11/ Composition selon les revendications 1 а 10 caractйrisйe en ce que l'huile essentielle
revendiquйe est utilisйe en tant qu'agent conservateur antibactйrien et antifongique seul ou
associй а d'autres agents conservateurs naturels ou d'origine synthйtique.
392/1651
65. FR2767061 - 12.02.1999
COMPOSITION CONTAINING PROPOLIS AND AT LEAST ON ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2767061
Inventor(s):
MORICE ANDRE PIERRE (--)
Applicant(s):
MORICE ANDRE PIERRE (FR)
IP Class 4 Digits: A61K
IP Class:
A61K47/44
E Class: A61K35/78+M
Application Number:
FR19970010414 (19970811)
Priority Number: FR19970010414 (19970811)
Family: FR2767061
Abstract:
COMPOSITION CONTAINING PROPOLIS AND AT LEAST ONE ESSENTIAL OIL, THEIR USE IN THE
TREATMENT OF VIRAL, BACTERIAL AND FUNGAL INFECTIONS, AND IN MEDICAMENTS FOR
CELL AND TISSUE REGENERATION.Description:
La prйsente invention concerne 1' utilisation cosmйtologique et pharmaceutique d' une association
de produits naturels: Propolis et Huiles Essentielles.
Ces associations sont anti-bactйriennes, anti-mycosiques, anti-virales et rйgйnйratrices.
393/1651
Composition chimique: 1. Propolis:
- 50 % a 55 % de rйsines et de baumes.
- 30% в 40% de cires.
- 5 % а 10 % d' huiles essentielles.
- 5 % de pollen.
- 5 % de matiйres diverses (organiques et minйrales ).
- Avec: a - Les composйs aromatiques
-Acide Berizoique -Benzaldehde
- Alcools Acide cinnamique
C3
z RI
Les
a Xs
i t I:
c- Les Terpenes
d- Autres: Vitamines;Oligo-йlйments; Sucre;Enzymes etc...
2 - Huiles Essentielles testйes seules et associйes par Aromatoaramme:
- Phйnol: Origan d' Espagne, Girofle.
- Esthers: Sauge.
- Alcools: Thym de France, Melaleuca alternifolia, Cypres.
394/1651
- Oxvdes: Lavande de France, Eucalyptus radiata.
- Aldehydes: Eucalyptus citronnй, Verveine odorante.
- Cetones: Romarin officinale, Eucalyptus dives.
- Lactones: Massoia.
- Terpenes: Sapin baumier.
- Autres: Sariette de Provence, Canelle de Ceylan, Canelle de Chine.
3 - Associations:
Teinture-Lotion (Usage externe):
-Propolis 10%
- Thym ( Linalol-Alcool)
- Lavande(Ester)Sauge(Ester) aa 0,1 %
- Alcool q. s. p. 100
Pommade (Usage externe )
- Propolis 10 %
- Thym
- Romarin(Cйtone )Sauge(Ester)Lavande(Ester) aa 4g.
-Vaseline q.s.p.
Autres:
- Propolis + Origan (Phйnol) Carvacrol.
+ Melaleuca (Alcool) Terpineol.
+ Sariette
+ Girofle
+ Sauge
Commercialisation: Suppositoires, Pommades, Teintures, Inhalation, Gйlules et
395/1651
Comprimйs.
Essais Pharmacologique: Thиse de Mr Eric Debuyser.
Universitй de Nantes. (Facultй de Pharmacie)
Annйe 1983-1984.
Thиse de Mlle Mireille Goыt.
Universitй de Rennes Annйe 1985.
Essentiellement bactйriologique - Mycologique.
Thиse de Mme Sauvager sur Propolis seule (Propriйtй anti-Virale).
Essais Cliniques: - Par le Dr Morice sur les Malades.
Essais sur Peau chimique prйvus: sans chorion, sans passage par 1' animal.
Applications: - Pathologie cutanйe.
- Lйsions Associйes d' origine bactйriennes, mycosiques et virales.
- Pathologie des muqueuses.
- Effets rйgйnйrateurs de la peau et des muqueuses. Claims:
Revendications
Revendications gйnйrales:
La Propolis ( produit naturel de la ruche ) composйe de rйsines, baumes, cires, huiles essentielles,
pollen, matiиres diverses organiques et minйrales avec des composйs
396/1651
Aromatiques - Flavonoides - Terpenes, est associйe aprиs nettoyage а froid enlevant les produits
non dйsirйs, а des Huiles Essentielles chimiquement pures essentiellement des " Phйnols - Esthers
- Alcools - Oxydes - Aldehydes - Cйtones - Lactones - Terpиnes et autres Molйcules
Les associations les plus йtudiйes sont:
Propolis + : Origan, Girofle, Sariette, Sauge, Thym, Melaleuca, Cyprиs, Lavande,
Eucalyptus, Verveine, Romarin, Massoia, Sapin Baumй, Cannelle de Ceylan et de Chine.
L' activitй de ces associations
- Antibactйrienne: Staphylocoques - Streptocoques B - Hemolytique
Enterobactйries ( Esch. Coli) Pyocyamique ( Pseudomonas Aeruginosa ).
- Antimycosique: Candida Albicans - Epidermophytes.
- Antivirale: Virus а ADN nu ( Adenovirus) et enveloppй ( Herpes et HSV1)
Papilloma virus.
Virus а ARN nu ( Poliovirus type 2 ) et enveloppйs.
est indiscutable en Mйdecine humaine et vйtйrinaire.
Sous-revendications:
Associations types : exemples.
- Teiture-Lotion (Usage externe):
- Propolis 10%
- Thym (Linalol-Alcool)
Lavande (Ester) Sauge (Ester) aa 0,1%
- Alcool q.s.p 100.
- Pommade (sape externe):
- Propolis 10%
- Thym
- Romarin (Cйtone) Sauge (Ester) Lavande (Ester) aa 4g
- Vaseline q.s.p.
397/1651
- Ovules: - Huiles Essentielles Melaleuca 6 gouttes.
- Propolis pure
- Excipient q.s.p Ovule.
Suppositoires: Huiles Essentielles Eucalyptus globulus 6 gouttes.
- Propolis pure
- Excipient q.s.p Suppositoire.
- Autres : - Propolis + Origan (Phйnol) Carvacrol.
+ Melaleuca (Alcool) Terpineol.
+ Sariette.
+ Girofle
+ Sauge.
- Autre produits en cours d' йlaboration qui se prйsenteront sous forme de Teinture - Lotion
Pommade - Gйlule - Ovule - Suppositoire.
398/1651
66. FR2787347 - 23.06.2000
PREPARATION OF ESSENTIAL OIL EMULSION USEFUL IN COSMETIC, DERMATOLOGICAL OR
FOOD COMPOSITIONS, FROM PLANT MATERIAL, COMPRISES COOLING AND STIRRING VAPOR
OBTAINED BY MICROWAVE IRRADIATION UNDER REDUCED PRESSURE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2787347
Inventor(s):
LAFORET JEAN PIERRE (--)
Applicant(s):
GATTEFOSSE ETS SA (FR)
IP Class 4 Digits: A61K; A23L; B01D; B01F; B01J
IP Class:
A61K35/78; A61K7/00; B01D3/38; A61K9/107; B01F3/08; B01J19/12; A23L1/29
E Class: A61K8/92C; A61Q19/00; A23L1/22C; A23L1/221; A61K8/06; A61K8/55C; A61K8/60;
A61K8/97; A61K47/26; B01J19/12D6; H05B6/80
Application Number:
FR19980016162 (19981217)
Priority Number: FR19980016162 (19981217)
Family: FR2787347
Abstract:
PREPARATION OF AN EMULSION BASED ON AROMATIC VEGETABLE MATERIAL INVOLVES
PLACING THE VEGETABLE MATERIAL IN A HEATED CHAMBER IN THE ABSENCE OF SOLVENTS,
IRRADIATING WITH MICROWAVES WHILE APPLYING REDUCED PRESSURE, COOLING THE
VAPOR CONTAINING THE ESSENTIAL OILS TO GIVE A 2-PHASE SOLUTION AND STIRRING TO
FORM AN EMULSION. PREPARATION OF AN EMULSION BASED ON AROMATIC VEGETABLE
MATERIAL COMPRISES: (A) PLACING THE VEGETABLE MATERIAL IN A HEATED CHAMBER IN
THE ABSENCE OF SOLVENTS; (B) IRRADIATING WITH MICROWAVES WHILE APPLYING
REDUCED PRESSURE, SUCH THAT THE CELLULAR STRUCTURES ARE BROKEN UP AND THE
AROMATIC OILS ARE DISTILLED OFF BY WATER VAPOR FROM THE VEGETABLE MATERIAL; (C)
399/1651
COOLING THE VAPOR CONTAINING THE ESSENTIAL OILS TO GIVE A 2-PHASE SOLUTION; AND
(D) STIRRING TO FORM AN EMULSION. AN INDEPENDENT CLAIM IS ALSO INCLUDED FOR THE
EMULSION OBTAINED BY ABOVE METHOD.
400/1651
67. FR2822678 - 16.10.2002
SAFE, ECO-FRIENDLY HEALTH PROTECTIVE HERBAL COLOURS AND AROMA USEFUL FOR
COSMACEUTICAL APPLICATIONS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2822678
Inventor(s):
GOVINDARAJAN RAGHAVAN (IN); KHATOON SAYYADA (IN); MEHROTRA
SHANTA (IN); PUSHPANGADAN PALPU (IN); RAWAT AJAY KUMAR SINGH (IN)
Applicant(s):
COUNCIL SCIENT IND RES (IN)
IP Class 4 Digits: A61K
IP Class:
A61K7/027
Application Number:
GB20010008033 (20010330)
Priority Number: GB20010008033 (20010330); FR20010004411 (20010330); JP20010096849
(20010329)
Family: FR2822678
Equivalent:
JP2002308724
Abstract:
A NOVEL SAFE AND ECO-FRIENDLY HEALTH PROTECTIVE AND BEAUTY ENHANCING HERBAL
COMPOSITION HAVING VARIOUS COSMETIC APPLICATIONS SUCH AS LIPSTICKS, EYE
SHADOWS, GLOW-GLITTERS AND ROUGES, SAID COMPOSITION CONTAINING COLOURANTS
FROM PLANTS, FOR EXAMPLE, OF THE FAMILY BORAGINACEAE, THE INVENTION ALSO
PROVIDES A METHOD FOR PREPARING THE SAID COMPOSITION. THE INVENTION ALSO
RELATES THE USE OF LIPSTICKS AS A MEDIUM OF AROMATHERAPY.Description:
401/1651
SAFE, ECO-FRIENDLY, HEALTH PROTECTIVE HERBAL COLOURS
AND AROMA USEFUL FOR COSMACEUTICAL APPLICATIONS FIELD OF THE INVENTION
The present invention relates to a safe, eco-friendly, health protective and cosmetic composition
useful as lipstick and for other cosmaceutical applications like eye-shadows, skin creams, glowglitters and rouges.
BACKGROUND AND PRIOR ART
There is worldwide revival of interest in the use of natural colours especially in cosmetics and
pharmaceuticals as the synthetic colours are likely to cause many side effects. Keeping this in view
the present invention is undertaken to develop purely natural herbal colorants for cosmetic
compositions. One aspect of the invention pertains to the development of a herbal composition
useful as Lipstick with moodaltering functional attributes including stimulation of creative thoughts on
persons who apply the same on lips. Such features of the composition are attributed to the selected
blended formulations of Natural colours and essential oils/aroma isolates incorporated.
Lips being-the-most-sensitive part-of skin ;-can effect fast transdermal absorption and also the lips
being very close to nose facilitate a continuous inhalation of the slowly vaporizing essential
oils/aroma chemicals blended in the composition, thus, providing a double effect on the specific
centers of the brain by releasing neurochemicals leading to mood alteration stimulation and change
of mental perceptions. The different blends of essential oil/aroma isolates/natural aroma chemical
selectively blended in the lipsticks provide anti-depressant, mood enhancing/mood lifting effect and
give rise to creative thoughts.
While lipsticks with different colour shades blended with aromatic principles have been developed
for women, another range of compositions useful as lipsticks has also been developed for men.
These compositions are without colours but provide a moisturizing transparent effect and have mood
altering functions and are designed to altered mental perception, functioning similar to the lipstick
compositions developed for developed for women. Both the groups of lipstick have some additional
health promotive/protective and beautifying attributes by preventing the lips from darkening and
providing it with moisturizing effects. These compositions also give attractive luster and texture to the
lips. The lipsticks with colour, developed for women, have antibacterial, antifungal and antiinflammatory effects. With regard to lip beatification topical application
402/1651
lipstick with different shades of colours are well known. Likewise, spraying of aromatic oils or sprays
for refreshing is also well known. Many studies have been carried out on the effect of fragrance on
mental perception ; for example, the nice fragrance has an aesthetic impression and multiple positive
effects on our life, they are not only for pleasure and seduction, healing and magic products but also
for positive mood creators.
DESCRIPTION OF PRIOR ART
Reference is made to a publication titled''Naphthaquinones of Arnebia Nobilis"by Y. N.
Shukla et al., Phytochemistry, 1971, Vol. 10, pp. 1909 to 1915, wherein, 4-naphthaquinones
designated as A-1, A-2, A-3 and A-4 have been reported. The use of the extract from Arnebia nobilis
is also reported. - Sayyada Khatoon and Shanta Mehrotra in"Naphtha quinones from some
Boraginaceous Texa-A Chemical Review" published in Natural Product Sciences, 1996 2 (2)-pp. 7585 report a number of naphthaquinones from boraginaceous plants. Varies properties of thesecompounds have also been reported.
V. P. Papageorgiou, has reported certain lipophilic red pigments obtained from various plants
including the genus Lithospermum, Echium Onosma Anchusa and Cynoglossum, in his publication
titled : Naturally occurring Isohexenylnaphthazarin Pigments : A New Class of Drugs"in Planta Medica,
1980, Vol. 38, No. 3.
US Patent 4996044 describes a lipstick formulation consisting of organic high staining dyes, said
formulation having creamy, shiny and soft laydown and long wear properties. The formulation does
not use any extracts from any plant.
Reference is made to a US patent (No. 5593662) wherein moisturizing lipstick has been described.
In this invention, use has been made with a composition of 30-80% lipophilic material,
which may have lesser shelf life and may promote microbial growth due to the presence of moisture.
They used about 0-35% synthetic colourant which seems to be too high for a cosmetic composition.
The synthetic colours mostly exhibit harmful side effects like loss of luster, blackening of skin and
may have some carcinogenic effects too as shown in a website (http://www. orst.
eduffoodresource/color/colorantsl. html).
403/1651
Another reference is made to patent no. 5665778 wherein a ceramide, process for their preparation
and their application in cosmetics and in dermato-pharmacy. These compounds are complex
mixtures of erythro & threo-diasterioisomers. They synthesize these compounds by a
complex and costly process. They have used organic pigments for lipstick and there is no herbal
colourants being used.
Reference may be made to a recent PCT application PCT/EPOO/02217 of 13 March 2000 wherein
the inventors have used Zinc salts, particularly Zinc citrate in lipstick to effect antimicrobial property.
The drawback in using Zinc or its salts is that mostly they are emetic and cause conjunctivitis as side
effect.
In an International Congress of Essential oils, fragrance and flavours (November 1989) the
description of use of aroma has not at all been mentioned in lipstick. The available lipsticks in the
international market are used as refreshing beautifying agents only.
US Patent 5665778 describes yet another cosmetic formulation consisting of ceramides and other
compounds. The composition of this patent is a totally synthetic composition.
US Patent 5676957 describes a skin external agent, said agent being an extract of the plant of
genes Euonymus such as Euonymus alata. This extract according to this invention may be
formulated with a costnetically acceptable b. ase. ~ ~ ~ Reference is made to a US patent No. 5, 85,
8348 wherein only a single isolate of essential oil like rose-oxide-has-been used in synthetic lipstick
and other cosmetic for refreshing feel. Such a single isolates of essential oil will not serve-the-desired-multiple-effeFcts-Eke mood enhancing, sensual pleasure and thought inducing state of mind.
To the knowledge of the applicants, there does not exist any lipstick with herbal colours and
functional attributes, the cosmaceuticals like eye shadows and glow glitters, rouges with use of
herbal colours, likewise the lipstick without colour with functional attributes for men.
OBJECTS OF THE INVENTION
404/1651
The main objective of the present invention is to provide safe, eco-friendly, health protective and
cosmetic composition containing natural colours and aroma/essential oils useful for various
cosmaceutical applications.
Another objective of the present invention is to use the herbal colours in lipsticks.
Another objective of the present invention is to provide transparent cosmetic compositions useful as
lipsticks and containing essential oils/aroma isolates.
Still another objective of the present invention is to use the herbal colours in other cosmetic
compositions like eye shadows, skin creams, glow glitters and rouges.
Yet, another objective of the present invention is to provide the use of the functional lipstick as a
means to camouflage leucodermic skin and particularly lips.
Yet another object of the invention is to provide a method for the production of cosmetic
compositions containing herbal colourants and useful in other cosmetic applications.
SUMMARY OF THE INVENTION
The invention provides a safe, eco-friendly, health protective and beautifying herbal composition
containing colourants and aroma, and useful for various cosmaceutical applications. The invention
also provides a process for the preparation of the herbal cosmetic composition comprising extraction
of colourants from natural sources such as plants, and mixing the colourants with aroma and other
base material for cosmaceutical applications.
DETAILED DESCRIPTION OF THE INVENTION
This invention relates to an herbal cosmetic composition containing colouring agents for - ---------- - - -- - - topical or external use. More particularly, the invention provides a novel cosmetic composition,
useful especially as lipstick. When used as lipstick, the composition contains herbal colourants for
405/1651
which is then blended-with-selected-blends of essential oils-or aroma isolates and the composition is
capable of altering the mood and mental perception of the person, who applies it.
A safe ecg. mendly, health protective and beautifying herbal cosmetic composition containing
herbal colourants together with a cosmetically acceptable amount of one or more additives providing
special properties and a cosmetically acceptable base material.
Accordingly the present invention provides a composition comprising additives providing special
properties are selected from essential oils/aroma isolates obtained from the group of plant species
belonging to genera Acquillaria, Cinnamomum, Cymbopogon Elettaria, Eucalyptus, Geranium,
Jasminum, Ocimum, Pelargonium, Rosa, Rosmarinus, Santalum and Vetiveria.
In one embodiment of the invention, the essential oils/aroma isolates act as mood lifting agents,
antidepressant agents, anti stress agents, sensual pleasure providing agents, creative thought
inducing agents, anxiety reducing agent, refreshing agent, stimulant, soothing agents, anti oxidants,
fixative, fragrants, and antimicrobial.
The applicants have found that the herbal colourants are obtained from various plants of the family
Boragznaceae. It is the finding of the applicants that a wide spectrum of colors can be obtained from
the said plants by using specific solvents in specific proportions. For instance, petroleum ether and
chloroform may successfully be used m different proportions for extraction of
the colored matter from the said plants in order to achieve a wide spectrum of colors such as pastel
red, purplish red, cerise, ruby red, deep magenta, beet root purple, amarynth, dark purple, dark
violet, deep violet, deep blue blackish blue, etc. It is pertinent to note that each of the plants listed
above are capable of yielding the above spectrum of colors.
The applicants have found that the herbal colorants obtained from various plants together with the
essential oil and conventional additives yield a herbal composition which is suitable for cosmetic
applications such as lipsticks.. This herbal composition is devoid of toxic effects. The applicants also
believe that the essential oils and aroma isolates may have the properties of mood enhancement,
sensual pleasure, antidepressant and creative thought inducer. Also, the essential oils and aroma
isolates may be used in transparent lipstick as a functional attribute.
406/1651
The proportion in which the coloring matter/coloring compounds can be mixed with essential oils
and additives can be readily determined by a person skilled in the art. However, it is preferred that
0.0005% of coloring matter may be-mixed with l04 % essential oil, 1% lustering agent such as
safEloweroilT'The base and other matters'added may make up 100%.
Herbal lipophilic, safe colours are extracted from the plants belonging to the genus
Arnebia, Bixa, Butea, Carthamus, Hibiscus, Jatropha, Lithospermum, Macrotomia, Maharanga, - -- --- -""'--- - -- ---Nyctanthes, Onosma, Rhododendron, and Tagetes which are known to be non toxic
and free from any strong side effects on human body particularly on topical application. The colours
extracted from these plants are bright and lustrous and have pronounced antibacterial and antiinflammatory activities. For example a good bright colourant-red-andora colour, plate No. 8.4 L of
Dictionary of colours (Maerz and Paul, 1950) and after applying on lips, pomegranate to Vemonia
purple (plate 6.3 L-6. 5 A of the same dictionary provides different functional effects such as mood
refreshing, concentration enhancing, CNS relaxant, accelerating working rate and improves capacity
to work. It is pertinent to note that each of the plants listed herein is capable of yielding a wide
spectrum of colours.
Accordingly, the present invention provides safe, eco-friendly, health protective herbal colours and
aroma useful for cosmaceutical applications which comprises safe, eco-friendly, health protective
and beautifying herbal colourants and aroma useful for cosmaceutical applications, comprising
extraction of organic compounds from natural sources such as plants, the said extracted organic
compounds being used as a colourant with aroma in base material for cosmaceutical applications.
An embodiment of present invention is that the safe herbal colourants may be isolated from different
plant species belonging to the genera of family Boraginaceae which are non-toxic and may be free
from any side effects.
407/1651
Another embodiment of present invention is that the aroma isolates/essential oils may be selected
from group of plants - Aquillaria, Cinnamomum, Cymbopogon, Elettaria, Eucalyptus, Geranium,
Pelargonium, Rosa, Rosamarinus, Santalum and Vetiveria.
In other embodiment, the herbal colourants may be used in lipsticks, eye shadows, glow glitters and
rouges.
In still other embodiment the lipstick containing essential oils and combinations of aroma isolates
may release neurochemicals in the brain through the receptors in mouth and nose and may have the
properties of mood enhancement, sensual pleasure, antidepressant and creative thought inducer.
; In yet another embodiment of the invention, the anti-depressant property imparted by the essential
oils are selected from
Essential Oils Preferred Ratio
1. Ocimum oiL'Jasminum oil : Cymbopogon oil (1 : 2 : 1)
2. Ocimum oil : Mentha oil: Rosmarinus oil (2 : 1 : 1)
3. Jasminum oil : Mentha oil : Rosmarinus oil (1 1
4. Cymbopogon oil: Ocimum oil: Mentha oil (1 : 2 : 1)
5. Ocimum oil: Cymbopogon oil (2 : 1)
6. Mentha oil : Rosmarinus oil
7 Ocimum oil
8. Rosmarinus oil
In yet another embodiment of the invention, the creative thought-inducing property is, imparted by
the essential oils selected from
Essential oil Preferred ratio
1. Santaium oil
408/1651
2. Santalum oil: Rosa oil (1 : 2)
In yet another embodiment of the invention, the anti-stress property is imparted by the essential oils
selected from
Essential oil Preferred ratio
1. Santalum oil: Lavandula oil (2 : 1)
2.Lavandula oil: Eucalyptus oil: Rosa oil (1 : 1 : 1)
3. Eucalyptus oil: Rosa oil (1 : 2)
4. Aquillaria oil: Elettaria oil: Rosmarinus oil (1 : 1 : 1)
5. Jasminum oil
6 Santalum oil
7. Lavandula oil
In yet another embodiment of the invention, the refreshing property is imparted by the essential oils
selected from
Essential oil Preferred ratio
1. Santalum oil : Rosa oil : Rosmarinus oil (1 : 1 : 1)
2. Santalum oil : Pelargonium oil (1: 2)
3 Jasminum oil: Lavandula oil (1 : 2)
5 Lavandula oil
6 Santalum oil : Oa oi/
6 Santulam oil
In yet another embodiment of the invention, the sensual feeling property is imparted by the essential
oils selected from
409/1651
Essential oil Preferred ratio
1. Jasminum oil : Lavandula oil : Pelorgonium oil (1: 2)
2. Ocimum oil: Jasminum oil : Cymbopogon oil (1 : 2: 1)
3. Jasminum oil
4. Jasminum oil: Lavandula oil (2: 1)
In yet another embodiment of the invention, the mood lifting property is imparted by the essential oils
selected from
Essential oil Preferred ratio
1. Jasminum oil : Rosa oil : Palergonium oil (1: 2)
2. Rosmarinus oil (1 : 2)
3. Cymbopogan oil: Rosa oil (2: 1)
4. Rosa oil
5. Jasminum oil : Rosa oil
In yet another embodiment of the invention, the anxiety reducing property is imparted by the
essential oils selected from
Essential oil Preferred ratio
1 Rosa oil: Cinnamomum oil (1: 2)
410/1651
Still another embodiment of the invention is that the essential oils and aroma isolates are used in
transparent lipstick as a functional attribute.
Still another embodiment of the invention relates to the composition wherein, tocopherol is used as
an antioxidant, which also functions as fixative, and may be present in traces to ppm.
An embodiment is that the process for extraction of organic compounds from natural sources such
as plants which comprises drying of plant parts, powdering by known means, the said dried powder
being used to extract herbal colourants, optionally treating the said colours with acids or bases taken
in different proportions, to produce various shades.
Yet another embodiment, the plant parts may be root, stem, leaf, and the quantum of essential oils
used in preparing compositions vanes based on the part from which the oil is
- ------ - extracted.
Still another embodiment of the present invention is that the plant parts may be dried at a
temperature in the range of 3045 C, n sha-de ~ ~ An another embodiment the dried plant parts may
be powdered to particles of the size in the range of 30-60 mesh.
Further embodiment, the herbal red colourants may be extracted from the plants of the genera
Arnebia, Bixa, Butea, Carthamus, Hibiscza, Jatropha, Lithosper ? num, Macrotomia, Maharanga,
Nyctanthes, Onosma, Rhododendron, and Tagetes. The plants or their parts are put in a Soxhlet
apparatus at a temperature of 20-800C. The solvents selected for the extraction may be nonpolarhexane, petroleum ether, toluene and cyclohexane, wherein the polar solvents are selected from
chloroform, acetone, ethyl alcohol and methyl alcohol. The non-polar and polar solvents may be
recovered at reduced pressure of 50-100 psi and a temperature of 40-800C. The herbal colourants
are obtained after the recovery of the solvents. The concentrates result colours of various shades
such as purplish red, cerise, ruby red, beetroot purple, dark violet, deep blue, and blackish blue
colours which are herbal in nature as no trace of organic solvent remains in the final concentrate.
Further, the present invention provides a process for preparation of herbal colourants, which
comprises the steps of drying the plant material, powdering the same and percolating it with ethyl or
methyl alcohol at a temperature of 20-480C. The alcohol soluble matter is concentrated at reduced
411/1651
pressure of 50-100 psi and a low temperature of 40-60oC. The concentrate is eluted with silica gel
column chromatography using non-polar solvents like-petroleum ether, hexane, cyclohexane, toluene
and a mixture of non-polar and polar solvents. The polar solvents used may be like chloroform,
acetone, ethylacetate and methanol. The ratio of the non-polar and polar solvents may be 20: 1 to 4:
1. The concentration of the column fractions may be made at a range of reduced pressure of 80-100
psi and a temperature of 30-60oC. The colours of the concentrate may be pastel red, pale red,
purplish red, rose red, cerise, ruby red, deep magenta, beetroot purple, amaranth, dark purple, dark
violet, deep violet, deep blue and blackish blue
In still another embodiment the herbal colourants may be antimicrobial, anti-inflammatory and may
be used in leucoderma, more particularly of lips.
The embodiment of the present invention the herbal colourants may be the mixture of naphthazarins
and may be cyclic unsaturated diketones in which double bonds and keto group may be conjugated.
The another embodiment of present invention the herbal colourants may be changed in different
shades with organic and inorganic acids. The intensity of colours may be increased with
"orgaaic acids-and may be decreased with morganiccidsrTne'anger of the concentration of the
acids may be 0.1-10%.
Still another embodiment of the invention that the herbal colours may be changed with organic and
inorganic bases.
Another embodiment of the present invention the base concentration may be in the range of 0.1 to
20%.
Yet another embodiment the herbal colour may be lipophilic and hydrophilic properties may be very
minimllII1.
Still another embodiment the herbal colours may be soluble in organic solvents likehexane,
petroleum ether, benzene, diethyl ether, ethylacetate, chloroform, acetone and alcohol in the range
of 30-100%.
412/1651
In an embodiment, the pH of the extracted herbal colours may be 5-6.
The present invention is aimed to prepare safe, eco-friendly, health protective herbal colours and
aroma useful for cosmaceutical applications which comprises extraction of organic compounds
from natural sources, the said extracted organic compounds being used as a colourant with aroma
in base material for cosmaceutical applications.
The safe herbal colourants may be isolated from different plant species belonging to the genera of
the family Boraginaceae which are non-toxic and may be free from any side effects.
The present invention is that the aroma isolates/essential oils may be selected from group of plantsAquillaria, Cinnamomum, Cymbopogon, Elettaria, Eucalyptus, Geranium, Pelargonium, Rosa,
Rosamarznus, Santalum and Vetiveria. The herbal colourants may be used in lipsticks, eye shadows,
glow glitters and rouges.
The lipstick containing essential oils and combinations of aroma isolates may release
neurochemicals in the brain through the receptors in mouth and nose and may have the properties of
mood enhancement, sensual pleasure, antidepressant and creative thought inducer.
The invention is that the essential oils and aroma isolates may be used in transparent lipstick - -------- - as a functional attribute.
Another aspect of the invention relates to a process for extraction of organic colourants from the
plants, said process comprising obtaining the plant parts, extracting with organic solvents, removing
the solvents by conventional methods, concentrating the extract under reduced pressure and
optionally treating with acids or bases to produce various shades.
Yet another aspect of the invention relates to a process for the extraction of organic colourants, said
process comprising the steps of : a) drying the plant parts, b) powdering the dried plant parts, c)
subjecting the dry powder obtained in step (b) to Soxhlet extraction at a temperature in the range of
40-80 C or cold percolation with organic solvents at a temperature ranging between 20 to 45 C, d)
concentrating the mixture of step (c) by conventional methods at reduced pressure in the range of
413/1651
50-100 psi and at a temperature not exceeding 50 C, e) mixing the concentrate of step (d) with silica
gel in the ratio 1: 3 to 2: 7 to obtain a slurry, f) eluting the slurry with organic solvents resulting in
various fractions, g) concentrating the fractions at a pressure in the range of 50-100 psi resulting in
herbal colourants, optionally treating the said colours with acids or bases to produce various shades,
and
h) obtaining various colours from by treating the said fractions with acids or bases to produce
colourants of various shades.
One more aspect of the invention relates yet another process of extraction of herbal colourants from
plants of the family Boraginaceae, which comprises; percolating powdered plant parts with alcohol at
room temperature resulting in alcohol soluble herbal material, the said herbal material being
concentrated by known means at pressures in the range of 50-100 psi and at a temperature in the
range of40-60 C, the said concentrate being made into a slurry with silica gel in a ratio in the range of
1: 3 to 2: 7, the said slurry being eluted by known means with organic solvents resulting in fractions,
the said : fractions further being concentrated by known methods at a pressure in the range of 50100 PSI resulting in herbal colorants, optionally treating the said colours with acids or bases to
produce various shades.
The herbal colours may be extracted from any of the three parts of the plants; namely root, stem or
leaves or by taking all of them. These parts may then dried by any conventional means
- ----- - --- - which may include heat treatment at a temperature between 30-45 C. Alternatively the
drying process may be effected in shade though the time for drying may be rather too long. The
dried plant material may-then-be-powdered and sieved-through mesh-to-get-a powder of particles of
a suitable size preferably in the range of 30-60 mesh
The-dried powder may then be extracted by using Soxhlet apparatus at a temperature range of 4080oC.
The dried powdered plant material may also be extracted by cold percolation at a temperature
range of 20-45oC.
414/1651
The extraction may be carried out with the non-polar and mixtures of non-polar and polar solvents
selected for the extraction. Non-polar solvents may be selected from hexane, petroleum ether,
toluene and cyclohexane whereas the polar solvents may be selected from chloroform, acetone,
ethyl alcohol and methyl alcohol. The herbal colours may be obtained by concentrating the extracts
at reduced pressure of 50-100 psi and a temperature at range of 40-60 C. This process of
concentration may result in purplish red, cerise, ruby red, beet root purple, dark violet, deep blue,
and blackish blue colours which are herbal in nature as no trace of organic solvent remains in the
final concentrate.
In another process, the dried, powdered plant material may be percolated with ethyl or methyl
alcohol at a temperature of 20-48oC. The alcohol soluble matter may be concentrated at
reduced pressure of 50-100 psi and a low temperature of 40-60oC. Thus, the said concentrate may
be eluted with silica gel column chromatography by using non-polar solvents like-petroleum ether,
hexane, cyclohexane, toluene and mixture of said non-polar and polar solvents. The polar solvents
may be used like-chloroform, acetone, ethylacetate & methanol. The ratio of the non-polar and polar
solvents may be 20: 1 to 4: 1. The concentration of the column fractions may be made at a range of
reduced pressure of 80-100 psi and a temperature of 30-60 C. The colours of the concentrate may
be pastel red, pale red, purplish red, rose red, cerise, ruby red, deep magenta, beet root purple,
amaranth, dark purple, dark violet, deep violet, deep blue and blackish blue
These novel colours may be used with or without the aroma isolate/essential oils. Proper mixture of
aroma isolates/essential oils may result in such desirable properties of mood enhancement, sensual
pleasure, antidepressant and-creative thoughts inducer To get these desired properties in cosmetics
like lipsticks the herbal colours may be mixed with selected mixture of aroma and applied to the base
material. These herbal colours may be used in other applications like eye shadow, glow-glitters,
rouges and-skin-conditioning agent.
These colours may be the mixture of naphthazarins and may be cyclic unsaturated diketones in
which double bonds, and keto group may be conjugated. These herbal colours may be changed to
different shades by treating it with organic and inorganic acids. The intensity of these colours may be
increased with organic acids and may be decreased with inorganic acids. The range of the
concentration of the acids may be 0.1-10%. The colour of the herbal colourants may be changed
415/1651
from red to blue with organic and inorganic bases. The range of the concentration of the bases may
be 0.1-20%.
These herbal colours may have excellent lipophilic properties and very minimum hydrophilic
properties. These colours may be soluble in organic solvents like-hexane, petroleum ether, benzene,
diethyl ether, ethylacetate, chloroform, acetone and alcohol in the range of 30- 100%. The pH of the
extracted colours may be within the range of 5-6. All these characteristics of the herbal colours are
very desirable for use in cosmaceutical applications. The process of the present invention can obtain
various colours such as described in the tables 3 to 6.
Some of the critical parameters, which are responsible for the generation of various colourants, are
as under: a) composition of the solvent used for runmng the column chromatography.
b) the ratio of the polar to non-polar solvent is also a critical parameter for the production of the
different colours. c) the temperature of the Rotavapours used in the process of the concentration of
the extract is also a critical parameter. d) the temperature of the hot air oven at which the lipstick
formulation is made is also a critical parameter. e) treating the said colours with specific
concentration of acids or bases to produce various shades.
Novel features of the invention: 1. Extraction of the herbal colours from plant materials which are nontoxic and highly lipophilic.
2. A novelty of the present invention lies in application of herbal colours in cosmaceutical
preparationshkeJJLpsticks, eye shadows-glow glitters and rouges.
3. Ability to tailor the shade of the basic herbal colours by a simple treatment of the produce with
organic or inorganic acids or bases.
Brief description of the drawings.
Thus, the process of the invention can be used to achieve different colourants. Some of the
colourants obtained are shown in the accompanying drawings. In the accompanying drawings: Fig 1
represents colourant of red-purple group (60C) Fig 2 represents colourant of red-purple group (61A)
416/1651
Fig 3 represents colourant of red-purple group (58A) Fig 4 represents colourant of red-purple group
(46A) Fig 5 represents colourant of red-purple group (53A) Fig 6 represents colourant of blue group
(103A) Fig 7 represents colourant of blue group (99A)
Fig 8 represents colourant of orange group (25B) Fig 9 represents colourant of orange red group (31
C) Fig 10 represents colourant of orange red group (34C)
Fig 11 represents colourant of orange red group (32C) Fig 12 represents colourant of orange red
group (33B) Fig 13 represents colourant of red group (46A) Fig 14 represents colourant of red group
(44A) Fig 15 represents colourant of red group (46B) Fig 16 represents colourant of red group (59A)
Fig 17 represents colourant of blue group (103B) Fig 18 represents colourant of blue group (103A)
Fig 19 represents colourant of blue-green group (1 14A) Fig 20 represents colourant of greyedpurple group (187B) Fig 21 represents colourant of greyed-purple'grdup (187A) Fig 22 represents
colourant of purple group (79A) Fig23represents colourantTof brown-group- (200A) Fig 24 depicts a
few of various shades of lipsticks obtained according to the invention.
Brief description of the tables.
Table 1 depicts preferred list of Aroma i. e. essential oils for the functional attributes in cosmaceutical
application Table 2 represents preferred list of Aroma isolates for the functional attributes in
cosmaceutical application Table 3 represents change of colours obtained from direct extraction
(process 1)-Change of colours with bases Table 4 represents change of colours obtained from direct
extraction (process 1)-Change of colours with acids Table 5 represents change of colours obtained
from column (process 2)-Change of colour with acids Table 6 represents change of colours obtained
from column (process 2)-Change of colour with bases.
Table 7: Table for correspondence of colour codes based on Flower Council of Holland.
The various colours shown are codified according to RHS colour chart in associatiation with Flower
417/1651
Council of Holland and The Royal Horticultural Society, London.
The following examples are given to illustrate the invention and should not be construed to limit the
scope of the present invention.
PREPARATION OF HERBAL COLOURANTS AND LIPSTICK:
The present invention is illustrated further by referring to the following examples.
However, the present invention is not limited to these examples.
Process Extracted the powdered material with non-polar solvents (like hexane, petroleum ether,
toluene and cyclohexane) and mixtures of non-polar and polar solvents (The polar solvents are
chloroform Acetone, Ethylacetate, methanol, ethanol).
The ranges of ratio of non-polar and polar solvents are 99: 1 to 0: 100.
The change of color by treating the color with traces of food grade acids e. g. Acetic acids less than
0.1% The change of color with the treatment of traces of bases i. e. less than 0. 1%.
Example - 1
100 gm air-dried coarsely powdered root of Onosma species is sieved in 40 mesh sieve and then
extracted in Soxhlet apparatus with hexane at a temperature of 500C for 12-18 hours which resulted
in the formation of hexane soluble herbal matter. The said matter was concentrated at a reduced
pressure of 70 psi and at a temperature of 3SoC, resulting in the yield of 6.0 gm. as the purplish red
colour (Plate NO 12 A7 of Methuen handbook of colour, 1978).
Example-2
100 gm air dried coarsely powdered stem and root in the ratio of 1: 4 of Onosma species is sieved in
40 mesh sieve and then extracted in Soxhlet apparatus, with chloroform, at a temperature of 60 C for
18-24 hours which resulted in the formation of chloroform soluble herbal matter. The said matter was
concentrated at a reduced pressure of 80 psi and at the temperature of 40 C, resulting in the yield of
8. 5 gm. as the beet-root purple (Plate No: 13 D8)
418/1651
Example-3
100 gm air dried coarsely powder stem, root and leaf in the ratio of 1: 1: 3 of Macrotomia species is
percolated at room temperature with the mixture of chloroform and hexane in the ratio of 5: 95 for 4
hours (3 times). Combined all the extracts and concentrated at a pressure of 70psi and a
temperature of 50oC. Thus 3.5 gm of cerise colourant (Plate No: 12 C8) was obtained.
Example-4
100 gm air-dried coarsely powdered root of Onosma species is sieved in 40 mesh sieve and then
extracted in Soxhlet apparatus with hexane at a temperature of 50 C for 12-18 hours which resulted
in the formation of hexane soluble herbal matter. The said matter was concentrated at a reduced
pressure of 70 psi and at a temperature of 35 C, resulting in the yield of 6.0 gm. as the purplish red
colour (Plate NO 12 A7) which gets changed to rose red after treatment with 1% formic acid
Example-5
100 gm air dried coarsely powdered stem and root in the ratio of 1: 4 of Onosma species is sieved in
40 mesh sieve and then extracted in Soxhlet apparatus, with chloroform, at a temperature of 60 C for
18-24 hours which resulted in the-formation of chloroform-soluble herbal matter. The said matter was
concentrated at a reduced pressure of 80 psi and at the temperature of 40oC, resulting in the yield of
8.5 gm. as the beet-root purple (Plate No: 13 D8) which gets changed with 0. 1% HC1 to ruby red
colour (Plate No: 12 D8).
Example-6
100 gm air dried coarsely powder stem, root and leaf in the ratio of 1: 1: 3 of Macrotomia species is
percolated at room temperature with the mixture of chloroform and hexane in the ratio of 5: 95 for 4
hours (3 times). Combined all the extracts and concentrated at a pressure of 70 psi and a
temperature of 50 C. Thus 3.5 gm of cerise colour (Plate No: 12 C8) was obtained which gets
changed to vivid blue (Plate No: 21 A8) with the addition of the 0. 1% NaO
Example-7
100 gm air dried coarsely powdered root of Onosma species is percolated with ethyl alcohol at room
temperature for 24 hours (4 times). The alcohol soluble portion of stem and root was concentrated at
reduced pressure of 70 psi and at a temperature of 50 C, resulting in the formation of 18 gm. of
ethanol soluble concentrate. The said concentrate was mixed with 54 gm of silica gel for preparing
slurry. This slurry was dried with the help of vacuum pump. The column
419/1651
chromatography of this dried slurry was carried out by using hexane: chloroform in the ratio of 95: 5.
The fractions obtained with aforesaid solvents were concentrated at the reduced pressure of 90 psi
and at a temperature of 40oC, thereby giving the yield of 0.3 gm as the pastel red colour (Plate No: 9
A5) which gets changed to vivid blue (Plate No: 21 A8) with the addition of the 0. 1% NaOH.
Preparation of cosmetic compositions
The herbal colourant obtained by the process described in Examples 1 to 7 can be used according
to the invention to develop various cosmetic compositions useful as lip stick, eye-liners, eye-shadows,
glow-glitters and rouges. Such compositions are prepared following the general principles used in
making cosmetic compositions. Specifically, the herbal colourant obtained from the plant parts is
mixed with a base in appropriate proportion. The base may be liquefied first and the colourant of
choice may be added and stirred. Alternatively, the colourant and the base are added, the mixture is
heated, and the ingredients are stirred to obtain a homogenous mixture. To this mixture, essential oil
is added together with softening agents, mood lifting agents and other
- ---- - ----- - - --additives as may be necessary for the compositions. For instance, if glow-glitters
composition is to be prepared, with the basic composition, additives that provide glitter are added.
The composition prepared when cooledto, room temperaturcbecomes suitable for use as a cosmetic
composition.
! While the above is only an outline describing the preparation of cosmetic composition, specific
instances of preparing different cosmetic compositions for various applications is described in
Examples 10 to 17 here below. The specific instances provided herein below are meant only to
illustrate the invention and the same should not be construed to limit the scope of the invention in any
manner.
Example-8
0.5 mg of herbal colour was mixed with I ml of Safflower oil and I ml Castor oil thoroughly. In the said
mixture 1. 5 gm of melted bees wax was mixed at a temperature of 70 C. After that 5 microlitre
tocopherol and 1 microlitre of Rosamarinus essential oil was added to the aforesaid mixture. Then the
mixture was cooled to room temperature. This cooled mixture is now ready for application.
420/1651
Substance Amount Percentage
1. Colour 0. 5mg 0. 5%
2. Safflower oil 1. 0mi 1.0%
3. Castor oil 1. O ml 1.0%
4. Tocopherol 5 Al 0.005%
5. Rosamarinus (Essential oil) 1. 0). 11 0. 001%
6.Bees wax 1.5 gm To make up 100%
Example-9 0.5 mg of herbal colour was mixed with 1 ml of Safflower oil and 1 ml Castor oil thoroughly.
In the said mixture 1.5 gm of melted bees wax was mixed at a temperature of 70 C. After that 5
microlitre tocopherol and 1 microlitre each of Jasminum and Santalum essential oils were added to
the aforesaid mixture. Then the mixture was cooled at room temperature. This cooled mixture is now
ready for application.
Substance Amount Percentage
1. Colour 0. 1 mg 0.5%
2. Safflower oil 1. 0 ml 1.0%
3. Castor oil 1.0 ml 1.0%
4. Tocopherol 5.0 l 0.005%
421/1651
5. Jasminum and Santalum 1.0 l 0.001%
(Essential oil)
6. Bees wax 1. 5 To makeu 100%
Example-10
0.5 mg of red colourant was mixed with 1 ml of safflower oil and 1 ml of castor oil thoroughly. In the
said mix, 0.5 gm of melted bees was mixed at a temperature of 70oC. After that 5 microliter
tocopheral and 1 microlitre of sandal wood oil was added to the aforesaid mixture. Then the mixture
was cooled to room temperature. Thus, cooled mixture is ready for application as eye shadows.
Substance Amount Percentage
1. Colour 0. 5mg 0.5%
2. Safflower oil 1. 0 ml 1.0%
3. Castor oil 1. 0 ml 1.0%
4. Tocopherol 5.0 jl 0. 005%
5. Sandal wood oil (Essential oil) 1. 0 il0. 001%
6. Bees wax0. 5 gmTo make up 100%
Example-11
1.0 mg of herbal colour was mixed with 1 ml of safflower oil and 1 ml of castor oil thoroughly. Then
mixed 0.2 gm of melted bees wax at a temperature of 70 C. After that 10 microliter tocopherol and 2
422/1651
microlitre of Rose oil was added to the aforesaid mixture. Then the mixture was cooled to room
temperature. Thus, cooled mixture is ready for application as glowglitters.
Substance Amount Percentage
1. Colour 1. 0 mg 1.0%
2. Safflower oil 1. 0ml 1.0%
3. Castor oil 1. 0ml 1.0%
4. Tocopherol 10 l 0.01%
5. Rose-oit (Essentialoil)--2 : 0-1 0. 002%
6. Bees wax 0. 2 To make u 100%
Example-120.25 mg of rose red colourant was mixed with 10 gm talc in ball mill. In said mixture 1 microliter of
Jasmine essential oil was added and mixed thoroughly. The colorant mixed is now ready for rouges.
Substance Amount Percentage
1. Colour 0. 25 mg 0.25%
2. Jasmine (Essential oil) 1.0 Al 0. 001%
3. Talc 10. 0 gm To make up 100%
I Example-13 (Antidepressant activity)
0.5 mg of herbal colour was mixed with 1 ml of Safflower oil and 1 ml Castor oil thoroughly. In the
said mixture 1.5 gm of melted bees wax was mixed at a temperature of 70 C. After that 5 microlitre
tocopherol and 1 microlitre blend of sweet basil oil (having linaloal and linolyl acetate), Jasminum
423/1651
and lemon grass oil/citral essential oil was added to the aforesaid mixture. Then the mixture was
cooled to room temperature. This cooled mixture is now ready for application.
Substance Amount Percentage
1. Colour 1. 5mg 1.0%
2. Safflower oil 1. 0 ml 1.0%
3. Castor oil 1. 0 ml 1.0%
4. Tocopherol 10. gel 0. 01%
5. Sweet basil oil, Jasmine and lemon 2. 0pu 0. 002%
grass oil
6. Bees wax 1.5 gm To make up 100%
Example-14 (Mood lifting)
1.5 mg of herbal colour was mixed with 1 ml of Safilower oil and 1 ml Castor oil thoroughly. In the
said mixture 1.5 gm of melted bees wax was mixed at a temperature of 70 C. After that 5 microlitre
tocopherol and 1 microlitre blend of Jasmine, Muskon oil and lavender oil essential oil was added to
the aforesaid mixture. Then the mixture was cooled to room temperature. This cooled mixture is now
ready for-application
. Substance Amount Percentage
1.Colour 1.5 mg 1.0%
2. Safflower oil 1.0ml 1.0%
3. Castor oil 1.0 ml 1.0%
4. Tocopherol 10 Al 0.01%
424/1651
5. Jasmine, Muskon oil and 2. 0 gel 0. 002%
Lavender oil (Essential oil)
6. Bees wax 1. 5 To make u 100%
Example - 15 (lipstick for men)
1 ml of Safflower oil and 1 ml Castor oil thoroughly. In the said mixture 1.5 gm of melted bees wax
was mixed at a temperature of 70 C. After that 5 microlitre tocopherol and 1 microlitre blend of
sandal wood oil'and basil oil was added to the aforesaid mixture. Then the mixture was cooled to
room temperature. This cooled mixture is now ready for application.
Substance Amount Percentage
1. Safflower oil 1.0 ml 1. 0%
2. Castor oil 1. 0 ml 1.0%
3. Tocopherol1010. 01%
4. Sandal wood oil or basil oil 2. 0 l 0.002%
(Essential oil)
5. Bees wax 1. 5 To make u 100%
Table 1: Preferred list of Aroma i. e essential oils for the functional attributes in cosmaceutical
application
425/1651
FUNCTIONAL ESSENTIAL OILS PREFERRED RATIO
ATTRIBUTES
1. Antidepressant 1. Ocimum oil : Jasminum oil : Cymbopogon oil (1 : 2 : 1)
2. Ocimum oil : Mentha oil: Rosmarinus oil (2 : 1 : 1)
3. Jasminum oil: Mentha oil: Rosmarinus oil (1 : 1 : 1)
4. Cymbopogon oil : Ocimum oil : Mentha oil (1 : 2 : 1)
5. Ocimum oil: Cymbopogon oil1 (2 : 1)
6. Mentha oil : Rosmarinus oil (1 : 1)
7 Ocimum oil
8 Rosmarinus oil
2. Anti stress 1. Santalum oil: Lavandula-oil (2 : 1)
2. Lavandula oil : Eucalyptusoil : Rosa oil (1 : 1 : 1)
3. Eucalyptus : l : Rosa oil (1 : 2)
4. Aluillaria oil: Elettaria oil: Rosmarinus oil (1 : 1 : 1)
5. Jasminum oil
6. Tantalum oit
7. Lavandula oil
3. Refreshing 1. Santalum : Rosa oil: Rosmarinus oil (1 : 1 : 1)
2. Santalum oil : Pelargonium oil (1 : 2)
3 Jasminum oil: Lavandula oil (1 : 2)
4 Lavandula oil
5 Santalum oil : Rosa oil (1 : 2)
6 Santulam oil
4. Sensual Feeling 1. Jasminum oil : Lavandula oil : Pelorgonium oil (1 : 2: 1)
2 Ocimum oil: Jasminum oil: Cymbopogon oil (1 : 2 : 1)
3 Jasminum oil
4 Jasminum oil: Lavandula oil (2 : 1)
5. Creative Thoughts 1. Santalum oil
2 Santalum oil: Rosa oil (1 : 2)
6. Mood lifting 1. Jasminum oil: Rosa oil: Palergonium oil (1 : 2)
2. Rosmarinus oil
3. Cymbopogan oil : Rosa oil (2 : 1)
4. Rosa oil
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5 Jasminum oil : Rosa oil
7. Anxiety 1. Rosa oil : Cinnamomum oil (1 : 2)
Table 2: Preferred list of Aroma isolates for the functional attributes in cosmaceutical application.
FUNCTIONAL AROMA ISOLATE PREFERRED RATIO
ATTRIBUTES
1. Anti stress Citral
2. Refreshing 1. Linalol
2. Benzyl alcohol
3. Terpeneol
4. Terpeneol : Linalol (1:2)
3. Sensual Feeling BMnc ac d
4. Creative Thoughts 1. Isobutyric acid: Butyric acid: linalol (1:2:1)
2. Isobutyruc acud: Benzyl: linalol (1:2:1)
3. Isobutyr acid :
4. Linalol: Isobutyric acid (1:2)
5. Mood lifting 1. Jasmone
2. Citral
3. Eugenol
4. Citral
5. Eugenol: Citral (1:2)
The change in color of the colourants, occurs then they are subjected to acid or base treatments.
For example, change of colour occurs by treating the colourant with traces of food grade acids
example acetic acid at a quantum less than 0. 1%, likewise, the change of colour occurs with the
treatment of base which can be as traces as less than 0. 1%.
427/1651
The following four tables provide information about the color changes change occur due to acid or
base treatments.
Table 3: DIRECT EXTRACTION (PROCESS 1) Change of colour with bases
Sodium Hydroxide Potassium Hydroxide Sodium acetate
Code Colours
2% 0.1% 0.05% 2% 0.1% 0.05% 2% 0.1% 0.05%
1. 58C 95A 98B 98B 98B 99C 100B 80D 97B 97C
2. 55A 101A 100D 100B 105D 94B 93D 82A 97C 97D
3. 58B IOIB 100B 100D 101D 93B 93C 80C 97B 97D
4. 55B 9SB 97D 100C 107A 99C 100B 80D 97C 97D
5. 55C 98A 98C 98D 101B 92B 92D 80B 97D 97D
6. 115B 115B 114B 94C 115A 114B 95D 201B 97D 114D
7. 115A 115A 113C 113C 114D 113C 115B 116B 111B 113C
8. 122A 122A 187B 187C 122B 187C 200D 201A 183C 182A
Table 4 : DIRECT EXTRACTION (PROCESS 1) Change of colour with acids
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Acetic acid Citric acid Oxalic acid
Code Colours 2% 0. 1% 0.05 2% 0. 1% O. Q5 2% 0. 1% 0. 05
%%%
1. 58C 46C 73B 65B 46B 5"5B 56A 47D 48D 49A
2. 55A 55C 68C 69A 51A 55C 56A 51B 52C 52D
3. 58B 73D 75D 75D 73C 38A 39C 73A 69A 69A
4. 55B 73B 73D 73D 73C 73D 69A 73A 69B 69B
555C 70D 68D 69A 73D 69A 69B 68D 38A 38B
6. 115B 95C 94B 94C 96B 95C 95D 97B 97D 97D
7. 115A 115B 113C 133C 116C 115A 115B 113A 111B 111B
8. 122A 200A 200C 200C 200B 200C 200D 183D 183C 182A
Table 5: From Column (PROCESS 2) Change of colour with acids
Acetic acid Citric acid Oxalic acid
Code Colours 2% 0.1% 0.05% 2% 0.1% 0.05% 2% 0.1% 0.05%
C1 25B 25C 24A 24A 24A 24A 24C 24C 24A 24C 24C 24A
C2 31C 29B 29C 29C 27A 27B 27B 29B 29C 27B
C334C 33A 33C 33C 33A 33C 33D 33A 33C 33C
C4 32C 29A 28C 28D 29A 28D 28D 29A 28C 28D
Cs 33B 40C 39C 39D 31B 30C 30D 31C 31D 31D
C6 46A 46A 45C 45D 32A 31B 30C 33B 32A 32B
C7 44A 43A 40B 40C 45D 42A 42B 45C 44B 44C
Cs 46B 47B 47D 47D 47B 48A 48B 46C 46A 46D
C9 59A 60A 59D 57D 59B 59D 59D 60B 60C 59C
Clo 95A 95C 94B 94C 96B 95C 95D 97B 97D 97D
C11 103A 200A 200C 200C 187A 187C 187D 187A 187C 187C
Cn 114A 115B 113C 113C 116C 115A 115B 113A 111B IIIB
C13 187B 182A 180C 180D 182C 181D 181D 180B 181C 181D
C14 187A 59A 60B 60C 59B 58A 58C 59D 58D 58C
C15 79A 187A 183A 183C 187B 187B 185C 182C 181D 181D
Ci6 200A 200A 200C 200C 200B 200C 200D 183D 183C I82A
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Table 6: From Column (PROCESS 2) Change of colour with bases
NaOH KOH CH3COON2
cOLOURS 2% 0.1% 0. 05% 2% 0. 1% 0.05% 2% 0. 1% 0. 05%
Cl 25B 90A 89A 24A 92A 89C 24C 181B 24C 89D
C2 31C 106B 106D 29C 98B 105d 27B 58C 29C 105D
C3 34C 86C 33C 33C 83B 83C 33D 171C 33C 83D
C4 32C 93B 93D 28D 102A 99C 28D 169C 28C 93C
Cs 33B 98B 98C 39D 105C 98C 30D 169B 31D 99C
C6 46A I03C 102C 45D 98B 102D 30C 34B 32A lOlC
C7 44A 102B 102C 40C-116A 102D'42B 40A 44B 102D
Cg 46B 116B 116D 47D 116A 116D 48B 46A 46A 116C
Cg 59A 116C 116D 57D 115B 116D 59D 53A 60C 116D
Cato 95A 115B 114B 94C 115A 114B 95D 201B 97D 114D
Cll 103A 188A 200C 200C 116B 200C 187D 83B 187C 200C
C, 2 114A 115A 113C 113C 114D 113C 115B 116B 111B 113C
C13 187B 122B 121C 180D 114B 121C 181D 199C 181C 119C
Cl4 187A 120C 120D 60C 114C 120D 58C 201B 58D 119D
C. s 79A 119B 119C 183C 114A-187B 185C 201C 181D 181D
C16 200A 122A 187B 187C 187B 187C 200D 201A 183C 182A
Table 7: Table for correspondence of colour codes based on Flower Council of Holland.
Codes Group
1-13 Yellow group
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14-23 Yellow-Orange group
24-29 Orange group
30-35 Orange-Red group
36-56 Red group
57-74 Red-Purple group
75-79 Purple group
80-82 Purple-Violet group
83-88 Violet group
89 - 98 Violet - Blue group
99-110 Blue group
111-124 Blue-Green group
125-143 Green group
144-154 Yellow-Green group
155 White group
156-157 Grey-White group
158-159 Orange-White group
160-162 Greyed-Yellow group
163-177 Greyed-orange group
178-182 Greyed-Red group
183-187 Greyed-Purple group
188-198 Greyed-Green group
199-200 Brown group
201 Grey group
202Black group
The various colours shown above are codified according to RHS colour chart in association with
Flower Council of Holland and The Royal Horticultural Society, London
The main advantages of the present invention are:
1. Herbal colourants offer an advantage in that they can be added or used without taking into
consideration certification by different agencies like FAO, WHO and Cosmetic authorities etc.
2. The herbal colourants are safe, eco-friendly and health protective.
431/1651
3. These herbal colourants may be used in more sensitive and delicate parts of the body like lips,
cheeks and eyelids.
4. These herbal colourants can be used in leucoderma particularly of lips region.
S. The herbal colours are 100% lipophilic in nature.
6. The herbal colours are antimicrobial and anti-inflammatory.
7. The herbal colours are free from any strong side effects like carcinogenic effects to the users.
8. The herbal colours can be made in different shades in a cost-effective manner.
9. Addition of different essential oil and their isolates promotes the stimulation of creative
thoughts, enhance sensual feeling induce positive mental health and well being and to help
~~qnhance sen thorts to overcome the depressant feelings (anti-depressant).
Thus an aim of the present invention is to develop a safe and eco-friendly health protective and
beauty enhancing herbal functional composition that contains only the natural products. The natural
safe colour has been obtained and developed from different plant species belonging to the genus
Arnebia, Bixa, Butea, Carthamus, Hibiscus, Jatropha, Lithospermum, Macrotomia, Maharanga,
Nyctanthes, Onosma, Rhododendron and Tagetes. Various shades of colours were differentially
extracted by following certain well-defined extraction methods. The invention also seeks to use
lipstick as a medium of aroma therapy. Essential oils isolated from different plants belonging to the
genus Aquillaria, Cinnamomum, Cymbopogon, Elettaria, Eucalyptus, Geranium, Jasminum, Ocimum,
Pelargonium, Rosa, Rosmarinus, Santalum and Vetiveria etc. Various blends of these essential oil
isolates have been used to get desired effect like anti-depressant and creative thoughts.Claims:
CLAIMS : 1. A safe ecofdendly, health protective and beautifying herbal cosmetic composition
containing herbal colourants together with a cosmetically acceptable amount of one or more
additives providing special properties and a cosmetically acceptable base material.
432/1651
2. A composition as claimed in claim 1 wherein, the additives providing special properties are
selected from essential oils/aroma isolates obtained from the group of plant species belonging
to genera Acquillaria, Cinnamomum, Cymbopogon Elettaria, Eucalyptus, Geranium, Jasminum,
Ocimum, Pelargonium, Rosa, Rosmarinus, Santalum and Vetiveria.
3. A composition as claimed in claim 1 wherein, the essential oils/aroma isolates act as mood lifting
agents, antidepressant agents, anti stress agents, sensual pleasure providing agents, creative
thought inducing agents, anxiety reducing agent, refreshing agent, stimulant, soothing agents, anti
oxidants, fixative, fragrants and antimicrobial.
4. A composition as claimed in claim 1 wherein, the essential oils/aroma isolates release
neurochemicals in the brain through the receptors in mouth and nose and provide mood
enhancement, sensual pleasure, anti-depressant and creative thought inducing properties.
5. A composition as claimed Jnclaml wherein, the colourants are isolated from specieces belong to
the genera of the family Boraginaceae, which are non-toxic and free from any side effects.
6. A composition as claimed in claim 1 wherein, the colourant is obtained from the plants
belonging to the genus Arnebia, Bixa, Butea, Carthamus, Hibiscus, Jatropha, Lithospermum,
Macrotomia, Maharanga, Nyctanthes, Onosma, Rhododendron, and Tagetes 7. A composition as
claimed in claim 1 wherein, the colourants are extracted from root, stem or leaves of the plants and
the quantum of the essential oils used base on the part from which the essential oil is extracted.
8. A composition as claimed in claim 1 wherein, the colourants are soluble in organic solvents
selected from hexane, petroleum ether, benzene, diethyl ether, ethylacetate, chloroform, acetone
and alcohol in the range 30 to 100 %.
9. A composition as claimed in claim 1 wherein, the colourants has pH between 5 to 6.
10. A composition as claimed in claim 1 wherein the colourant is present in an amount of 0.1 to
10%.
433/1651
11. A composition as claimed in claim 1 wherein the colourant are anti microbial, anti- inflammatery
and are used in leucoderma more particularly of lips.
12. A composition as claimed in claim 1 wherein, the colourant has lipophilic properties.
13. A composition as claimed in claim 1 wherein, the colourant is a mixture of naphthazarins and/or
cyclic unsaturated diketones in which double bonds and keto groups may be conjugated.
14. A composition as claimed in claim 1 wherein, the colourant has different shades of colours
selected from purplish red, cerise, ruby red, beet root purple, dark violet, deep blue, blackish blue,
pastel red, pale red, purplish red, rose red, cerise, ruby red, deep magenta, beet root purple,
amaranth, dark purple, dark violet, deep violet, deep blue and blackish blue.
15. A composition as claimed in claim 1 wherein, the red colour of the colourant may be changed to
different shades with organic and inorganic acids.
16. A composition as claimed in claim 15 wherein, the intensity of the red colour of the herbal
colourant may be increased with organic acids and decreased with inorganic acids.
17. A composition as claimed in claim 15 wherein, the concentration of the acids is 1 to 20%.
18. A composition as claimedTiTclainri whereinTthe red'colour of the herbal colourant may be
changed to different shades with organic and inorganic bases.
19. A composition as claimed in claim 18 wherein the intensity of the red colour of the herbal
- - colourant may be increased with organic bases and decreased with inorganic bases.
20. A composition as claimed in claim 18 wherein the concentration of the bases is 1 to 20%.
21. A composition as claimed in claim 1 useful as a lipstick for man for aromatherapy.
434/1651
22. A composition as claimed in claim 1 useful as an eye-shadow application.
23. A composition as claimed in claim 1 useful as a glow glitter.
24. A composition as claimed in claim 1 useful as a rose.
25. A composition as claimed in claim 1 wherein the essential used is in the range of traces to ppm.
26. A composition as claimed in claim 1 wherein the softening agents used are in the range of
0.5% to 2% of the total weight of the composition.
27. A composition as claimed in claim 1 wherein lusture producing agents are in the range of
0.5% to 2%.
28. A composition as claimed in claim 1 wherein skin protecting agents are in the range of 0.0001 to
0. 09%.
29. A composition as claimed in claim 1 wherein essential oil used for functional attributes range
between 0.0001 to 0.009 %.
30. A composition as claimed in claim 1 wherein beeswax is used as a base material and forms the
balance amount of the composition.
31. A composition as claimed in claim 1 wherein the aroma is provided by essential oils obtained
from the group of plant species belonging to genera Acquillaria, Cinnamomum, Cymbopogon
Elettaria, Eucalyptus, Geranium, Jasminum, Ocimum, Pelargonium, Rosa, Rosmarinus,
Santalum and Vetiveria.
435/1651
32. A composition as claimed in claim 1 wherein the cosmaceutical application and use of extracted
organic compound in lipsticks, eye shadow, glow glitters, rouges and skin conditioning agents.
33. A composition as claimed in claim 1 wherein the composition is a lipstick having improved
moisturizing effect.
34. A composition as claimed in claim 1 wherein, the additives are a mixture of essential oils
functioning as a mood-lifting agent, anti stress agent, anxiety reducing agent, sensual feeling agent,
an anti-depressant agent, a creative thought inducing agent, a refreshing agent, anti oxidant, fixative
and a stimulant.
35. A composition-as-jclaimedinclaim L wherein, anti-depressant property imparted by the essential
oils are selected from
Essential Oils Preferred Ratio
1. Ocimum oil : Jasminum oil : Cymbopogon oil (1 : 2 : 1)
2. Ocimum oil : Mentha oil: Rosmarinus oil (2 : 1 : 1)
3. Jasminum oil : Mentha oil: Rosmarinus oil (1 : 1 : 1)
4. Cymbopogon oil : Ocimum oil : Mentha oil (1 : 2 : 1)
5. Ocimum oil: Cymbopogon oill (2 : 1)
6 Mentha oil : Rosmarinus oil (1 : 1)
7 Ocimum oil
8. Rosmarinus oil
36. A composition as claimed in claim 1 wherein, the creative thought-inducing property is imparted
by the essential oils selected from
Essential oil Preferred rato
1 Tantalum oit
2 Santalum oil: Rosa oil (I : 2)
436/1651
37. A composition as claimed in claim 1 wherein, the anti-stress property is imparted by the
essential oils selected from
Essential oil Preferred ratio
1. Santalum oil: Lavandula oil (2: 1)
2. Lavandula oil : Eucalyptus oil : Rosa oil (1 : 1 : 1)
3. Eucalyptus oil: Rosa oil (1 : 2)
4. Aluillaria oil: Elettaria oil: Rosmarinus oil (1 : 1 : 1)
5. Jasminum oil (1 : 2)
6 Santalum oil
7 Lavandula oil
38. A composition as claimed in claiml wherein, the refreshing property is imparted by the essential
oils selected from
Essential oil Preferred ratio
1. Santalum oil: Rosa oil: Rosmarinus oil (1 : 1 : 1)
2. Santalum oil: Pelargonium oil (1: 2)
2. Jasminum oil: Lavandula oil (1 : 2)
3. Santalum oil: Rosa oil (1 : 1)
4. Lavandula oil
J. Santalum oil
39. A composition as claimed in claim 1 wherein, the sensual feeling property is imparted by the
essential oils selected from
437/1651
Essential oil Preferred ratio
1. Jasminum oil : Lavandula oil: Pelorgonium oil (1 : 2)
6 Ocimum oil: Jasminum oil: Cymbopogon oil (1: 2: 1)
7 Jasminum oil
8 Jasminum oil : Lavandula oil (2: 1)
40. A composition as claimed in claim 1 wherein, the mood lifting property is imparted by the
essential oils selected from
Essential oil Preferred ratio
1. Jasminum oil : Rosa oil : Palergonium oil (I : 1: 1)
2. Rosmarinus oil
3. Cymbopogan oil : Rosa oil (2: 1)
4. Rosa oil
5. Jasmmum oil : Rosa oil
41. A composition as claimed in claim 1 wherein, the anxiety reducing property is imparted by the
essential oils selected from
Essential oil Preferred ratio
1 Rosa Oil : Cinnamomum os 2)
42. A composition as claimed in claim 1 wherein, the anti-stress property is imparted by the aroma
isolate Citral 43. A composition as claimed in claim 1 wherein, the refreshing property is imparted by
438/1651
the aroma isolate selected from linalol, benzyl alcohol, terpeneol, terpeneol and linaol at a preferred
ratio of 1: 2.
44. A composition as claimed in claim 1 wherein, the sensual feeling property is imparted by the
aroma isolate butyric acid.
45. A composition as claimed in claim 1 wherein, the creative thoughts property is imparted by the
aroma isolate selected from
Aroma Isolate Preferred ratio
1. Isobutyric acid: Butyric acid: linalo (1:2:1)
2. Isobutyruc acud: Benzyl alcohol: linalol (1:2:1)
3. Isobutyric acid:
4. Linalol: Isobutyric acid (1:2)
46. A composition as claimed in claim 1 wherein, the mood lifting property is imparted by the aroma
isolate selected from jasmone, citral, eugenol, eugenol and citral at a preferred ratio
1: 2.
47. A composition as claimed in claim 1 wherein, the fixative is tocopherol and santulam oil,
tocopherol also functions as fixative, which may present in traces to ppm.
48. A process for extraction of organic colourants from the plants, said process comprising obtaining
the plant parts, extracting with organic solvents, removing the solvents by conventional methods,
concentrating the extract under reduced pressure and optionally treating with acids or bases to
produce various shades.
49. A process for the extraction of organic colourants, said process comprising the steps of : a)
drying the plant parts, b) powdering the dried plant parts, c) subjecting the dry powder obtained in
step (b) to Soxhlet extraction at a temperature in the range of 40-80 C or cold percolation with
organic solvents at a temperature between 20 to 45 C, d) concentrating the mixture of step (c) by
conventional methods at reduced pressure in the range of 50-100 psi and at a temperature not
exceeding 50 C,
439/1651
e) mixing the concentrate of step (d) with silica gel in the ratio 1: 3 to 2: 7 to obtain a slurry, f) eluting
the slurry with organic solvents resulting in various fractions, g) concentrating the fractions at a
pressure in the range of 50-100 psi resulting in herbal colourants, optionally treating the said colours
with acids or bases to produce various shades, and h) obtaining various colours from by treating the
said fractions with acids or bases to produce colourants of various shades.
50. A process as claimed in claim 49 wherein, the organic solvent is selected from polar solvents,
non-polar solvents or mixtures thereof.
51. A process as claimed in claim 49 wherein, the polar solvents are selected from acetone,
chloroform, ethyl acetate, methanol and ethanol.
52. A process as claimed in claim 49 wherein, the non-polar solvents are selected from petroleum
ether, hexane, toluene and cyclohexane 53. A process of extraction of herbal colourants from plants
of the family Boraginaceae, which comprises ; percolating powdered plant parts with alcohol at room
temperature resulting in alcohol soluble herbal material, the said herbal material being concentrated
by known means at pressures in the range of 50-100 psi and at a temperature in the range of 40-60
C, the said concentrate being made into a slurry with silica gel in a ratio in the range of 1: 3 to 2: 7,
the said slurry being eluted by known means with organic solvents resulting in fractions, the said
fractions further being concentrated by known methods at a pressure in the range of 50-100 psi
resulting in herbal colorants, optionally treating the said colours with acids or bases to produce
various shades.
54. A process as claimed in claim 53 wherein, the plants are selected from the group of plants
belonging to the family Boraginaceae 55. A process as claimed in claims 49 and 53 wherein, the
plant parts are selected from root, stem and leaf the quantum of the essential oils used base on the
part from which the essential oil is extracted 56. A process as claimed in claims 49 and 53 wherein,
the plant parts are dried at a temperature in the range of 30-450 C, in shade.
57. A process as claimed in claims 49 and 53 wherein, the dried plant parts are powdered to particle
size in the range of 30-60 mesh.
440/1651
58. A process as claimed in claim 53 wherein, the alcohol used is selected from group consisting of
methanol and ethanol.
59. A process as claimed in claim 53 wherein, the organic polar solvents are selected from acetone,
chloroform, ethyl acetate, methanol and ethanol.
60. A process as claimed in claim 53 wherein, the non-polar solvents are selected from petroleum
ether, hexane, toluene and cyclohexane 61. A process as claimed in claims 49 and 53 wherein, the
ratio of polar and non-polar solvent caries according to the nature of the solvents.
62. A process as claimed in claims 49 and 53 wherein, the mixture of non-polar solvent to chloroform
is prepared in the ratio of 99 : 1 to 0 : 100.
63. A process as claimed in claims 49 and 53 wherein, the colourants ranges from purplish red,
cerise, ruby red, beetroot purple, dark violet, deep blue, blackish blue, pastel red, pale red, purplish
red, rose red, cerise, ruby red, deep magenta, beet root purple, amaranth, dark purple, dark violet,
deep violet, deep blue and bla-cldili blue.
64. A process as claimed in claims 49 and 53 wherein, the acid used is selected from the group
consisting of organic acids such as formic acid and acetic acid, inorganic acids such as HC1,
HN03 and H2SO4 65. A process as claimed in claims 49 and 53 wherein, the acid concentration is in
the range of
0.1% to 10%.
66. A process as claimed in claims 49 and 53 wherein, the change of colour in the colourant is
effected by treating the colourant with traces of food grade acids such as acetic acid, taken in an
amount of 0. 1 %.
67. A process as claimed in claims 49 and 53 wherein, the change of colour in the colourant is
effected by treating the colourant with traces of bases taken in an amount of 0. 1%.
441/1651
68. A process as claimed in claims 49 and 53 wherein, the bases are selected from organic bases
such as sodium acetate, potassium acetate and diethyl amine and inorganic bases such as
NaOH, KOH, Na2C03 and NaCl 69. A process as claimed in claims 49 and 53 wherein, the
concentration of the base is in the range of 0.1% to 20%.
70. A process as claimed in claims 49 and 53 wherein, the herbal colourant is antimicrobial, antiinflammatory and is used in leucoderma more particularly of lips.
71. A composition according to any one of claims 1 to 47, formulated as a lipstick.
72. A composition according to any one of claims 1 to 47, formulated as eye- shadow.
73. A composition according to any one of claims 1 to 47, formulated as a skin cream.
74. A composition according to any one of claims 1 t o47, formulated as glow-glitter.
75. A composition according to any one of claims 1 to 47, formulated as rouge.
76. A safe eco friendly, health protective and beautifying herbal cosmetic composition, substantially
as hereinbefore described.
77. A safe eco friendly, health protective and beautifying herbal cosmetic composition, substantially
as hereinbefore described with reference to the accompanying drawings.
78. An organic colourant, extracted by means of a process according to any one of claims 48 to 52.
79. A herbal colourant from a plant of family Boraginaceae, extracted by means of a process
according to any one of claims 53 to 70.
80. A process for extraction of organic colourants from plants, substantially as hereinbefore
described.
81. A process for extraction of herbal colourants from plants of the family
442/1651
Boraginaceae, substantially as hereinbefore described.
443/1651
68. FR2830198 - 04.04.2003
COMPOSITIONS CONTAINING RAVENSARA AROMATICA ESSENTIAL OIL AND ONE OR MORE
OTHER ESSENTIAL OILS FOR TREATMENT OF VIRAL, FUNGAL, AND PARASITIC INFECTIONS,
CYSTIC FIBROSIS, AIDS, AND CERTAIN TUMORS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2830198
Inventor(s):
WILLEM JEAN PIERRE (--)
Applicant(s):
WILLEM JEAN PIERRE (FR)
IP Class 4 Digits: A61K; A61P
IP Class:
A61K35/78; A61K9/48; A61P35/00; A61P31/12; A61P31/04; A61P31/10; A61P31/18
E Class: A61K35/78
Application Number:
FR20010012543 (20010928)
Priority Number: FR20010012543 (20010928)
Family: FR2830198
Abstract:
COMPOSITIONS CONTAINING THE ESSENTIAL OIL OF RAVENSARA AROMATICA
(AGATHOPHYLLUM AROMATICA) TOGETHER WITH OTHER ESSENTIAL OILS. COMPOSITIONS
CONTAINING THE ESSENTIAL OIL OF RAVENSARA AROMATICA (AGATHOPHYLLUM AROMATICA)
TOGETHER WITH OTHER ESSENTIAL OILS SELECTED FROM THOSE OBTAINED FROM
ORIGANUM COMPACTUM, MELALEUCA QUINQUENERVIA, HELICHRYSUM ITALICUM, LAURUS
NOBILIS, TRACHYSPERMUM AMMI, EUGENIA AROMATICA, EUGENIA CARYOPHYLLATA, INULA
GRAVEOLENS, CYMBOPOGON MARTINII, ROSMARINUS OFFICINALE, EUCALYPTUS RADIATA,
OCIMUM BASILICUM, LAVANDULA SPICA, THYMUS OFFICINALIS, CISTUS LADANIFER, ANIBA
ROSAEDORA, MELALEUCA ALTERNIFOLIA, CINNANOMUMCASSIA, CINNANOMUM
444/1651
AROMATICUM, LEDUM GROENLANDICUM, CALATROPIS PROCERA, AND CAJANUS CATJAN, IN
A CARRIER, EXCIPIENT OR DILUENT APPROPRIATE FOR THERAPEUTIC USE.Description:
COMPOSITIONS PHARMACEUTIQUES COMPRENANT DES HUILES
ESSENTIELLES ET LEURS UTILISATIONS La prйsente invention se rapporte а l'utilisation de plantes
ou de parties de plantes, pour la rйalisation de compositions pharmaceutiques.
L'invention concerne plus particuliиrement des compositions pharmaceutiques renfermant
principalement de l'huile essentielle de Ravensara aromatica (Agathophyllum aromatica) associйe а
d'autres extraits de plantes.
Elle a spйcifiquement pour objet des compositions pharmaceutiques caractйrisйes en ce qu'elles
contiennent principalement de l'huile essentielle de Ravensara aromatica associйe а d'autres huiles
essentielles choisies parmi l'Origan (Origanum compactum), le Niaouli (Melaleuca quinquenervia),
l'Hйlichryse (Helichrysum italicum), le Laurier noble (Laurus nobilis), l'Ajowan (Trachyspermum
ammi), le Giroflier (Eugenia aromatica et Eugenia caryophyllata), l'inule odorante (Inula graveolens),
le Palmarosa (Cymbopogon martinii), le Romarin (Rosmarinus officinalis), l'Eucalyptus radiй
(Eucalyptus radiata), le Basilic (Ocimum basilicum), la Lavande aspic (Lavandula spica), les Thym
(Thymus officinalis et autres), la Ciste
ladanifиre (Cistus ladanifer), le bois de rose (Aniba rosaedora), le Tea Tree (Melaleuca alternifolia),
la Cannelle de Chine (Cinnanomum cassia et Cinnanomum aromaticum), le Ledon du groлnland
(Ledum groenlandicum), la Pomme de Sodome (Calotropis procera) et le Pois d'Angole (Cajanus
cajan) dans un excipient, un vйhicule ou un diluant appropriй pour l'usage thйrapeutique.
Les huiles essentielles peuvent йgalement кtre utilisйes telles quelles.
Les compositions pharmaceutiques selon l'invention peuvent contenir en outre un extrait de Poivrier
(Piper nigrum ou Piper longum) ou de la pipйrine qui renforce sensiblement les effets des principes
actifs contenus dans les huiles essentielles des plantes utilisйes dans la prйsente invention.
445/1651
Les compositions pharmaceutiques selon l'invention s'adressent plus particuliиrement au traitement
des affections virales, et/ou infectieuses, et/ou fongiques, et/ou parasitaires, des maladies comme la
mucoviscidose, des immunodйficiences telles que le SIDA et le traitement de certaines tumeurs.
Les propriйtйs anti-infectieuses et antivirales de Ravensara aromatica sont connues et utilisйes en
aromathйrapie. Les rameaux feuillus de Ravensara aromatica sont utilisйs traditionnellement en
infusion comme stomachique et carminatif et en sirop comme expectorant.
Les jeunes rameaux feuillus fournissent l'huile essentielle qui possиde des propriйtйs
neurotoniques, immunostimulantes, antivirales, anti infectieuses et dйcontractantes.
De mкme les huiles essentielles des autres plantes utilisйes dans les compositions
pharmaceutiques de la prйsente invention sont connues pour leurs propriйtйs fongicides (Ajowan,
Lavande aspic, Clou de Girofle, Origan), antivirales (Eucalyptus), parasiticide (Ajowan, Cannelle de
Chine) et immunostimulantes (Clou de Girofle, Eucalyptus, Origan).
Par exemple, le Niaouli est rйputй comme ayant des propriйtйs anti-infectieuses, anti-fongiques et
antivirales. L'huile essentielle de cette plante, riche en oxydes monoterpйniques (45 а 60% de 1-8
cinйole), en monoterpиne (10 % d'a-pinиne, 5 а 9 % de limonиne), en sesquiterpйnols (2 а 10%
de viridiflorol) est utilisйe pour traiter les infections des voies respiratoires, la grippe et l'herpиs.
L'association d'Eucalyptus radiй, d'Hйlichryse, d'Inule odorante, de Laurier noble, de Lavande
aspic, de Romarin, de Niaouli et de Ravensara aromatica forme une composition pharmaceutique
idйale pour le traitement de la mucoviscidose.
L'association d'Ajowa, de Cannelle de Chine, de Clou de Girofle, de Laurier noble,, de Lavande
aspic, d'Origan et de Ravensara forme une composition pharmaceutique idйale pour le traitement
des infections fongiques.
446/1651
L'association d'Ajowan, d'йcorce de Cannelle de Chine, de Clou de Girofle, de Tea Tree et de Thym
thymol forme une composition pharmaceutique idйale pour le traitement des infections parasitaires.
L'association de Ravensara, d'extrait de graines de Pois d'Angole et de Pomme de Sodome forme
une composition pharmaceutique idйale pour le traitement de la drйpanocytose.
L'association d'Ajowan, de bois de Rose, de Cannelle de Chine, de Ciste ladanifиre, d'Eucalyptus
radiй, de Clou de Girofle, de Lavande aspic, d'Origan, de Tea Tree, de Thym thymol, de Thym
thujanol, de Ravensara et de Palmarosa forme une composition pharmaceutique idйale pour le
traitement de l'immunodйficience humaine (SIDA).
L'association de Ravensara, de Ledon du groenland, de Basilic exotique, de Thym thujanol et de
Romarin forme une composition pharmaceutique idйale pour le traitement des hйpatites.
On peut йgalement citer а cet йgard la demande de brevet FR 2 709 964 qui a pour objet
l'utilisation de Ravensara aromatica en association avec certaines variйtйs de Lavande, de Niaouli,
de Basilic, avec du sulfate de zinc, de l'oxyde de zinc et du sulfate de cuivre, pour le traitement de
l'herpиs et de l'immunodйficience humaine (SIDA).
Les compositions pharmaceutiques selon la prйsente invention sont nettement plus actives.
Les compositions pharmaceutiques de la prйsente invention contiennent de 30% а 80% d'huile
essentielle de Ravensara aromatica qui est riche en 1-8 cinйole, un oxyde monoterpйnique dont les
propriйtйs antivirales, immunostimulantes et anti bactйriennes sont dйjа connues.
L'intйrкt de la prйsente invention est l'obtention de compositions pharmaceutiques contenant
principalement de l'huile essentielle de Ravensara aromatica, en association avec d'autres extraits
de plantes pour obtenir une potentialisation des
effets antiviraux, anti infectieux, fongicides, parasiticides, immunostimulants et/ou anticancйreux.
Les compositions de la prйsente invention peuvent кtre appliquйes localement notamment sous la
forme de mйlanges d'huiles essentielles brutes ou bien d'йmulsions H/E ou E/H, de gels, de
447/1651
pommades, d'huiles, de laits, de liposomes. Les compositions pharmaceutiques peuvent йgalement
кtre administrйes par voie orale, per-cutanйee, ou rectale, selon les cas, sous la forme de capsules
molles, de gйlules, de biogranules (malt), de suppositoire, de solutions ou d'йmulsions huileuses.
De faзon avantageuse, les compositions pharmaceutiques sont prйsentйes sous la forme de
mйlange d'huiles essentielles dispersйe dans une huile pйnйtrante et peuvent кtre utilisйes en
massage sur le thorax, les poignets et la nuque, а raison de 8 а 12 gouttes, trois fois par jour.
Parmi les huiles pйnйtrantes ou pourra citer l'huile d'amande douce, l'huile de noisette ou l'huile de
bourrache.
Des exemples non limitatifs de compositions pharmaceutiques selon l'invention sont prйsentйs cidessous : - Composition pour application topique antivirale (SIDA)
Huile
Huile
Huile
Huile
Huile
Huile
essentielle de Ravensara aromatica 30%
essentielle d'Origan compactum 10%
essentielle de Niaouli 6%
essentielle de Laurier noble 8%
essentielle d'Eucalyptus radiata 6%
d'Amande douce 40%
- Composition orale pour usage anti-cancйreux :
Huile essentielle de Ravensara aromatica 60%
Huile essentielle de Ledum groenlandicum 10%
Huile essentielle d'Helichrysum italicum 10%
Poloxamer 188 2%
448/1651
Vйhicule aqueux qsp 100%
Les compositions selon l'invention peuvent encore кtre formйes d'une йmulsion buvable rйpartie
en ampoules.
- Suspension buvable antivirale
Huile essentielle de Ravensara aromatica 40%
Huile essentielle d'Origan compactum 4%
Huile essentielle de Lavande aspic 8%
Hydroxy-йthyl-cellulose 2%
Hydroxy-propyl-mйthyl-cell ulose 4%
Tween 80 0,2%
Eau purifiйe qsp 100%
- Capsules molles On dissout dans 100ml d'huile de germe de blй, un mйlange de 60% d'huile
essentielle de Ravensara aromatica, 20% d'huile essentielle d'Origan, et de 20% d'huile essentielle
de Basilic. On ajoute au mйlange 0,1 g de pipйrine et on homogйnйise le mйlange.
Le mйlange est ensuite rйparti en capsules de gйlatine contenant chacune 0,2g de la solution
huileuse.Claims:
REVENDICATIONS 1. Compositions pharmaceutiques caractйrisйes en ce qu'elles contiennent
principalement l'huile essentielle de Ravensara aromatica associйe а d'autres huiles essentielles
choisies parmi l'Origan (Origanum compactum), le Niaouli (Melaleuca quinquenervia), l'Hйlichryse
(Helichrysum italicum), le Laurier noble (Laurus nobilis), l'Ajowan (Trachyspermum ammi), le Giroflier
(Eugenia aromatica et Eugenia caryophyllata), l'Inule odorante (Inula graveolens), le Palmarosa
(Cymbopogon martinii), le Romarin (Rosmarinus officinalis), l'Eucalyptus radiй (Eucalyptus radiata),
le Basilic (Ocimum basilicum), la Lavande aspic (Lavandula spica), les Thym
449/1651
(Thymus officinalis et autres), la Ciste ladanifиre (Cistus ladanifer), le bois de rose (Aniba
rosaedora), le Tea Tree (Melaleuca alternifolia), la Cannelle de Chine ( Cinnanomum cassia et
Cinnanomum aromaticum), le Ledon du groлnland (Ledum groenlandicum), la Pomme de Sodome
(Calotropis procera) et le Pois d'Angole (Cajanus cajan) dans un excipient, un vйhicule ou un diluant
appropriй pour l'usage thйrapeutique.
2. Compositions pharmaceutiques selon la revendication 1, caractйrisйes en ce qu'elles
contiennent de 30% а 80% d'huile essentielle de Ravensara aromatica.
3. Compositions pharmaceutiques selon la revendication 1, caractйrisйes en ce que l'excipient ou
le vйhicule est un de ceux qui conviennent pour кtre appliquйes localement sous forme
d'йmulsions H/E ou E/H, de gels, de pommades, d'huiles, de laits, de liposomes.
4. Compositions pharmaceutiques selon la revendication 1, caractйrisйes en ce que l'excipient ou
le vйhicule est un de ceux qui conviennent pour кtre pour кtre administrйes par voie orale, percutanйee, ou rectale, notamment sous la forme de capsules molles, de gйlules, de biogranules
(malt), de suppositoire, de solutions ou d'йmulsions huileuses.
5. Compositions pharmaceutiques selon la revendication 1, caractйrisйes en ce qu'elles
conviennent pour кtre appliquйes sous la forme de mйlanges d'huiles essentielles brutes.
6. Utilisation des compositions pharmaceutiques selon l'une des revendications 1 а 5 pour le
traitement des affections virales, et/ou infectieuses, et/ou fongiques, et/ou parasitaires, des maladies
comme la mucoviscidose, des immunodйficiences telles que le SIDA et le traitement de certaines
tumeurs.
450/1651
69. FR2832642 - 30.05.2003
ANTI-SKID PRODUCT, E.G. FOR SURFBOARDS OR TENNIS RACQUETS, COMPRISES A PASTE,
LIQUID OR OILY COMPOSITION CONSISTING OF A TACKY POLYBUTENE MATRIX AND AN OILY
COMPONENT SUCH AS SILICONE OIL OR ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2832642
Inventor(s):
KOWALSKI CHRISTIAN (--)
Applicant(s):
KOWALSKI CHRISTIAN (FR)
IP Class 4 Digits: A63C
IP Class:
A63C5/03
E Class: C08K5/01+L23/20; C08L23/20+B; C08L23/20+B4S; C09K3/14F
Application Number:
FR20010010613 (20010807)
Priority Number: FR20010010613 (20010807)
Family: FR2832642
Abstract:
AN ANTI-SKID PRODUCT (1) FOR SPORTS ARTICLES, TO BE APPLIED AS A THIN LAYER TO THE
SURFACE IN CONTACT WITH THE USER SO AS TO GIVE THE LATTER PERFECT ADHERENCE,
COMPRISES A PASTE, LIQUID OR OILY COMPOSITION CONSISTING OF A POLYBUTENE MATRIX
(A) SHOWING A TACKY PROPERTY AND AN OILY COMPOUND (B) SELECTED FROM SILICONE
OILS AND ESSENTIAL OILS.Description:
ANTIDERAPANT POUR ENGIN DE GLISSE TEL QU'UN SURF
451/1651
La prйsente invention concerne un antidйrapant pour engin de glisse, et plus particuliиrement un
produit antidйrapant du type composition pвteuse destinйe а кtre appliquйe en mince couche sur
la surface supйrieure d'un surf de vague pour permettre а l'utilisateur une adhйrence parfaite de
ses pieds
La pratique du surf est devenue un sport de plus en plus en vogue et de plus en plus sportif, et les
pratiquants font des figures et suivent des trajectoires sur l'eau particuliиrement difficiles surtout
dans les vagues. Les pratiquants recherchent les sites sur lesquels les vagues sont les plus grosses
voir les plus dangereuses. La pratique du surf est donc devenue trиs йlitiste nйcessite bien
entendu des conditions physiques particuliиrement bonnes et du matйriel appropriй. Les planches
proprement dites sont maintenant lйgиres et de bonne rйsistance, toutefois le problиme
d'adhйrence des pieds de l'utilisateur sur la surface supйrieure du surf, n'est pas encore
satisfaisante. De nos jours les surfeurs dйposent sur leur planche de la paraffine, en grattant la
surface de leur planche а l'aide d'un pain, afin d'y dйposйe une couche suffisante
La prйsente invention propose un nouveau produit destinй а recouvrir les zones ou doivent
adhйrer les pieds de l'utilisateur de la surface supйrieure du prйsente l'avantage d'кtre un
antidйrapant particuliиrement sur, et d'кtre utilisй en trиs faible quantitй, ce qui diminue le poids
de la planche. Ajoutons que le produit est non toxique, qu'il est stable en prйsence d'eau, et peut
supporter les fortes tempйratures. Par ailleurs, il a l'avantage de constituй une fois appliquй une
couche mince transparente laissant apparaоtre les marquages йventuels que proposent les
constructeur ou les sponsors. Ajoutons que le produit n'adhиre pas aux combinaisons en nйoprиne
que portent les utilisateurs.
Ainsi, le produit antidйrapant pour planche de surf, selon l'invention, du type destinй а кtre
appliquйe en mince couche sur la surface supйrieure du dit surf pour permettre а l'utilisateur une
adhйrence parfaite de ses pieds, est caractйrisй en ce qu'il est constituй par une
composition pвteuse dont la formulation lui confиre un aspect identique а une pommade, un gel,
ou une crиme, constituйe par au moins une matrice, et une huile.
Selon une caractйristique complйmentaire, la composition comprend un йpaississant et un parfum.
Selon des caractйristiques complйmentaires, la matrice est du polybutиne, tandis que l'huile une
huile de type silicone et l'йpaississant est une silice pyrolysйe.
452/1651
D'autres caractйristiques et avantages de l'invention se dйgageront de la description qui va suivre
en regard des dessins annexйs qui ne sont donnйs qu'а titre d'exemples non limitatifs.
La figure 1 est une vue montrant un surfeur en cours d'йvolution, pour illustrer le contexte
d'utilisation du produit.
La figure 2 reprйsente un exemple de conditionnement de la composition selon l'invention.
Les figure 3 et 4 reprйsentent la mise en oeuvre sur le surf, de la composition.
L'invention concerne donc un produit antidйrapant (1), qui est une composition pвteuse dont la
formulation lui confиre un aspect identique а une pommade, un gel, ou une crиme pour que
l'utilisateur (2) puisse l'appliquer aisйment sur la surface supйrieure (3) du surf (4) а l'aide par
exemple d'une raclette (5). La composition antidйrapante est avantageusement conditionnйe dans
un tube dйformable (6) tel qu'un tube du type dentifrice ou crиme cosmйtique.
Le produit antidйrapant (1) est constituй par au moins une matrice, et une huile. On y ajoutera
avantageusement un йpaississant et un parfum.
Comme matrice, on utilise avantageusement un polybutиne et comme huile une huile de type
silicone, tandis que comme йpaississant on utilisera une silice pyrolysйe.
A titre d'exemple la composition du produit peut кtre la suivante : - un polybutиne de poids
molйculaire 200 - une huile silicone comme par exemple celle commercialisйe sous la marque
Rhodorsil de rйfйrence 47V100000 - une charge constituйe par une charge minйrale comme une
solution colloпdale de silice
Comme йpaississant on a prйfйrй une silice pyrolysйe, car c'est un produit stable jusqu'а une
tempйrature de 150 degrйs.
453/1651
On ajoutera que l'йpaississant йradique l'effet de collage que donne le polybutиne seul, et permet
ainsi de calibrer l'effet antidйrapant.
Comme huile siliconй on pourrait tout aussi bien utiliser la rйfйrence 41V50000, mais cela
nйcessiterait d'en tripler la quantitй.
Il va de soi que l'on pourrait utiliser tout autre type d'йpaississant.
On utilise prйfйrablement de l'huile de silicone pour sa caractйristique de solubilitй dans le
polybutиne. Cette huile permet de minimiser l'effet de collage du polybutиne. Grвce а cette huile
l'utilisateur qui porte une combinaison en nйoprиne pourra кtre en contact corporel avec sa
planche sans que sa combinaison s'imprиgne du produit antidйrapant.
Les figures 3 et 4 illustrent comment l'utilisateur applique le produit antidйrapant de l'invention sur
sa planche. Ainsi, aprиs avoir ouvert le tube de produit (6), il dйpose une petite quantitй (7) de
produit (1) dans la zone (8) а recouvrir (figure 3), puis avec une petite raclette (5) par exemple en
matiиre plastique, il racle le produit pour l'йtaler (figure 4), et laisser ainsi une trиs fine couche de
produit antidйrapant.
Bien entendu, l'invention n'est pas limitйe aux modes de rйalisation dйcrits et reprйsentйs а titre
d'exemples, mais elle comprend aussi tous les йquivalents techniques ainsi que leurs
combinaisons.Claims:
REVENDICATIONS
1-Produit antidйrapant (1), pour planche de surf, du type destinй а кtre appliquйe en mince
couche sur la surface supйrieure du dit surf pour permettre а l'utilisateur une adhйrence parfaite de
ses pieds, caractйrisй en ce qu'il est constituй par une composition pвteuse dont la formulation lui
confиre un aspect identique а une pommade, un gel, ou une crиme.
2-Produit antidйrapant (1), selon la revendication 1, caractйrisй en ce que la composition est
constituй par au moins une matrice, et une huile.
3-Produit antidйrapant (1), selon la revendication 2, caractйrisй en ce que la composition
comprend un йpaississant.
454/1651
4-Produit antidйrapant (1), selon la revendication 3, caractйrisй en ce que la composition
comprend un parfum
5-Produit antidйrapant (1), selon la revendication 4, caractйrisй la matrice est du polybutиne.
6-Produit antidйrapant (1), selon la revendication 5, caractйrisй en ce que l'huile une huile de type
silicone.
7-Produit antidйrapant (1), selon la revendication 5, caractйrisй en ce que l'йpaississant est une
silice pyrolysйe.
8-Produit antidйrapant (1), selon la revendication 7, caractйrisй en ce que la composition du
produit peut кtre la suivante :
un polybutиne de poids molйculaire 200 --une huile silicone comme par exemple celle
commercialisйe sous la marque dйposйe Rhodorsil de rйfйrence 47V100000 une charge
constituйe par une charge minйrale comme une solution colloпdale de silice
455/1651
70. FR2837105 - 19.09.2003
SYNERGISTIC MEDICINAL COMBINATION OF PROPOLIS AND LAVENDER ESSENTIAL OIL, E.G.
AS EXTRACT OBTAINED BY MACERATION, USEFUL E.G. FOR TREATING INFECTIONS,
INFLAMMATION, WOUNDS, PAIN OR HEMORRHOIDS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2837105
Inventor(s):
BRINGER JEAN (--)
Applicant(s):
BRINGER JEAN (FR)
IP Class 4 Digits: A61K; A61P
IP Class:
A61K47/44; A61P17/02; A61P25/06; A61P29/00; A61P31/00
E Class: A61K9/00M18D; A61K35/64+M; A61K35/78+M
Application Number:
FR20020003093 (20020313)
Priority Number: FR20020003093 (20020313)
Family: FR2837105
Abstract:
A NATURAL PRODUCT-BASED COMPOSITION (I), FOR USE IN THE PRODUCTION OF MEDICINAL
EXTRACTS, COMPRISES AN ALCOHOL-FREE COMBINATION OF PROPOLIS AND LAVENDER
ESSENTIAL OIL. INDEPENDENT CLAIMS ARE INCLUDED FOR: (1) AN ALCOHOL-FREE LIQUID
EXTRACT (II), OBTAINED FROM (I) (PREFERABLY BY MACERATION); (2) THE PREPARATION OF (I),
BY INTRODUCING 5-20 (ESPECIALLY 12) PARTS PROPOLIS (PREVIOUSLY GROUND TO FINE
POWDER AT 10-15 DEGREES C) INTO A CONTAINER, ADDING LAVENDER OIL TO A TOTAL OF
100 PARTS AND MANUALLY MIXING; AND (3) THE PREPARATION OF (II) BY FORMING (I) AS IN (2)
THEN ALLOWING THE MIXTURE TO MACERATE FOR 1-4 (ESPECIALLY 2.5) MONTHS, FILTERING
THE LIQUID PHASE AND RECOVERING AND STORING THE FILTRATE.
456/1651
71. FR2846231 - 30.04.2004
COSMETIC COMBINATION USEFUL IN COMPOSITIONS FOR TREATING THE HAIR AND/OR SKIN
COMPRISES CLIMBAZOLE AND A PHENOLIC ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=FR2846231
Inventor(s):
MAURIN VERONIQUE (--)
Applicant(s):
HAARMANN REIMER SA (FR)
IP Class 4 Digits: A61K
IP Class:
A61K7/48; A61K7/075
E Class: A61K8/92C; A61Q19/00; A61K8/49F1; A61Q5/02
Application Number:
FR20020013214 (20021023)
Priority Number: FR20020013214 (20021023)
Family: FR2846231
Abstract:
COSMETIC COMBINATION (COMPLEX) COMPRISES CLIMBAZOLE AND A PHENOLIC ESSENTIAL
OIL. AN INDEPENDENT CLAIM IS ALSO INCLUDED FOR A COSMETIC COMPOSITION
COMPRISING THE COMBINATION.Description:
La prйsente invention concerne un complexe cosmйtique comprenant du
climbazole et au moins une huile essentielle d'origine vйgйtale, des compositions cosmйtiques
renfermant ce complexe ainsi que leurs utilisations dans le domaine de la cosmйtique, notamment
pour diminuer, prйvenir et/ou
traiter le regraissage des cheveux.
457/1651
Les shampooings destinйs aux cheveux gras sont gйnйralement des produits trиs dйtergents et
trиs concentrйs en tensio-actifs. Ce sont des produits agressifs, qui dessиchent le cheveu. Ces
shampooings prйsentent de faibles qualitйs d'usage en terme de performances moussantes et
cosmйtiques: ainsi la mousse obtenue est rкche, et des cheveux mouillйs 15 rкches sont des
cheveux difficiles а dйmкler. De plus, les cheveux sйchйs sont secs, cassants, ternes et
manquent de douceur. Les cheveux sont donc abоmйs. Outre d'кtre agressifs pour le cheveu, ces
shampooings agressent йgalement le cuir chevelu. En effet, ils ne respectent pas l'йquilibre du cuir
20 chevelu car ils modifient la flore bactйrienne naturellement prйsente du cuir chevelu. D'autres
shampooings, plus "cosmйtiques", car destinйs aux cheveux normaux а gras, existent йgalement.
Il s'agit de produits а base de tensio-actifs et d'agents conditionneurs du cheveu tels que les
polymиres 25 cationiques et/ou les silicones ou dйrivйs. Nйanmoins, lorsque ces shampooings
sont plus particuliиrement destinйs aux cheveux gras, la composition de ces produits est fondйe
sur un rййquilibrage des constituants habituellement prйsents dans ce type de produits, ce qui
signifie que l'on йquilibre le ratio entre le tensio-actif et les polymиres cationiques et/ou les 30
silicones et dйrivйs. C'est donc par un abaissement du niveau cosmйtique, c'est а dire par une
diminution des agents conditionneurs du cheveu tels que les polymиres cationiques et/ou les
silicones et dйrivйs, que ces produits
destinйs aux cheveux а tendance grasse sont prйparйs. Cependant, ces shampooings
prйsentent l'inconvйnient de ne pas rйpondre aux besoins des cheveux gras. D'autre part, les
agents conditionneurs prйsents dans ces produits peuvent s'accumuler а la surface du cheveu et
ainsi alourdir le cheveu. 5 Ceci se traduit par un aspect plat du cheveu et un graissage plus rapide
des cheveux.
La demanderesse a dйcouvert que l'association du climbazole avec au moins une huile essentielle
d'origine vйgйtale permet d'йviter tout ou
partie des dйsavantages et inconvйnients mentionnйs ci-dessus.
En effet, cette association prйsente les avantages surprenants de pouvoir diminuer, prйvenir ettou
traiter le regraissage des cheveux, tout en
respectant l'йquilibre de la flore bactйrienne du cuir chevelu.
458/1651
Les composйs du complexe cosmйtique de l'invention ne sont pas
dйtergents, sont facilement absorbйs par les cheveux йvitant ainsi leur 15 accumulation а la
surface du cheveu et l'alourdissement de la chevelure.
La prйsente invention a pour premier objet un complexe cosmйtique caractйrisй en ce qu'il
comprend du climbazole et une huile
essentielle monocyclique aromatique de la famille des phйnols.
Selon un mode prйfйrй de l'invention, l'huile essentielle 20 monocyclique aromatique de la famille
des phйnols est un dйrivй du cumиne
comme le thymol.
Selon un autre mode prйfйrй de l'invention, l'huile essentielle monocyclique aromatique de la
famille des phйnols est choisie dans le groupe constituй par Thymus vulgaris (thym), Origanum
compactum (origan), Satureja 25 montana (sarriette), Laurus nobilis (laurier), Rosmarinus officinales
(romarin), Myrtus communes (myrte), Citrus reticulata (mandarine) et Citrus limonum (citronnier).
Le complexe cosmйtique de l'invention comprend de prйfйrence en outre une huile essentielle de
la famille des alcools sesquiterpйniques, de 30 prйfйrence de l'alpha-bisabolol.
L'alpha-bisabolol est notamment utilisй pour son action apaisante. Selon un autre mode prйfйrй
de l'invention, l'huile essentielle de la
famille des alcools sesquiterpйniques est choisie dans le groupe constituй par Matricaria
chamomilla (camomille matricaire), Chamaemelum nobile (camomille romaine), Ormenis mixta
(camomille vulgaire), Citrus bergamia (bergamote), Cymbopognon citratus (verveine des Indes),
Salvia sclarea (sauge scalrйe), 5 Salvia officinalis (sauge officinale), Daucus carota (carotte) et
Santalum album (santal).
Selon un mode prйfйrй de l'invention, le climbazole compris dans
459/1651
le complexe cosmйtique peut reprйsenter de 10 а 40% en poids, par rapport au poids. total du
complexe, de prйfйrence de 15 а 35%, et encore plus 10 prйfйrentiellement 20% environ.
Selon un autre mode prйfйrй de l'invention, l'huile essentielle
monocyclique aromatique de la famille des phйnols comprise dans le complexe cosmйtique peut
reprйsenter de 0,1 а 5% en poids, par rapport au poids total du complexe, de prйfйrence de 0,2 а
3%, et encore plus prйfйrentiellement 15 0,5% environ.
Selon un autre mode prйfйrй de l'invention, l'huile essentielle de la famille des alcools
sesquiterpйniques comprise dans le complexe cosmйtique peut reprйsenter de 5 а 60% en poids,
par rapport au poids total du complexe,
de prйfйrence de 10 а 50%, et plus prйfйrentiellement 40% environ.
Prйfйrentiellement le complexe cosmйtique de l'invention est caractйrisй en ce qu'il comprend
(pourcentage en poids par rapport au poids total du complexe): - 20% environ de climbazole, - 0,5%
environ de thymol et,
- 40% environ d'alpha-bisabolol.
Le complexe cosmйtique est habituellement de couleur incolore а jaune. Il ne prйsente pas
d'odeur particuliиre et prйsente l'avantage d'кtre neutre. Un complexe selon l'invention peut кtre
utilisй pour la prйparation 30 de compositions cosmйtiques, qui constituent un autre objet de la
prйsente invention. La prйsente invention a ainsi pour autre objet une composition
cosmйtique comprenant un complexe cosmйtique tel que dйfini prйcйdemment.
Une composition cosmйtique selon l'invention comporte habituellement, outre ledit complexe
cosmйtique, au moins un ou des agents cosmйtique(s) tel(s) que l'eau, un agent tensioactif
anionique, non ionique et/ou 5 amphotиre, un polymиre anionique, non ionique et/ou amphotиre,
une protйine, un hydrolysat de protйine, une cйramide, un pseudocйramide, un acide gras а
chaоnes linйaires ou ramifiйes, un alphahydroxyacide (AHA), une vitamine, un ester d'acide gras,
une silicone volatile ou non volatile, soluble ou non soluble sous forme d'huile, de gomme, de rйsine
et/ou ses homologues 10 organomodifiйes, un agent hydratant, un agent antipelliculaire, un agent
460/1651
antisйborrhйique, un agent йpaississant, de l'йthanol, un filtre solaire, un agent antibactйrien, un
agent conservateur tel que le butylиneglycol, un parfum, un colorant, un agent anti-oxydant, un
agent rйgulateur de pH, un agent antitranspirant, un agent anti-radicaux libres, un solvant de la
famille des glycols et 15 dйrivйs tel que le propylиneglycol, une huile minйrale, une huile
organique et/ou
une huile de synthиse, un agent nacrant, un agent opacifiant, un agent colorant.
Les agents tensioactifs anioniques peuvent кtre de type sulfate comme les sels (en particulier les
sels alcalins, notamment de sodium, les sels d'ammonium, les sels d'amines, les sels d'aminoalcools
ou les sels de 20 magnйsium) des alkylsulfates, alkylйthersulfates, alkylamidoйthersulfates,
alkylarylйthersulfates ou alkylйthersulfosuccinates. On utilise de prйfйrence un agent tensioactif
anionique choisi parmi les alkyl (C12-14) йthersulfates de sodium, de triйthanolamine ou
d'ammonium oxyйthylйnйs а environ 2,2 moles d'oxyde d'йthylиne. Les agents tensioactifs
anioniques peuvent aussi кtre de type
phosphate, sulfonate et/ou carboxylate comme les alkylsulfonates, alkylphosphates,
alkylamidesulfonates, alkylarylsulfonates, cL-olйfinesulfonates, paraffine sulfonates,
alkylsulfosuccinates, alkylйthersulfosuccinates, alkylamidesulfosuccinates, alkylsulfosuccinamates,
alkylsulfoacйtates, 30 alkylйtherphosphates, acylsarcosinates, acylisйthionates et les Nacyltaurates.
Les agents tensioactifs non ioniques sont prйfйrentiellement des alkylpolyglycosides, notamment
des alkylpolyglucosides.
Les agents tensioactifs amphotиres peuvent кtre, notamment, des dйrivйs secondaires ou
tertiaires aliphatiques, dans lesquels le radical aliphatique est une chaоne linйaire ou ramifiйe
comportant de 8 а 18 atomes de carbone et contenant au moins un groupe anionique
hydrosolubilisant tels qu'un groupe 5 carboxylate, sulfonate, sulfate, phosphate ou phosphonate; ou
des alkyl (C8.20) bйtaines, des alkyl (C8a2o) sulfobйtanes, des alkyl (C8.20) amidoalkyl (C1.6)
bйtanes ou des alkyl (C8 20) amidoalkyl (C1.6) sulfobйtaines.
461/1651
Les polymиres anioniques utilisables peuvent кtre choisis parmi tous ceux dйjа connus en soi
comme amйliorant les propriйtйs cosmйtiques des 10 cheveux traitйs par des compositions
dйtergentes. Ils ont йgalement un rфle
d'agent viscosant, stabilisant et/ou modificateur de rhйologie.
Une composition cosmйtique selon l'invention peut consister notamment en un produit destinй aux
cheveux tel qu'un shampooing, un aprиsshampooing, une crиme conditionnante pour les cheveux,
une crиme 15 dйmкlante pour les cheveux, un gel pour cheveux, une lotion pour cheveux, un
conditionneur capillaire ou tout produit capillaire.
A titre indicatif, on peut notamment citer les shampooings et aprиsshampooings rincйs ou non
rincйs, destinйs а tous types de cheveux (y compris pelliculaires), les lotions alcooliques,
hydroalcooliques ou aqueuses, 20 les produits de coiffage sous toutes leurs formes (spray, gel,
gomme, aйrosol), les produits techniques tels que les permanentes ou les produits de coloration ou
dйcoloration, les produits de maquillage des cheveux etc Une composition cosmйtique selon
l'invention peut йgalement consister en un produit pour l'application sur le visage et/ou le corps tel
qu'une 25 crиme, un lait, une lotion, un gel, un gel crиme, un masque, un sйrum, une huile
et une pommade.
A titre indicatif, on peut citer les produits destinйs au soin ou au traitement du visage pour tous
types de peaux, et notamment pour les peaux а problиmes comme les peaux grasses et/ou
acnйiques, tels que: 30 - les masques purifiants, dйsincrustants, hydratants, - les lotions, laits,
crиmes et huiles dйmaquillantes, hydratantes, tonifiantes, - les gels, laits, crиmes et lotions
moussantes ou non moussantes, rinзables ou non rinзables а l'eau, monophase, bi-, tri- ou
multiphases, - les lingettes,
- les poudres liquides (talc powder par exemple) etc....
Selon un mode prйfйrй de l'invention, le complexe cosmйtique de 5 l'invention reprйsente de
0,01 а 5% en poids, par rapport au poids total de la composition, de prйfйrence de 0,02 а 4%, et
encore plus prйfйrentiellement de
462/1651
0,5 а 2%.
La prйsente invention a йgalement pour objet un procйdй cosmйtique de traitement de la peau
et/ou des cheveux, caractйrisй en ce qu'il 10 consiste а appliquer sur les cheveux et/ou la peau
une composition cosmйtique
telle que dйfinie prйcйdemment.
La prйsente invention a йgalement pour objet l'utilisation d'un complexe cosmйtique ou d'une
composition cosmйtique tels que dйfinis
prйcйdemment, pour le traitement des cheveux et/ou de la peau.
Le complexe ou la composition cosmйtique peut notamment кtre utilisй pour diminuer, prйvenir
et/ou traiter le regraissage des cheveux, pour
rййquilibrer la flore bactйrienne du cuir chevelu.
En outre, le complexe ou la composition cosmйtique de l'invention
prйsente l'avantage d'adoucir et d'apaiser le cuir chevelu, et non seulement de 20 rendre les
cheveux propres, mais aussi de les garder propres plus longtemps.
Les exemples ci-aprиs illustrent l'invention.
EXEM PLES
Exemple 1: Complexe cosmйtique en solution On a prйparй une solution de complexe
cosmйtique de l'invention ayant la composition suivante: - 25% de climbazole, - 3% de thymol, et
- 72% de propyleneglycol.
а partir d'un complexe ayant la composition suivante.
- 25% de climbazole, et
463/1651
- 3% de thymol.
Dans ce qui prйcиde et dans ce qui suit, les pourcentages sont donnйs en poids par rapport au
poids total de la composition.
Exemple 2: Complexe cosmйtique en solution On a prйparй une solution de complexe
cosmйtique de l'invention ayant la composition suivante: - 20% de climbazole, - 0,5%de thymol, 40% d'alpha-bisabolol, et
- 39,5% de propylиneglycol.
Exemple 3: Shampooing nacrй Les diffйrents constituants du shampooing nacrй, ainsi que leurs
proportions (pourcentages en poids) sont les suivants: 15 Laurylethersulfate de sodium (Texapon N
70 -Cognis) 14 Cococamphodiacйtate disodique (Miranol C2M -Rhфne Poulenc) 8
CocoamideDEA (Comperlan 100 - Cognis) 3 Solution de complexe cosmйtique de l'exemple 2 1,5
Distйarate de glycol (Tegin BL 315 - Goldschmidt) 2 Dimйthicone-copolyol (Dow Corning) 0,5
Polyquaternium-10 (Ucar JR 400 Amerchol) 0,4 Parfum 0,5 Conservateurs / Sйquestrants I Tampon
pH Qs Colorants Qs Eau Qsp 100 Qs signifie "quantitй suffisante" Qsp signifie "quantitй suffisante
pour" Exemple 4: Shampooing Laurylethersulfate de sodium (Texapon N 70 -Cognis) 14
Alkylpolyglucoside (Plantacare PS 10 - Cognis) 8 Coco-amidopropylbйtaine (Dйhyton K - Cognis)
8 Solution de complexe cosmйtique de l'exemple 2 1,5 Parfum 0,5 Conservateurs / Sйquestrants /
Tampon pH Qs Colorants Qs Eau Qsp 100 ExE mole 5: ADrиsshamoooina Alcool cйtylique
stйarylique а mole d'oxyde d'йthylиne 2,5 (Lanette O - Cognis) Cйtйareth-20 (Eumulgin B2 Cognis) 0,7 Phosphate ammoniacal d'oxyйthyl alkyle (Quaternium-52 ) 0,5 Solution de complexe
cosmйtique de l'exemple 2 1,5 Parfum 0,5 Conservateurs / Sйquestrants / Tampon pH Qs Colorants
Qs Eau Qsp 100 Exemple 6: Lotion nettoyante & hydratante peaux grasses 1,3-Butylиne Glycol 3
Glycйrine 4 Chlorure de sodium 0,9 Solution de complexe cosmйtique de l'exemple 2 1,5 Parfum
0,5 Conservateurs / Sйquestrants / Tampon pH Qs Colorants Qs Eau Qsp 100 Exemple 7: crиme а
effet d'hydratation naturelle Triglycйride caprylique/caprique 13 Cocoate йthyl hexylique 3 Esters
cйthyliques 3 Alcool cйtйarylique 3 Stйarate de sorbitanne 2 Glycйrine 3 Solution de complexe
cosmйtique de l'exemple 2 1,5 Parfum 0,5 Conservateurs / Sйquestrants / Tampon pH Qs Colorants
Qs Eau Qsp 100 Exemple 8: Lotion йmolliente hydratante Alcool de lanoline 1,25 Huile minйrale 35
Vaseline pure 4,20 Acide stйarique 1,60 Polawax GP200 0,83 Glycйrine 0,83 Climbazole 0,1 Citrus
Reticulata (Huile essentielle de mandarine - Agipal) 0,001 Salvia Officinalis (Huile essentielle de
464/1651
sauge Scarlйe - Agipal) 0, 1 Parfum 0,5 Conservateurs / Sйquestrants / Tampon pH Qs Colorants
Qs Eau Qsp 100 Exemple 9: Shampooing On a prйparй un shampooing ayant la composition
suivante: Phase Ingredients - fournisseurs Pourcentages B Laurylethersulfate de sodium 45 B CocoBйtane 8 C Cocamide MEA 1,5 A Polyquaternium-10 (Ucar Polymer JR-400 - National Starch) 0,25 D
Parfum 0, 5 D Huile de ricin hydrogйnйe 0,5 E Solution de complexe cosmйtique de l'exemple 2 1
E Methyl paraben de sodium 0,3 E DMDM Hydantoin (GlydantLonza) 0,2 F Acide citrique 0,5 G1
Acide citrique jusqu'а pH 7 G2 Hydroxyde de sodium jusqu'а pH 7 Eau desionisйe 41,7 Procйdй
de fabrication: La phase A est dispersйe dans l'eau et chauffйe а 75-80 C. On
mйlange jusqu'а la solubilisation complиte. On ajoute sйparйment les ingrйdients de la phase B,
puis celui de la phase C. On ajoute, а 40 C, les ingrйdients des phases D, E et F. On ajuste ensuite
le pH en ajoutant les 10 ingrйdients des phases G1 et G2, si nйcessaire pour obtenir un pH de 7 +
0,5.
Exemple 10:Test dйmontrant l'effet anti-regraissage des cheveux du shampooing de l'exemple 9
L'effet anti-regraissage de la composition de l'exemple 8 a йtй 15 йvaluй dans un test in vivo en
double aveugle.
Le test est rйalisй sur deux groupes de 15 sujets вgйs entre 18 et
ans а type de peau caucasien.
On procиde а un examen clinique du cuir chevelu des patients il arrivйs sans s'кtre lavй les
cheveux et on dйtermine des zones de mesure sur
le cuir chevelu.
On mesure ensuite le taux de sйbum du cuir chevelu а l'aide d'un
sйbumиtre et on prйlиve une mиche de cheveux.
Dиs le dйbut du test (Jl), les sujets se lavent les cheveux avec, d'une part le shampooing de
l'exemple 8 (Groupe 1) et, d'autre part, un placebo
465/1651
(Groupe 2).
Immйdiatement aprиs le shampooing puis aprиs 4 H, 8 H et 24 H on procиde aux opйrations
suivantes: 10 - mesure avec sйbumиtre, - prйlиvement d'une autre mиche de cheveux, extraction des lipides du cheveu en milieu йthanolique, - йvaporation du milieu - coloration
fluorescente des lipides а l'aide du colorant "NILE RED" - lecture de la fluorescence а l'aide d'un
appareil FLUOROSCAN 2 de LAB
SYSTEM aprиs excitation а 485 nm et lecture а 538 nm.
Entre J2 et J20 les sujets se lavent les cheveux trois fois par
semaine avec les produits а tester.
A J21, les sujets ne se sont pas lavй les cheveux et on mesure le 20 taux de sйbum avec le
sйbumиtre sur les zones dйfinies au premier jour du test, on procиde а un examen du cuir chevelu,
et on soumet aux sujets un
questionnaire d'йvaluation subjective.
Les rйsultats sont les suivants: Effet de sebo-regulation Aprиs 21 jours de test (3 shampooings par
semaine) un effet de sйbo-rйgulation a йtй observй sur 47 % des volontaires ayant testй le
shampooing de l'exemple 8.
Analyse des lipides du cheveu A 24 H, le regraissage йtait complet avec le placebo alors que le
shampooing de l'exemple 8 йvite le complet regraissage des cheveux.Claims:
REVENDICATIONS
1. Complexe cosmйtique caractйrisй en ce qu'il comprend du climbazole et une huile essentielle
monocyclique aromatique de la famille des phйnols. 2. Complexe cosmйtique selon la
revendication 1 caractйrisй en ce qu'il comprend en outre une huile essentielle de la famille des
alcools sesquiterpйniques. 3. Complexe cosmйtique selon la revendication 1 ou la 10 revendication
2 caractйrisй en ce que l'huile essentielle monocyclique aromatique de la famille des phйnols est
466/1651
un dйrivй du cumиne comme le thymol. 4. Complexe cosmйtique selon la revendication 1 ou la
revendication 2 caractйrisй en ce que l'huile essentielle monocyclique 15 aromatique de la famille
des phйnols est choisie dans le groupe constituй par Thymus vulgaris (thym), Origanum
compactum (origan), Satureja montana (sarriette), Laurus nobilis (laurier), Rosmarinus officinalis
(romarin), Myrtus
communis (myrte), Citrus reticulata (mandarine) et Citrus limonum (citronnier).
5. Complexe cosmйtique selon l'une des revendications 2 а 4 20 caractйrisй en ce que l'huile
essentielle de la famille des alcools
sesquiterpйniques est de l'alpha-bisabolol.
6. Complexe cosmйtique selon l'une des revendications 2 а 4
caractйrisй en ce que l'huile essentielle de la famille des alcools sesquiterpйniques est choisie
dans le groupe constituй par Matricaria 25 chamomilla (camomille matricaire), Chamaemelum nobile
(camomille romaine), Ormenis mixta (camomille vulgaire), Citrus bergamia (bergamote),
Cymbopognon citratus (verveine des Indes), Salvia sclarea (sauge scalrйe), Salvia officinalis (sauge
officinale), Daucus carota (carotte) et Santalum album (santal). 7. Complexe cosmйtique selon l'une
quelconque des
revendications 1 а 6 caractйrisй en ce que:
- le climbazole reprйsente de 10 а 40% en poids, par rapport au poids total du complexe, et l'huile essentielle monocyclique aromatique de la famille des phйnols
reprйsente de 0,1 а 5% en poids, par rapport au poids total du complexe.
8. Complexe cosmйtique selon l'une quelconque des 5 revendications 2 а 7 caractйrisй en ce
que l'huile essentielle de la famille des alcools sesquiterpйniques reprйsente de 5 а 60% en poids,
par rapport au
poids total du complexe.
467/1651
9. Complexe cosmйtique selon l'une quelconque des
revendications 1 а 8 caractйrisй en ce qu'il comprend (pourcentage en poids 10 par rapport au
poids total du complexe):
- 20% environ de climbazole, - 0,5% environ de thymol et,
- 40% environ d'alpha-bisabolol.
10. Composition cosmйtique caractйrisйe en ce qu'elle 15 comprend un complexe cosmйtique
tel que dйfini а l'une quelconque des
revendications 1 а 9.
11. Composition cosmйtique selon la revendication 10 caractйrisйe en ce qu'elle comprend en
outre au moins un ou des agent(s) cosmйtique(s) choisi(s) parmi l'eau, un agent tensioactif
anionique, non ionique 20 et/ou amphotиre, un polymиre anionique, non ionique et/ou amphotиre,
une protйine, un hydrolysat de protйine, une cйramide, un pseudocйramide, un acide gras а
chaоnes linйaires ou ramifiйes, un alphahydroxyacide (AHA), une vitamine, un ester d'acide gras,
une silicone volatile ou non volatile, soluble ou non soluble sous forme d'huile, de gomme, de rйsine
et/ou ses homologues 25 organomodifiйes, un agent hydratant, un agent antipelliculaire, un agent
antisйborrhйique, un agent йpaississant, de l'йthanol, un filtre solaire, un agent antibactйrien, un
agent conservateur tel que le butylиneglycol, un parfum, un colorant, un agent anti-oxydant, un
agent rйgulateur de pH, un agent antitranspirant, un agent anti-radicaux libres, un solvant de la
famille des glycols et 30 dйrivйs tel que le propylиneglycol, une huile minйrale, une huile
organique et/ou
une huile de synthиse, un agent nacrant, un agent opacifiant, un agent colorant.
12. Composition cosmйtique selon l'une quelconque des
revendications 10 et 11, caractйrisйe en ce qu'elle consiste en un produit destinй aux cheveux tel
qu'un shampooing, un aprиs-shampooing, une crиme conditionnante pour les cheveux, une crиme
dйmкlante pour les cheveux, un gel pour cheveux, une lotion pour cheveux, un conditionneur
capillaire ou tout
468/1651
produit capillaire. 13. Composition cosmйtique selon l'une quelconque des
revendications 10 et 11, caractйrisйe en ce qu'elle consiste en un produit pour l'application sur le
visage et/ou le corps tel qu'une crиme, un lait, une lotion, un
gel, un gel crиme, un masque, un sйrum, une huile et une pommade.
14. Composition cosmйtique selon l'une quelconque des
revendications 10 а 13, caractйrisйe en ce que le complexe cosmйtique
reprйsente de 0,01 а 5% en poids, par rapport au poids total de la composition.
15. Procйdй cosmйtique de traitement de la peau et/ou des
cheveux, caractйrisй en ce qu'il consiste а appliquer sur les cheveux et/ou la 15 peau un
complexe cosmйtique tel que dйfini а l'une des revendications 1 а 9 ou
une composition cosmйtique telle que dйfinie а l'une quelconque des
revendications 10 а 14.
16. Utilisation d'une composition cosmйtique telle que dйfinie а l'une quelconque des
revendications 10 а 14, pour le traitement des cheveux 20 et/ou de la peau.
17. Utilisation selon la revendication 16 pour diminuer, prйvenir et/ou traiter le regraissage des
cheveux.
18. Utilisation selon la revendication 16 pour rййquilibrer la flore bactйrienne du cuir chevelu.
469/1651
72. GB1130230 - 09.10.1968
A METHOD FOR PREPARING AN ESSENTIAL OIL OF TURPENTINE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=GB1130230
Applicant(s):
FARMO CHIMICA DOTT E CORVI FAR (--)
E Class: C11B9/02B; C07C45/78
Application Number:
GB19670042381 (19670918)
Priority Number: IT19660022405 (19660929)
Family: GB1130230
Equivalent:
IT1056707
Abstract:
1,130,230. MODIFYING TURPENTINE. FARMO- CHIMICA DOTT. E. CORVI "FARDECO" S.P.A. 18
SEPT., 1967 [29 SEPT., 1966], NO. 42381/67. HEADING C5C. ESSENTIAL OIL OF TURPENTINE IS
SUBJECTED TO OXIDATION BY BLOWING IN AIR AND THE ACTION OF U.V. RADIATION, THE
PRODUCTS ARE VACUUM DIS- TILLED AND THE FRACTION DISTILLING AT 55-75 C. UNDER 10
MM. HG. PRESSURE IS COLLECTED IN A CONTAINER COOLED TO ABOUT -20 C. THE PRODUCT
CONTAINS OXIDATION PRODUCTS SUCH AS KETONES, ALCOHOLS AND TERPENE OXIDES AND
IS IN THE FORM OF A YELLOW-GREENISH OIL HAVING A CAMPHOREOUS ODOUR AND A
DENSITY OF 0А92-0А96 G./C.C.Description:
COMPLETE SPECIFICATION
A method for preparing all Essential Oil of Turpentine
We, FARMO-CHIMICA DOTT. E. CORVI "FARDECO" S.p.A., a Company organised and existing
under the laws of Italy, of Via G.
470/1651
Morigi 45, Piacenza (Italy), do hereby declare the invention, for which we pray that a patent may be
granted to us, and the method by which it is to be performed, to be particularly described in and by
the following statement:
This invention is concerned with the preparation of a particularly pure essential oil of turpentine.
It is already known from literature that since 1939 researches have been carried out by various
French Authors, such as Patron,
Desdrosier, Joltrain and Caillon, on the oxidation products of turpentine oil, which products show
particularly desirable properties (in particular from a therapeutic standpoint, especially for treating
respiratory apparatus diseases).
In addition, F. A. Sauvage has disclosed an ozonizing process of turpentine oil by exposure to the
air and light, and subsequent fractional distillation of the products; and the Societe de Financement
et d'Exploitation de Marques (Societe Anonyme) obtains water-soluble terpene oxides from
turpentine oil air oxidated to the light and subsequent fractional distillation of the products.
It has now been found that so-called "Beta
Terpenes" products may be obtained from essential oil of pure turpentine, these products being
formed of ketones, alcohols and terpene oxides, which show particularly desirable properties,
especially for a subsequent processing to pharmaceutic products.
The method according to the invention for obtaining the above-mentioned products develops
according to the following steps:
a) Blowing in of air into the essential oil of turpentine under the action of ultraviolet rays;
bj Vacuum distillation of the products in a proper rectifier;
c) Cooling at -200C of the collected products.
The product according to the present invention corresponds to the fractions distilling between 550
and 750C at 10 mm.; it is in the form of a yellow greenish oil, having a bitter caustic taste, a
camphoreous odour and a density from 0.92 to 0.96 g/cc.
For a better understanding of the present invention, a preferred embodiment of the method
according to the invention will be hereinafter described:
EXAMPLE 20 liters of essential oil of turpentine are introduced into suitable capsules of a capacity of
30 liters. Then air is blown in, at a rate of 20 liters per minute, simultaneously subjecting the contents
471/1651
of the capsule to the action of ultraviolet rays. The operation is continued for six days. Thereafter the
oxidated liquid is supplied to a vacuum rectifier, provided with a condenser and a cooler, having a
suitable rectifying column. Therefrom, the fractions distilling between 550 and 750C at 10 mm. are
collected at -200C within two containers provided with a suitable cooling.
The product is a yellow greenish oil, having a bitter caustic taste and a comphoreous odour and a
density from 0.92 to 0.96 g/cc.
The yield is of 5 liters for each capsule.
WHAT WE CLAIM IS:1.- A method for preparing essential oils of turpentine, characterized in that the commercially
available pure essential oil of turpentine is subjected to oxidation by air blowing in and under the
action of ultraviolet rays, the products are vacuum distilled and the fractions distilling between 550
and 750C at 10 mm.
are collected within containers cooled at about -200C.
2.-- Essential oil of turpentine obtained according to the method of Claim 1, characterized by
containing oxidation products, such as ketones, alcohols and terpene oxides.
**WARNING** end of DESC field may overlap start of CLMS **.
Claims:
**WARNING** start of CLMS field may overlap end of DESC **.
COMPLETE SPECIFICATION
A method for preparing all Essential Oil of Turpentine
We, FARMO-CHIMICA DOTT. E. CORVI "FARDECO" S.p.A., a Company organised and existing
under the laws of Italy, of Via G.
472/1651
Morigi 45, Piacenza (Italy), do hereby declare the invention, for which we pray that a patent may be
granted to us, and the method by which it is to be performed, to be particularly described in and by
the following statement:
This invention is concerned with the preparation of a particularly pure essential oil of turpentine.
It is already known from literature that since 1939 researches have been carried out by various
French Authors, such as Patron,
Desdrosier, Joltrain and Caillon, on the oxidation products of turpentine oil, which products show
particularly desirable properties (in particular from a therapeutic standpoint, especially for treating
respiratory apparatus diseases).
In addition, F. A. Sauvage has disclosed an ozonizing process of turpentine oil by exposure to the
air and light, and subsequent fractional distillation of the products; and the Societe de Financement
et d'Exploitation de Marques (Societe Anonyme) obtains water-soluble terpene oxides from
turpentine oil air oxidated to the light and subsequent fractional distillation of the products.
It has now been found that so-called "Beta
Terpenes" products may be obtained from essential oil of pure turpentine, these products being
formed of ketones, alcohols and terpene oxides, which show particularly desirable properties,
especially for a subsequent processing to pharmaceutic products.
The method according to the invention for obtaining the above-mentioned products develops
according to the following steps:
a) Blowing in of air into the essential oil of turpentine under the action of ultraviolet rays;
bj Vacuum distillation of the products in a proper rectifier;
c) Cooling at -200C of the collected products.
The product according to the present invention corresponds to the fractions distilling between 550
and 750C at 10 mm.; it is in the form of a yellow greenish oil, having a bitter caustic taste, a
camphoreous odour and a density from 0.92 to 0.96 g/cc.
For a better understanding of the present invention, a preferred embodiment of the method
according to the invention will be hereinafter described:
473/1651
EXAMPLE 20 liters of essential oil of turpentine are introduced into suitable capsules of a capacity of
30 liters. Then air is blown in, at a rate of 20 liters per minute, simultaneously subjecting the contents
of the capsule to the action of ultraviolet rays. The operation is continued for six days. Thereafter the
oxidated liquid is supplied to a vacuum rectifier, provided with a condenser and a cooler, having a
suitable rectifying column. Therefrom, the fractions distilling between 550 and 750C at 10 mm. are
collected at -200C within two containers provided with a suitable cooling.
The product is a yellow greenish oil, having a bitter caustic taste and a comphoreous odour and a
density from 0.92 to 0.96 g/cc.
The yield is of 5 liters for each capsule.
WHAT WE CLAIM IS:1.- A method for preparing essential oils of turpentine, characterized in that the commercially
available pure essential oil of turpentine is subjected to oxidation by air blowing in and under the
action of ultraviolet rays, the products are vacuum distilled and the fractions distilling between 550
and 750C at 10 mm.
are collected within containers cooled at about -200C.
2.-- Essential oil of turpentine obtained according to the method of Claim 1, characterized by
containing oxidation products, such as ketones, alcohols and terpene oxides.
3.-- Essential oil of turpentine obtained according to the method of Claim 1, characterized by being
in the form of a yellow greenish oil, having a bitter caustic taste, a camphoreous odour and a density
from 0.92 to 0.96 g/cc.
4.- A method of preparing essential oils of turpentine substantially as hereinbefore described.
5.-- Essential oil of turpentine obtained according to the method of Claim 1 or Claim 4.
474/1651
73. GB1402744 - 13.08.1975
CARRIER FOR ESSENTIAL OIL COMPOSITION AND METHOD OF MAKING ESSENTIAL OIL
COMPOSITION EMBODYING SAME
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=GB1402744
Applicant(s):
BECK E E (--)
IP Class 4 Digits: A23L
IP Class:
A23L1/222; A23L2/00; A23L1/10
E Class: A23L1/222; A23L1/22B; A23L1/22B8
Application Number:
GB19720044707 (19720927)
Priority Number: GB19720044707 (19720927)
Family: GB1402744
Abstract:
1402744 FLAVOURING CARRIERS E E BECK 27 SEPT 1972 44707/72 HEADING A2B A CARRIER
COMPOSITION FOR ESSENTIAL OILS COMPRISES HYDROLYSED CEREAL SOLIDS, E.G. CORN,
HAVING A DEXTROSE EQUIVALENT (D.E.) OF LESS THAN 20, AND A SUGAR, E.G. SUCROSE,
AND IS IN THE FORM OF ROD-LIKE PARTICLES, AND HAS AN INERT ANTI-CAKING AGENT MIXED
THEREWITH. THE COMPOSITION IS MADE BY MIXING AND HEATING THE SUGAR AND
HYDROLYSATE TO 122 C IN A TANK 10 WITH AN EMULSIFYING AGENT, E.G. MONO- AND DIGLYCERIDES OF NA SULPHOACETATE, MIXING AN ESSENTIAL OIL AND AN ANTIOXIDANT E.G.
BUTYLATED HYDROXYANISOLE (BHA) OR BUTYLATED HYDROXY- TOLUENE (BHT) IN A
SECOND TANK 13, AND TRANSFERRING BOTH MIXTURES TO AN EMULSIFICA- TION TANK 12
AND THEN BY AIR PRESSURE (60- 100 PSIG) TO AN EXTRUDER 15 HAVING 1/64" ORIFICES. THE
COMBINED MIX IS EXTRUDED INTO A TANK 16 CONTAINING ISOPROPANOL WHICH SOLIDIFIES
THE EXTRUDATE AND IS THEN AGITATED TO BREAK UP THE EXTRUDED RODS TO THE DESIRED
SIZE AND TO REMOVE EXCESS OILS THEREFROM. THE RODS ARE THEN CENTRIFUGED, MIXED
475/1651
WITH ABOUT 0.5% BY WT. OF ANTI-CAKING AGENT E.G. A SILICA POWDER (PREFERABLY
PYROGENIC SILICA), SCREENED AND DRIED AT ABOUT 100 F. ALTERNATIVELY THE ANTICAKING AGENT MAY BE ADDED TO THE ISOPROPANOL BEFORE EXTRUSION. THE OIL
CONTENT CARRIED BY THE COMPOSITION IS 0.1-10%, PREFERABLY 8-10%. PARTICLE SIZE IS
20 MESH OR FINER. OILS WHICH CAN BE USED ARE CITRUS, E.G. ORANGE. ANIS,
WINTERGREEN OR SPEARMINT. ARTIFICIAL SWEETENERS SUCH AS SACCHARIN MAY BE
ADDED. INSTEAD OF SUCROSE, DEXTROSE OR LAEVULOSE MAY BE INCLUDED.Description:
(54) CARRIER FOR ESSENTIAL OIL COMPOSITION AND
METHOD OF MAKING ESSENTIAL OIL COMPOSITION
EMBODYING SAME
(71) 1, EUGENE EMORY BECK, a citizen of the United States of America, of 207
Summit View Drive, Calimesa, California,
United States of America, 92320, do hereby declare the invention, for which I pray that a patent may
be granted to me, and the method by which it is to be performed, to be particularly described in and
by the following statement::
This invention relates to a carrier composition for essential oils in relatively stable, non-crystallizable
particulate form, which can have a high content of essential oils for use as solid essential oil
flavouring compositions in the preparation of beverage products, including dehydrated
compositions containing essential oils and suitable for reconstitution as beverages or for use in the
flavouring of pastries and other food products.
One of the features of my invention is the use of a hydrolyzed central product having a
comparatively low dextrose equivalent (DE), below 20 and, in general, between about 10 and 15.
Such a hydrolyzed cereal product even when made from corn is not, technically speaking, properly
designated as "corn syrup solids", since the latter have a DE of at least 20, and generally
considerably higher, with a
correspondingly sweet taste, as compared with the bland taste of the hydrolyzed cereal product
used in my composition. Such a low DE cereal hydrolysate has itself no tendency to crystallize upon
long standing, nor will the addition thereto of sucrose impart to the composition a tendency to
crystallize to any objectionable extent.This is in contrast to the crystallizing tendency that sugar
would impart to what are properly termed "corn syrup solids", as disclosed, for instance, in
United States Patents Nos. 2,809,895 and 3,041,180.
476/1651
Another feature of my carrier composition for essential oils is that it is in a finely divided, rod-like,
particulate form, having on the surfaces thereof a powdered anticaking agent, such as a pyrogenic
silica, to prevent any tendency of the rod-like particles to stick together.
The invention also provides a method of making a carrier composition for an essential oil which
comprises forming a hot melt of a sugar, an emulsifying agent and a cereal solids hydrolyzate having
a dextrose equivalent of less than 20, extruding the said melt into rod-like form, and admixing an inert
anticaking agent with the rod-like extrudates. The essential oil can be incorporated in the
composition during the performance of the method, preferably by taking a homogeneous emulsion,
in the form of a melt having a boiling point of about 122"C., comprising sucrose, hydrolyzed cereal
solids and an emulsifier, cooling it first to about 114 C.
during the mixing therewith of an essential oil, and then extruding the resulting melt into a relatively
cool liquid solvent, such as isopropanol to form the melt into rods. The isopropanol is kept agitated to
break up the rods into the desired lengths and to wash off the exposed oil from the surface of the
rods.
Subsequently, the rods are subjected to centrifugal action to remove the solvent prior to final drying
and screening. Preferably, finely divided silica is added to the rod-like, particulate mass ahead of the
final drying and screening process so that the fines, both of the composition itself and of the siliceous
material, are screened out of the final product before packaging thereof.
The invention will now be described further by way of example with reference to the drawing which
constitutes a block-type flow diagram of the method of preparing a carrier incorporating an essential
oil composition in accordance with a preferred form of my invention.
in the drawing, the reference numeral 10 indicates a tank into which water, sucrose and hydrolyzed
cereal solids are charged.
The tank 10 is provided with heating and agitating means to effect the steps of cooking and mixing.
An emulsifying agent is introduced through a line 22 into the tank 10 during the operations carried
out therein, at the completion of which the resulting melt is transferred by a pump 11 into an
emulsifier tank 12. The transfer may also be effected by gravity.
477/1651
In a second flow stream, an essential oil and a suitable anti-oxidant are charged into a closed mixing
tank 13. The mixture in the tank 13 is then transferred by a pump 14 to the emulsifier tank 12
Alternatively, air introduced under pressure into said tank 13 through a line (not shown) can serve to
transfer the resulting mix from the tank 13 into the emulsifier tank 12.
By way of example, the mixture of material in the tank 10 comprises the following:
400 ml of distilled water
6840 grams of sucrose (containing about
0.1to moisture)
5160 grams of hydrolyzed cereal solids,
10-13 DE
This mixture is agitated in the tank 10 and heated until the boiling point of the mixture reaches about
122"C, when heating is stopped. The resulting melt is agitated and 240 grams of an emulsifier, such
as a mixture of mono- and di-glycerides of sodium sulphoacetate are introduced through the line 22
into the melt, or any of the other emulsifiers or dispersing agents listed in the United
States Patent No. 3,041,180, can be used.
After the melt in the tank 10 has reached a boiling point of about 1220C, thereby lowering the water
content to the desired minimum, the heating of the melt is stopped and the melt pumped into the
emulsifier tank 12.
The amount of essential oil introduced into the mixing tank 13 is 1247 ml, plus a small amount, 0.5%
by weight, of an anti-oxidant such as butylated hydroxyanisole. This is added, at ambient
temperature to the melt in the closed emulsifier tank 12 by means of the pump 14. As mentioned
previously. alternatively the transfer can be effected by means of air introduced under pressure into
the tank 13 through a line (not shown). The melt and essential oil are intimately mixed under high
agitation. The combined mix is continuously forced from the emulsifier tank 12 through an extruder
15 under air pressure.
The extruder has a head provided with a large number of 1 164th inch diameter orifices through
which the combined mix is forced under 60 to 100 psig air pressure.
From the extruder 15, the extruded material is discharged into a vessel 16 containing a suitable
liquid solvent for the essential oil, such as isopropanol. The liquid solvent is drawn from a tank 17 into
the tank 16 at a temperature such as to effect solid fication of the extruded melt.
478/1651
After solidification, the extruded rods are subjected, in the tank 16, to agitation in the isopropanol at 200C to 23"C to wash off the excess surface oil. The tank 16 also includes a motor-driven impeller
with blades (not shown) that serve both as an agitator and also to break up the extruded rods to the
desired lengths.
From the tank 16, the broken-up rods are separated from a major portion of the liquid solvent by a
settling or draining action, and the broken-up rods are then charged into a centrifuge 18 to remove
most of the liquid solvent, the solvent being discharged from the centrifuge into the solvent tank 17.
The particulate, rod-like solids from the centrifuge 18 are discharged into a mixer 19, into which is
also charged an anticaking agent. The preferred anticaking agent is siliceous material, preferably
pyrogenic silica, of a particle size comparable to that desired in the final essential oil composition.
As shown in the drawing, the anticaking agent is incorporated into the melt mix prior to drying and
screening, but can be added to the liquid solvent prior to extrusion or can be added to the rod-like
particles after the centrifuging step in the centrifuge 18.
After mixing of the preferred anticaking agent, pyrogenic silica, in the mixer 19, drying is
accomplished in a screening and/or drying device 20. The drying and screening may be
accomplished by the use of screens as the supporting surface during the drying operation.
In the latter case, the rod-like particles are moved over a screen, or preferably a series of
successively smaller mesh size screens in the device 20, while at the same time drying of the
particles is accomplished either with ambient air or with warm air passed through andior over the
surfaces of the screens.
From the screen-dryer device 20. the undersized rod-like particles and the excess of fine anticaking
agent are discharged through the screens while the oversized rodlike particles are discharged over
the ends of the screens. Particle sizing is thus accomplished at the same time as the particles are
being dried. The efficiency of the drying operation can be increased by the use of a closed system
and a reduced pressure, but, in general, temperatures of not greatly over 100"F are preferred for use
in the drying operation.
479/1651
From the screens in device 20, the suitably dried and screened essential oil composition is
conveyed to a packing station 21.
The finished product contains an amount of essential oil equivalent to about 8 to 10% of oil by weight
of the finished product, The product has good keeping properties in that it will not crystallize upon
long standing, nor is it subject to substantial deterioration if suitably packaged and protected by
antioxidants. The use of about 0.5% by weight of the final composition of anticaking agent such as
pyrogenic silica powder effectively prevents the rod-like particles of the composition from sticking
together upon long standing in a packaged condition and, also, of course, facilitates the transfer of
the composition from the packages to the points of actual use of the composition.
In place of sucrose, various simple sugars having a desirable sweetening effect, such as dextrose
or levulose, may be used. In that case, somewhat lower melt points than those corresponding to a
boiling point of about 122"C will prove necessary.
Other anti-oxidants than butylated hydroxyanisole (BHA), such as butylated hydroxytoluene (BIlT)
can be used. Also while citrus essential oils, such as orange, are more popular than other essential
oils, the composition of my invention can be used as a carrier for anise, oil of wintergreen, spearmint
oil, and any other relatively volatile, palatable essential oils. The essential oils are present in the final
product within the range of from 0.1% to 12% by weight, and preferably from 8 to 10%.
In order to sweeten the final product, artificial sweeteners such as saccharin can be employed,
together with citric or other fruit acid as a supplement for household use.
In place of isopropanol, other liquid solvents, such as ethanol (denatured), may be used to remove
the excess essential oil left on the surfaces of the rod-like particles of my essential oil composition.
The final product of my invention has the advantage of being non-deliquescent, free-flowing, and
stable without crystallizing tendencies over a prolonged shelf life. In general, the rod-like particles
are all of about 20 mesh size (U.S.
standard) or finer.
WHAT I CLAIM IS:1. A particulate carrier composition for essential oils comprising rod-like particles of a homogenized
emulsion of sucrose and hydrolyzed cereal solids, said solids having a dextrose equivalent of less
480/1651
than 20, and an inert anticaking agent in admixture with said rod-like particles and reducing the
tendency of said particles to stick together.
2. A carrier composition according to claim 1 wherein said anticaking agent is present in the final
composition in an amount equivalent to 0.5% by weight of said composition.
3. A carrier composition according to any one preceding claim and further including 8 to 10% by
weight essential oil.
4. A method of making a carrier composition for an essential oil which comprises forming a
homogenised hot melt of a sugar, an emulsifying agent and a cereal solids hydrolyzate having a
dextrose equivalent of less than 20, extruding the said melt into rod-like form, and admixing an inert
anticaking agent with the rod-like extrudates.
5. A method as defined in claim 4 wherein said extruded melt is broken up into rod-like particles and
screened to eliminate fines and oversize particles.
6. A method as defined in claim 5 wherein the anticaking agent is a pyrogenic silica powder mixed
with said extruded melt prior to screening in a proportion of 0.5to by weight.
7. A method of preparing a particulate essential oil composition, which comprises: agitating and
boiling an aqueous mixture of sucrose, hydrolyzed cerial solids having a dextrose equivalent of less
than 20, and an emulsifier until the resulting emulsion is at a boiling point of about 122cm; cooling
said emulsion to about 114"C while mixing therewith an essential oil in the presence of a sufficient
amount of an emulsifier to form a homogeneous melt; extruding said melt into an agitated liquid
solvent at a sufficiently low temperature to form said melt into solid rods, to break up the rods into the
desired lengths and to wash off the exposed oil from the surface of said rods; subsequently
subjecting said rods to centrifugal action to. remove said solvent therefrom; and prior to final drying
thereof adding to said rods inert anticaking agent and screening said brokenup rods in the presence
of said anticaking agent.
8. A method as defined in claim 7 wherein said cereal solids are hydrolyzed corn solids having a
dextrose equivalent of between 10 and 15.
9. A method as defined in claim 8 wherein said liquid solvent is isopropanol.
481/1651
10. A method as defined in claim 8 or 9 wherein an excess of a pyrogenic silica is added as the
anticaking agent to said rods prior to final screening and drying and a quantity of silica is removed
during final screening and drying to leave sufficient silica in the product to prevent the particulate
rods from sticking together.
11. A method as defined in claim 11 or
12 wherein said rods are subjected to agitation in the isopropanol solvent to break up the rods and
the broken-up rods and isopropanol associated therewith are subjected to centrifuging to remove
the isopropanol.
**WARNING** end of DESC field may overlap start of CLMS **.
Claims:
**WARNING** start of CLMS field may overlap end of DESC **.
nor is it subject to substantial deterioration if suitably packaged and protected by antioxidants. The
use of about 0.5% by weight of the final composition of anticaking agent such as pyrogenic silica
powder effectively prevents the rod-like particles of the composition from sticking together upon long
standing in a packaged condition and, also, of course, facilitates the transfer of the composition from
the packages to the points of actual use of the composition.
In place of sucrose, various simple sugars having a desirable sweetening effect, such as dextrose
or levulose, may be used. In that case, somewhat lower melt points than those corresponding to a
boiling point of about 122"C will prove necessary.
Other anti-oxidants than butylated hydroxyanisole (BHA), such as butylated hydroxytoluene (BIlT)
can be used. Also while citrus essential oils, such as orange, are more popular than other essential
oils, the composition of my invention can be used as a carrier for anise, oil of wintergreen, spearmint
oil, and any other relatively volatile, palatable essential oils. The essential oils are present in the final
product within the range of from 0.1% to 12% by weight, and preferably from 8 to 10%.
482/1651
In order to sweeten the final product, artificial sweeteners such as saccharin can be employed,
together with citric or other fruit acid as a supplement for household use.
In place of isopropanol, other liquid solvents, such as ethanol (denatured), may be used to remove
the excess essential oil left on the surfaces of the rod-like particles of my essential oil composition.
The final product of my invention has the advantage of being non-deliquescent, free-flowing, and
stable without crystallizing tendencies over a prolonged shelf life. In general, the rod-like particles
are all of about 20 mesh size (U.S.
standard) or finer.
WHAT I CLAIM IS:1. A particulate carrier composition for essential oils comprising rod-like particles of a homogenized
emulsion of sucrose and hydrolyzed cereal solids, said solids having a dextrose equivalent of less
than 20, and an inert anticaking agent in admixture with said rod-like particles and reducing the
tendency of said particles to stick together.
2. A carrier composition according to claim 1 wherein said anticaking agent is present in the final
composition in an amount equivalent to 0.5% by weight of said composition.
3. A carrier composition according to any one preceding claim and further including 8 to 10% by
weight essential oil.
4. A method of making a carrier composition for an essential oil which comprises forming a
homogenised hot melt of a sugar, an emulsifying agent and a cereal solids hydrolyzate having a
dextrose equivalent of less than 20, extruding the said melt into rod-like form, and admixing an inert
anticaking agent with the rod-like extrudates.
5. A method as defined in claim 4 wherein said extruded melt is broken up into rod-like particles and
screened to eliminate fines and oversize particles.
6. A method as defined in claim 5 wherein the anticaking agent is a pyrogenic silica powder mixed
with said extruded melt prior to screening in a proportion of 0.5to by weight.
483/1651
7. A method of preparing a particulate essential oil composition, which comprises: agitating and
boiling an aqueous mixture of sucrose, hydrolyzed cerial solids having a dextrose equivalent of less
than 20, and an emulsifier until the resulting emulsion is at a boiling point of about 122cm; cooling
said emulsion to about 114"C while mixing therewith an essential oil in the presence of a sufficient
amount of an emulsifier to form a homogeneous melt; extruding said melt into an agitated liquid
solvent at a sufficiently low temperature to form said melt into solid rods, to break up the rods into the
desired lengths and to wash off the exposed oil from the surface of said rods; subsequently
subjecting said rods to centrifugal action to. remove said solvent therefrom; and prior to final drying
thereof adding to said rods inert anticaking agent and screening said brokenup rods in the presence
of said anticaking agent.
8. A method as defined in claim 7 wherein said cereal solids are hydrolyzed corn solids having a
dextrose equivalent of between 10 and 15.
9. A method as defined in claim 8 wherein said liquid solvent is isopropanol.
10. A method as defined in claim 8 or 9 wherein an excess of a pyrogenic silica is added as the
anticaking agent to said rods prior to final screening and drying and a quantity of silica is removed
during final screening and drying to leave sufficient silica in the product to prevent the particulate
rods from sticking together.
11. A method as defined in claim 11 or
12 wherein said rods are subjected to agitation in the isopropanol solvent to break up the rods and
the broken-up rods and isopropanol associated therewith are subjected to centrifuging to remove
the isopropanol.
12. A method as defined in claim 11
wherein the final drying of said broken-up rods is carried out during screening thereof over
successively smaller mesh screens to
accomplish the desired degree of screening
and remove undesired fines both of the rods
containing the essential oil and of the silica.
484/1651
13. A method according to claim 4 substantially as hereinbefore described with reference to the
drawing.
485/1651
74. GB2341091 - 08.03.2000
ESSENTIAL OIL COMPOSITION FOR TREATMENT OF HEAD-LICE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=GB2341091
Inventor(s):
WARK STEWART JOHN (GB)
Applicant(s):
ORE AN LTD (GB)
IP Class 4 Digits: A61K; A01N
IP Class:
A01N65/00; A61K7/06
E Class: A61K8/92C; A01N65/00+M; A61K7/40F
Application Number:
GB19980024592 (19981111)
Priority Number: GB19980024592 (19981111)
Family: GB2341091
Abstract:
THE PRESENT INVENTION RELATES TO A METHOD OF TREATING HEAD-LICE INVOLVING
APPLYING TO THE HAIR AND SCALP A FORMULATION, SUCH AS A SHAMPOO, CONDITIONER
OR TREATMENT OIL FORMULATION, COMPRISING, IN COMBINATION, TEA-TREE ESSENTIAL OIL,
LAVENDER ESSENTIAL OIL AND EUCALYPTUS ESSENTIAL OIL.
486/1651
75. GB2362574 - 28.11.2001
ESSENTIAL OIL MIXTURE FOR DESTRUCTION OF POULTRY RED MITE (DERMANYSSUS
GALLINAE) & ITS EGGS BASED ON EUCALYPTUS OIL, CITRONELLOL, TERPINEN-4-OL & MYRICA
GALE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=GB2362574
Inventor(s):
(GB)
STUART CAROLINE (GB); BLACKWELL ALISON (GB); STUART ANGUS ERSKINE
Applicant(s):
(GB)
STUART CAROLINE (GB); BLACKWELL ALISON (GB); STUART ANGUS ERSKINE
IP Class 4 Digits: A01N
IP Class:
A01N65/00
E Class: A01N65/00+M
Application Number:
GB20010000812 (20010112)
Priority Number: GB20010000812 (20010112)
Family: GB2362574
Abstract:
A NOVEL FORMULATION OF ESSENTIAL OILS, WHICH HAS BEEN NAMED 'ARD 75' AND IS
COMPOSED AS FOLLOWS: . ¦. EUCALYPTUS OIL: 1 PART . ¦. CITRONELLOL: 1 PART . ¦.
TERPINEN-4-OL: 0.25 PART . ¦. OIL OF MYRICA GALE: 0.25 PART . ¦. ORGANIC SEAWEED
SURFACTANT: QUANTUM SUFFICIT, IS DESCRIBED WHICH ACT SYNERGISTICALLY TO
PREVENT THE DEVELOPMENT OF EGGS OF THE POULTRY RED MITE, DERMANYSSUS GALLINAE
(ILLUSTRATED IN FIGURE 1). IN ADDITION, THE FORMULATION IS TOXIC AGAINST ADULT MITES,
RESULTING IN DEATH WITHIN MINUTES OF EXPOSURE (ILLUSTRATED IN FIGURE 2). THE OILBASED FORMULATION CAN BE APPLIED WITH A BRUSH, OR CONVERTED TO AN EMULSION
487/1651
FOR SPRAY-APPLICATION BY SIMPLE HOMOGENISATION WITH WATER AND AN APPROPRIATE
DETERGENT. EACH COMPONENT IS OF 'FOOD AND FRAGRANCE' QUALITY, USED IN THE
PERFUME- AND FOOD INDUSTRY. THE FORMULATION IS NEITHER TOXIC TO CHICKENS NOR
TO HANDLERS, AND DOES NOT TAINT CHICKEN EGGS.
488/1651
76. GB2369055 - 22.05.2002
COLOURED ESSENTIAL OIL SKIN PATCH
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=GB2369055
Inventor(s):
MAW JOANNA (GB)
Applicant(s):
MAW JOANNA (GB)
IP Class 4 Digits: A61K; A61F
IP Class:
A61K9/70; A61F13/02
E Class: A61K9/70E
Application Number:
GB20000026108 (20001025)
Priority Number: GB20000026108 (20001025)
Family: GB2369055
Abstract:
HEXAGONAL COLOUR CODED, SELF-ADHESIVE SKIN PATCHES IMPREGNATED WITH A BLEND
OF ESSENTIAL OILS. THE PATCHES ARE HERMETICALLY SEALED 1 PRIOR TO USE AND
PROVIDES THE USER WITH THERAPEUTIC BENEFITS. PREFERABLY THE PATCHES ARE SEVEN
DIFFERENT COLOURS WITH SEVEN DIFFERENT OIL BLENDS TO REFLECT THE RAINBOW
SPECTRUM. THE THERAPEUTIC ELEMENTS OF EACH COLOUR MAY MATCH THE HEALING
PROPERTIES OF EACH OIL BLEND. THE PATCHES MAY PROVIDE AN ALTERNATIVE METHOD
FOR ALLEVIATING THE SYMPTOMS OF STRESS.Description:
SPECIFICATION ;
ESSENTIAL OIL ENERGY PATCH
DESCRIPTION;
489/1651
This invention relates to the diffusion of Aromatherapy essential oils directly into the skin.
Essential oils are natural organic substances produced by the dissemination of the flowering plant.
They are well known for their therapeutic actions.
There are a variety of ways the molecules of essential oils are able to penetrate the skin. The most
popular methods, being in a carrier oil or cream, by inhalation or through water.
These methods are, however, time consuming and often inconvenient.
Furthermore, oils are substantially weakened once diluted into a cream or oil base, which can reduce
the overall benefits achieved.
The proposed invention presents a blend of essential oils penetrating the skin through a hexagonal
shaped self-adhesive patch. The oils, stored within the material, are activated by heat when placed
onto the body.
The patches have been designed in seven different'rainbow'colours with seven complementary oil
blends.
A specific embodiment of the invention will now be described by way of example with reference to
the accompanying drawing in which:
Figure 1 shows the anterior view of the hermetically sealed packet, which houses the patch.
Figure 2 shows the posterior view of the hermetically sealed packet, which houses the patch.
Figure 3 illustrates opening the protective packet and exposing the patch inside.
Figure 4 illustrates the'Energy Patch'.
Referring to the drawing Figure's 1 and 2, the packet has been hermetically sealed on all four sides 1.
To open, a childproof plastic edge 2 is located on the top left comer of the packet Applying pressure
snaps the edge back and allows the covering to be peeled open.
For identification, the top third of the packet is colour-coded 3 to match the colour of the patch inside.
490/1651
The back of the packet 4 provides relevant information on product composition, dosage, safety
precautions and directions of use. All relevant information on essential oils/colour therapy will be
provided within the future packaging and design of the product.
Referring to the drawing Figure 3, as previously stated, the protective covering 1 peels away from the
backing material 2 by snapping the childproof edge 3. The outside of the exposed patch 4 has a
protective non permeable waterproof coating and is colour coded to complement the blend of oils
inside.
The design of the hermetically sealed packet allows only the outside of the patch to be exposed
when opened. The inner-adhesive surface and oil composition remains unexposed on the protective
backing until removed.
Referring to the drawing Figure 4 the rigid clear plastic backing 1 protects the outer adhesive skin
contact layer. By removing and adhering the two pieces separately the patch is protected against
excess handling/contamination.
The essential oil composition lies directly beneath the skin contact layer. The rate and frequency of
diffusion is regulated by a continuous and controlled time release system.Claims:
CLAIMS.
Claim 1.
The invention presents a hexagonal-shaped colour coded range of self-adhesive patches that are
permeated with a complementary blend of essential oils.
They are stored in a dark hermetically sealed environment for protection.
Once activated, the oils will diffuse into the body on a controlled and continuous time release and
provide the user with the therapeutic benefits that each unique blend of oil has to offer.
Claim 2.
491/1651
A hexagonal shaped colour coded patch as claimed in claim 1 wherein the patches have been
designed in seven different colours.
Seven colours: red orange yellow green blue indigo and violet with seven different oil blends.
Both the colours and blends of oil reflect the visible'rainbow'spectrum. This means the therapeutic
elements of each colour, matches the healing properties, of each oil blend.
Claim 3.
A colour coded hermetically sealed patch infused with a complementary oil blend as claimed in
claim 1 wherein the design of the colour/oil coding creates an alternative method for helping to
alleviate the many and varied symptoms confronted during times of stress.
492/1651
77. GB421152 - 14.12.1934
IMPROVEMENTS IN AND RELATING TO ECUELLING MACHINES FOR THE EXTRACTION OF
ESSENTIAL OIL FROM THE RIND OF CITRUS FRUITS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=GB421152
Applicant(s):
ARTHUR SEAGAR BURLEIGH (--)
E Class: A23L1/222B
Application Number:
GB19340012221 (19340423)
Priority Number: GB19340012221 (19340423)
Family: GB421152
Abstract:
A MACHINE FOR EXTRACTING OIL FROM THE RIND OF CITRUS FRUITS CONSISTS OF AN
ARCUATE MEMBER 2 PROVIDED WITH MEMBERS RUPTURING THE RIND AND A REVOLUBLE
DRUM 11 MOUNTED CONCENTRICALLY WITH THE ARCUATE MEMBERS AND PROVIDED WITH
PRESSURE YIELDING MEMBERS 9 WHICH ROLL THE FRUIT OVER AND AGAINST THE
RUPTURING MEMBERS. THE PRESSURE MEMBERS 9 CONSIST OF SPRING-OPERATED
PLUNGERS PROVIDED WITH A PLATE 30 WHICH HAS A BENT PORTION 31. THE RUPTURING
MEMBERS CONSIST OF PLAIN, SAW-TOOTHED AND BLADED MEMBERS ARRANGED IN SETS,
EACH SET OCCUPYING A LENGTH NOT LESS THAN THE PERIPHERY OF THE LARGEST FRUIT
BEING TREATED. THE TEETH OR BLADES IN ADJACENT SETS ARE MOUNTED OUT OF
ALIGNMENT WHEREBY THE WHOLE SURFACE OF THE FRUIT IS TREATED. IN OPERATION,
LEMONS, LIMES, ORANGES OR GRAPE FRUIT 13 PASS ALONG A DOUBLE RAIL IN A SHOOT 12
FROM WHICH THEY ARE FED SINGLY BETWEEN THE ARCUATE AND REVOLVING MEMBERS.
THE FRUIT IS PRESSED AGAINST A SERIES OF RUPTURING MEMBERS CONSISTING OF:-PINTOOTHED MEMBERS, SAWTOOTHED MEMBERS, A SEMICIRCULAR GRID OF TOOTHED
BLADES, TWO SIMILAR SECTIONS HAVING SMALLER TEETH AND FINALLY MEMBERS WITH
LARGE SERRATIONS. THE EXTRACTED OIL FLOWS DOWN THE CHANNEL 14 AND IS DRAWN
OFF THROUGH A PIPE 15. THE TREATED FRUITS ARE DELIVERED TO A SHOOT 5 IN WHICH
493/1651
THEY ARE SPRAYED WITH WATER, AND THE OIL AND WATER IS COLLECTED AND SEPARATED
IN SETTLING TANKS. THE FRUIT MAY ALSO BE WASHED WITH WATER DURING TREATMENT IN
THE ARCUATE MEMBER 2.Description:
PATENT SPECIFICATION
Application Date: April 23, 1934. No. 12,221/34.
421,152 Complete Specification Accepted: Dec. 14, 1934.
COMPLETE SPECIFICATION.
Improvements in and relating to Ecuelling Machines for the Extraction of Essential Oil from the Rind
of Citrus Fruits.
I, Aunun SEAGAR BrLEIGeH, of Picard, Portsmouth, Dominica, British West Indies, a British subject,
do hereby declare the nature of this invention and in what manner the same is to be performed, to be
particularly described and ascertained in and by the following statement:This invention relates to an improved ecuelling machine for the extraction of essential oil from the
rind of citrous fruits, for example, from limes, oranges, lemons and grape-fruit. of the well known type
in which the fruit after being fed i5 into the machine, is rolled over a rupturing device adapted to
rupture the oil cells in the rind, the essential oil being expressed by pressure applied to the fruit while
being rolled.
More particularly, the invention relates to an improved machine of the well-known kind in which one
of the devices is a revolving wheel or drum, the periphery of which presses the fruits against the
other device. In the well known machine said device is preferably a flexible trough having pins or
prickers on elements linked together, and the wheel preferably has a serrated periphery. The
pressure exerted on the fruits is preferably caused by weights or springs attached to one end of the
flexible trough. The flexible trough is preferably enclosed in a casing for collecting the oil which
casing is provided with an outlet. The trough is provided with a hopper and with a discharge shoot
for the fruits.
An ecuelling machine according to the present invention comprises a frame, an arcuate device,
which is preferably semicircular and which is mounted on said frame and which comprises rupturing
494/1651
members adapted to rupture the oil cells in the rind when the fruit is rolled over them under pressure,
and a revoluble drum mounted on said frame concentric ally with said arcuate device and provided
with yieldable pressure-influenced peripheral parts or contacts. whieb are adanted when said
revoluble drum is rotated and when fruit is introduced between -,id arruate device and said revolubhl
drum. to make contact with said [Prioe 1/-1 EKe s fruit and to roll the same along the arcuate device
while yieldingly pressing 65 it against the aforesaid rupturing members on the latter. Said peripheral
parts or contacts are preferably in the form of radial spring-influenced pressure-units or plungers the
outer ends of which make 60 contact with.the fruit under treatment.
Machines according to the invention are preferably provided with delivering shoots (not claimed to
be new per se) for the fruit delivered from the arcuate devices 65 and with means for supplying
washing water to the fruit therein, said delivering shoots preferably being adjustable in inclination.
Moreover there are preferably arranged under the rupturing members oil-collecting and oilconducting means (also not claimed to be new per se) for collecting and conducting away oil
escaping from the fruit. Further, though it is perhaps hardly worth the 75 extra expense involved,
there may be provided means for supplying washing water to the fruit while being rolled over the
rupturing members.
The arcuate device which comprises the 80 rupturing members for rupturing the oil cells may, with
a view to facilitating cleaning operations, be displaceable on its frame in a direction parallel to the
axis of revolution of the revoluble member provided with the pressure-influenced contacts. rails
preferably being provided on said frame for this purpose. on which rails the arcuate device can be
readily run out.
The rupturing members are preferably 90 grouped together in a number of groups or sections, all
the members of a given section being similar to one another. and the members of different sections
being dissimilar, and the length of each section 95 Preferalfl being substantially equal to or greater
than the periphberv of the largest fruit within the capacity of the machine.
One form of ecuelling machine according to the present invention is illustrated 100 liv way of
examnle in the accompanying drawings. in which:Fi. 1 is a nart sectional side elevation of the
machine. many of the less important detailq being omitted. 105 Fig. 2 is a plan, the upper cover of !
the revolublea member being removed and the trough of the arcuate device being in its run out
position.
495/1651
Fig. 3 is a detail side elevation to an enlarged scale showing the outer ends of two plungers and of
one plungerretaining clip. These clips. are provided for the purpose of compressing the pressure
units on the revoluble member to enable the arcuate device to be withdrawn on the rails for the
purpose of cleaning the rupturing devices.
Fig. 4 is a corresponding, somewhat diagrammatic, end elevation of the said i5 parts shown in Fig. 3.
Fig. 5 is a cross-sectiOn through the arcuate device and a washing device under the same.
Fig. 6 is a part sectional side elevation to an enlarged scale of the right-hand part of the arcuate
device, the washing device and trough. under the same and of a part of the revoluble member, the
position of some of the plungers being indicated by chain-dotted lines.
Fig. 7 is-a cross-section to an enlarged scale t-lhrough the delivering shoot and its washing device,
a lime being shown in elevation and jets of water being indicated by clhain-dotted lines.
Fig. 8 is a part sectional side elevation to an enlarged scale of the inner end of the fruit feeding
shoot. of the arcuate device and of-the revoluble member with its plungers and of adjoining parts, a
few limes of various sizes being shown in various, positions.
Fig. 9 is a part sectional end elevation to -an enlarged scale of the arcuate device and of--the
revoluble member and adjacent parts, a. lime being shown under the lowermost plunger. Fig. 10 isa--part sectional side- elevation to an enlarged scale of- four. plungers and the outer peripheral
porton of-the revoluble member- on- which they are mounted..
Figs, 11, 13,_ 1.5, 17 and-19,are sections through the arcuate member on the lines XL-XI, X[II-XIII,
XV-X l, X7VI.i-XVI and X!X.-XIX of Fig. 8 respectively.
Figs. o12.. 14, 16, i8, and 20 are part sectional side, elevations -of- parts of the, are'ate -in'member
thr-otlgh - which the, sections of Figs. 11, 13, 15, 17. and 19 respectively pass. -tig. 21 is a detail.o'f
attaehment of one of the rupturing -menmbers shown in Figs.
15 and 16.
496/1651
Referrihg more particularly in the. firstr place to Fies, 1, 2, 6, 8'and 9 the. machine comprises the
frame 1 and. the following three more -important. parts, viz. thearcuate member 2, The drum 3
and.the washing device 4, which is incorporated with the delivery shoot 5.
The arcuate member 2 is mounted on said machine frame 1 and comprises a semi-circular frame 8
and rupturing 70 members 6 (see Figs. 8 and 9) supported thereon and designed to rupture the oil
cells in the rind of the fruit 7.
The drum 3 is revolubly mounted on the shaft 10 on said machine frame 1 75 concentrically with and
within said semicircular frame 8 and comprises the drum proper 11 and spring-influenced plungers
or pressure units 9, nmounted thereon and adapted to press the fruit against the 80 rupturing
members 6.
The washing device 4, as stated above, is incorporated:with the delivering shoot whereby the fruit is
washed free from adherent oil on emergence from the 85 arcuate and revoluble members.
When the machine is in action the fruit 13 (see Fig. 8) is fed down the feed shoot 12, which in effect
is a double rail along which the fruit can pass only in single o90 file and-is drawn into the machine
proper and rolled over the rupturing members 6 whereby the oil cells in the rind of the fruit are
ruptured and the essential oil expressed. The oil falls into a trough 14 95 below said members and
then flows out through the outlet 15 into a receptacle 16 (see Fig. 1). On emerging from between the
arcuate member and revoluble drum tile fruit passes down the delivering shoot 200 and as stated
above adherent oil is washed off. The effluent from the washer' passes through a series of separators
17, 18,. 19-Fig. -iL in which the. oil rises to the surface as a scum- which is skimmed off 105 for;
treatment for the recovery of the oil.
Referring now to the details of the arcuate mdember 2, the rupturing miembers. 6- and- their
supports 20 (see Figs; 13,. 15 and 17) together form a grid which 110 is, held; on the semi-circular
frame 8.
These, rupturing members 6 and their supports 20 are grouped into groups or sections of different
designs. These sections are however preceded by a series 115 of plain traiisverse units 21-, Figs; 11
and 12, whieh provide- an easy entrance for the fruit.
497/1651
T-he first rupturing section of rupturingmembers consists of six pairs. of saw-like 120 members- or
ecuelling blades 22 runningco-axially with the arcuate member and supported on four transverse
supports 20.
The blades- are, arranged six on each- sides the twor sides being alike and the teeth 125 are
preferably so graduated that tearing of- the fruit is: eliminated. This section treats? the ends of the
fruit.
The second rupturing section. of rupturing meiembers provides a somewhat semi421,152 on the
threaded end of the body 34 so that the contact is prevented from turning. To the end of the shank
opposite to the contact is affixed a spindle 32, Fig. 10, on which is placed, first, a collar 70 33, which
is a sliding fit in the body 34 and then a helical spring 35. This assembly is enclosed within the body
34 and retained by a plug 36 which is bored to accommodate the spindle 32. On the 75 protruding
portion of the spindle is placed a short helical spring 37 which is retained by a cup washer and. pin
38. The body 34 has external threads 39 for part of its length. As stated above the cap 340 is 80
screwed on the end of the body. When placed in its socket 29, the unit is secured in the desired
position by locknuts and washers 40, 41. Two lengths of body and spindle are employed, these
being placed 85 in the drum alternately and on the shorter units a collar 4 Fig. 8 is inserted between
the lock nut and the bushing. Above the drum the detachable casing 49 is provided. 0 Referring now
to the details of the washing device 4 which is incorporated with the delivering shoot 5, the latter is
provided with a trough bottom 43, Figs.
1 and 7, which projects slightly beyond 95 the shoot proper 5 and is provided with an outlet 44.
Placed above the trough are rails 45. 45 on which the fruit runs clear of the trough. Suspended above
the rails is a UJ-shaped washing device or tube 100 4. the outer ends of the members of which Ushaped tube are plugged and the inner ends of which are supplied with water through a tube 46. On
their undersides the members of the U-tube are provided i05 with orifices, through which issue jets
which spray the fruit passing along the shoot. The directions of these jets are such that the whole
surface of the fruit is covered as the latter passes along. By 110 means of the racks 47 and pins 48
the angle of the shoot can be adjusted and consequently the speed at which the fruit passes through
the washer can be varied.
Having now particularly described and 115 ascertained the nature of my said invention and in what
manner the same is to be performed, I declare that what IClaims:
claim is:-
498/1651
1. An ecuelling machine for the extraction of essential oil from the rind of citrus fruits, comprising a
frame, an arcuate device which is mounted on said frame and which comprises rupturing members
adapted to rupture the oil cells 125 in the rind when the fruit is rolled over them under pressure, and
a revoluble drum mounted on said frame concentrically with said arcuate device and provided with
yieldable pressure-influenced 130 circular grid for treatment of the remaining surface of the fruit and
is suited to the largest fruit within the capacity of the machine. The-top blade 23 Fig. 15 on each side
is without teeth and acts as a guard rail. The teeth of the other blades 24 in this section and of the
blades 25 in the succeeding sections of similar design are more acute than those of the first section
and are " set " like saw-teeth.
The next two sections are similar to the second section but provide a grid of slightly smaller crosssection to deal with the smaller sizes of fruit. The blades of sections one to four are held in place in
slots in the supports by wire clips 26, Fig. 21, and are removable. Those sections two to four are so
arranged that no two blades come in line, thus covering the surface of the. fruit thoroughly. Each
section is of a length substantially equa-l to or greater than the periphery of the largest fruit within the
capacity of the machine so that the largest fruit makes a complete revolution upon each section.
The fifth section is composed of a number of transverse members 27 set at a small distance apart.
These are provided with serrations of a larger section which are not set like saw-teeth. For certain
fruit it might be advisable to substitute for the fifth section as shown in Fig. 19, a section, similar to
Figs. 15, 17; or, again, in a lai'ge machine, more sections might be inserted, although these would
preferably be of the same design as those already specified.
The complete arcuate member is mounted on rails 28 attached to the machine frame I, so that said
member can be drawn out on said rails for purposes of cleaning or adjustment. The trough 14,
referred to above, is affixed to the semi-circular frame 8.
Referring now to the details of the revoluble drum 3 which comprises the drum proper 11 and the
spring-influenced plungers or pressure-units 9 mounted thereon, the said drum 11, Figs. 8, 9 and 10,
is provided on its periphery with a number of bushings or sockets 29 and the sides of the drum
instead of being in one piece as shown may be detachable in sections to provide special access to
the interior for the purpose of adjusting the pressure units. Secured in said sockets are a number of
adjustable and selfadjusting plungers or pressure units 9 which comprise flat top parts or contacts
499/1651
30 secured to square shanks 300. One end 31 of each contact 20 is bent so that it comes under the
unbent end of the preceding contact but at a distance below it.
The sqiare shank 300 passes through a square hole in the guide cap 340 screwed 421,15.
:s 421,152 peripheral parts or contacts which revolve withi it and which are adapted when said
revoluble drum is rotated and when fruit is introduced between said arcuate device and said
revoluble drum, to make contact with said fruit and to roll the same along the arcuate device while
yieldingly pressing it against the aforesaid rupturing members on the latter.
2. An ecuelling machine as claimed in claim 1, in which the periphery of the revoluble drum is
provided with a plurality of radial spring-influenced pressureunits or plungers, the outer ends of
which i5' make contact with the fruit under treatment, these pressure-units or plungers preferably
being arranged and constructed substantially as described with reference to the accompanying
drawings.
3. An ecuelling machine as claimed in claim 1, or in claim 2, comprising a delivering shoot for the
fruit delivered from the arcuate device and means for supplying washing water to the fruit therein,
said delivering shoot preferably being adjustable in inclination and, if desired, being, together with
said washing means, arranged and constructed substantially as described with reference to the
accompanying drawings.
4. An ecuelling machine as claimed in claim 1, 2 or 3. comprising oil-collecting and oil-conducting
means under the rupturing members for collecting and conducting away oil escaping from the fruit,
said means being if desired, arranged and constructed substantially as described with reference to
the accompanying drawings.
5. An ecuelling machine as claimed in claim 1, 2, 3 or 4. comprising means for supplying washing
water to the fruit while being rolled over the rupturing members, said means being, if desired,
arranged and constructed substantially as described with reference to the accompanying drawings.
6. An ecuelling machine as claimed in claim 1 or in claim 2, in which the arcuate device is
displaceable on the frame in a direction parallel to the axis of revolution of the revoluble member and,
preferably, on rails arranged substantially as described with reference to the accompanying
drawings.
500/1651
7. An ecuelling machine as claimed in claim 1 or in clainm 2, in which the arcuate device comprises
a plurality of sections of rupturing members, all the members of a given section preferably being
similar to one another, and the members of different sections preferably being dissimilar, and the
length of each section preferably being substantially equal to or greater than the periphery of the
largest fruit within the capacity of the machine, and one or more of the sections being, preferably,
arranged and constructed substantially as illustrated in the accompanying drawings.
8. An ecuelling machine for the extraction of essential oil from the rind of citrus fruits, substantially
as described with reference to the accompanying drawings.
Dated this 23rd day of April, 1934.
CLEMENT LEAN.
B.Sc., A.M.I.Mech.E., Chartered Patent Agent, Thanet House, 23112. Strand, London, W.C.2.
Redhill: Printed for His MajesEy's Stationery Office, by Love & Malcominson, Ltd.-1935.
501/1651
78. GB573789 - 06.12.1945
IMPROVEMENTS IN OR RELATING TO ESSENTIAL OIL COMPOSITIONS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=GB573789
Applicant(s):
ATLAS POWDER CO (--)
E Class: C11B9/00
Application Number:
GB19430005554 (19430407)
Priority Number: GB19430005554 (19430407)
Family: GB573789
Abstract:
HYDROXY POLYOXYETHYLENE ETHERS OF PARTIAL HIGHER FATTY ACID ESTERS OF LOW
MOLECULAR WEIGHT POLYHYDROXYLIC COMPOUNDS ARE PREPARED BY REACTING THE
PARTIAL ESTERS WITH ETHYLENE OXIDE IN THE PRESENCE OF SODIUM METHYLATE. OF A
LARGE NUMBER OF ACTUAL COMPOUNDS SPECIFIED, MANNITAN MONOLAURATE HYDROXY
POLYOXYETHYLENE ETHER WITH 20 OXYETHYLENE GROUPS PER MOL IS TYPICAL. THE
POLYHYDROXYLIC COMPOUNDS SPECIFIED, FROM WHICH THE ETHER-ESTERS ARE DERIVED,
COMPRISE POLYHYDRIC ALCOHOLS SUCH AS ETHYLENE GLYCOL, GLYCEROL,
PENTAERYTHRITOL, MANNITOL, SORBITOL; THEIR INTERNAL ETHERS SUCH AS MANNITAN,
SORBITAN, SORBIDE, MANNIDE; THEIR EXTERNAL ETHERS SUCH AS POLYGLYCEROLS,
DIPENTAERYTHRITOL; AND SUGARS SUCH AS GLUCOSE, SUCROSE AND CYCLITOLS SUCH AS
INOSITOL.ALSO:ESSENTIAL OIL COMPOSITIONS COMPRISE A MIXTURE OF AN ESSENTIAL OIL
AND AT LEAST AN EQUAL QUANTITY OF A WATER SOLUBLE HYDROXY POLYOXYETHYLENE
ETHER OF A PARTIAL HIGHER FATTY ACID ESTER OF A LOW MOLECULAR WEIGHT
POLYHYDROXYLIC COMPOUND. IN SUFFICIENT DILUTION, THE COMPOSITIONS ARE SUITABLE
AS PERFUMES, FLAVOURINGS AND THEATRE SPRAYS. AQUEOUS SOLUTIONS OF THE
COMPOSITIONS MAY BE MADE, THE ETHER-ESTER ACTING AS A DISPERSING AGENT. THE
POLYHYDROXYLIC COMPOUNDS SPECIFIED, FROM WHICH THE ETHER-ESTERS ARE DERIVED,
COMPRISE POLYHYDRIC ALCOHOLS SUCH AS ETHYLENE GLYCOL, GLYCEROL,
502/1651
PENTAERYTHRITOL, MANNITOL, SORBITOL; THEIR INTERNAL ETHERS SUCH AS MANNITAN,
SORBITAN, SORBIDE, MANNIDE; THEIR EXTERNAL ETHERS SUCH AS POLYGLYCEROLS,
DIPENTAERYTHRITOL; AND SUGARS SUCH AS GLUCOSE, SUCROSE AND CYCLITOLS SUCH AS
INOSITOL. THE USUAL FATTY ACIDS ARE USED, PREFERABLY OF 12 TO 16 CARBON ATOMS.
ETHYLENE OXIDE IS USED TO INTRODUCE THE OXYETHYLENE GROUPS ON TO THE
UNESTERIFIED HYDROXYLS OF THE PARTIAL ESTERS; THESE GROUPS SOLUBILIZE THE
COMPOUNDS AND THE ETHER-ESTERS CONCERNED HAVE FROM 6 TO 60 OXYETHYLENE
GROUPS PER MOL. THE COMPOUNDS ARE PREPARED BY REACTING THE PARTIAL ESTERS
WITH ETHYLENE OXIDE IN THE PRESENCE OF SODIUM METHYLATE. OF A LARGE NUMBER OF
ACTUAL COMPOUNDS SPECIFIED, MANNITAN MONOLAURATE HYDROXY POLYOXYETHYLENE
ETHER WITH 20 OXYETHYLENE GROUPS PER MOL IS TYPICAL. THE ESSENTIAL OILS SPECIFIED
COMPRISE THE OILS OF ORANGE, SPEARMINT, LEMON, CASSIA, CLOVE, CEDAR LEAF,
PEPPERMINT, TEA TREE, CHENOPODIUM, PINE NEEDLE, AND BENZALDEHYDE, EUCALYPTOL,
TERPINEOL, METHYL SALICYLATE, AND BENZYL ACETATE.Description:
PATENT SPECIFICATION
Application Date: April 7, 1943. No. 5554/43.
573i789 Complete Specification Accepted: Dec. 6, 1945.
COMPLETE SPECIFICATION
Improvements in or relating to Essential Oil Compositions (Communication fromn ATLAS PowDR
COMrPANY, a (Corporation organized under the laws of the State of Delaware, United States of
America,, of Delaware Trust Building, Wilmington, State of Delaware, United States of America.) I,
A.TniuR1 HAROLD STvuEms, a British Subject, of the Firm of Stevens, Laugner, Parry & Rollinson,
Chartered Patent Agents, of 5/9, Quality Court, Chancery Lane, London, W.G.2, do hereby declare
the nature of this invention and in what manner the same is to be performed, to be particularly
described and ascertained in and by the following statement:-The present invention relates to improvements in essential oil compositions.
Essential oils comprise a wide variety of flavouring, perfuming and medicinal materials. The various
essential oils have in common, in addition to their characteristic ability to be distilled, the property of
being virtually insoluble and very difficultly dispersible in water. Furthermore, the effects of the
503/1651
essential oils as regards taste and odour are obtainable to best advantage when the essential oil is
ad, a great dilution. Many of the essential oils used in flavouring and perfumery do not produce
pleasant sensations at all until they are diluted to d very eonsiderable extent. These facts are all
wellknown, and they have led to the use of a number of means for extending, diluting and dispersing
these oils in various media.
Many of the oils have been diluted with large quantities of alcohol and distributed in this form.
Instead of alcohol, other solvents, such as glycerol monoethyl ether, glycols, isopropyl alcohol, and
similar compounds, have been used for the purpose of extending and solubilizing the essential oils.
For the preparation of aqueous dispersions or solutions there have also been used a number of the
usual emulsifying and dispersing agents.
These materials have various objections.
such as undesirable odours or tastes of their own, undesirably high toxicity, expense either due to
the cost of the material or due to the large amount of material that must be used, and inability to
produce satisfactory aqueous solutions or [Prioe U] dispersions of the oils.
An object of the present invention is 55 to provide clear extended compositions of essential oils.
Another object is to provide a composition of an essential oil and a miscible solubilizing or dispersing
material which 60 composition is stable and capable of dilution with water to form solutions or
dispersions of the essential oil in water.
A further object is to provide a solution or dispersion of essential oil in water. 65 In accordance with
the present invention, an essential oil composition is provided, comprising an essential oil, and at
least an equal quantity 9f a water-soluble hydroxy polyoxyethyllfie ether of a, partial higher fatty acid
ester of a low molecular weight polyhydroxylic compound.
These essential oil compositions can be diluted with water to form stable dispersions or solutions- of
the essential oils. 75 Alternatively, such aqueous dispersions or solutions can be' prepared by
adding water to the essential oil and/or to the ether-ester before admixture thereof.
504/1651
The ether-esters used in the present in- 8G vention can be defined as water-soluble hydroxy
polyoxyethylene ethers of partial higher fatty acid esters of low molecular weight polyhydroxylic
compounds.
By "low molecular weight polyhydroxylie compounds" as meant compounds which' have two or more
hydroxyl groups and whose molecular weight is not greater than that of the oligosaccharides.
Preferred polyhydroxylic compounds of 90 thi- class are the polyhydrice alcohols such as ethylene
glycol, glycerol, pentaerythritol; hexitols, such as mannitol and sorbitol; the internal ethers of
polyhyd(lric alcohols, such as hexitans, for example, 95 mannitan and sorbitan, and hexides, for
example, sorbide and mannide; and the external ethers of the polyhydric alcohols, such as
polyglycerols and dipentaer.ythritol. Of the preferred group the 100 hexitans have been found best.
In addition to these preferred pollrhydroxylic compounds, others of the broad group can bhe used,
such as the sugars like glucose and sucrose, cyclitols, such as inositol, and others whiich will be
ap)parent.
r1 Price 75p Priice 4s,8A Prie 25p ) 0,789 As the fatty acid there can be used any of the aliphatic
monocarboxylic acids with not less than 10 carbon atoms, but preferably the fatty acids with from 12
to 18 carbon atoms are used and those with from 12 to 16 carbon atoms are best.
In the water soluble ether-esters employed in the invention, the fatty acid group is attached directly
to the polyhydroxylic compound, as distinguished from a compound in which the fatty acid is at the
end of a long plolyoxyethylene chain. The partial esters themselves are either completely or virtually
insoluble in water. However, by adding a sufficient number of oxyethylene units or groups to the
unestertified hydroxyls of the partial esters, the resulting etherester compound becomes watersoluble.
The number of oxyethylene units required to produce a particular watersoluble ether-ester is
dependent upon the length of the fatty acid chain and upon the number of fatty acid groups in the
molecule. Thus, a stearate requires more oxyethylene units to solubilize it than does a laurate.
Similarly, a diester requires about twice as many oxyvethylene units to solubilize it than does a
monoester. The solubility behaviour changes rapidly as the number of oxyethylene units passes
through the point indicated by the expression n =- - 12, where n is 3 the number of oxyethylene units
and C is the number of carbon atoms in the acid radical. In a range within about 1 or 2 units of this
number the compounds show water-solubility at the lower end and complete miscibility with water at
505/1651
the upper end. These figures are for a compound containing one acid equivalent per mol. (monoesters). compounds containing more than one acid equivalent per meol. require, in general, multiples
of these figures of oxyethylene units.
It has been found that the watersoluble hydro;xy polyoxyethylene ethers which have from 6 to about
60 oxyethylene units per mol, are satisfactory for the purposes of the invention. Within this range the
preferred compounds are those with from 12 to about 50 oxyethylene units per mol. It will be
understood that these numerical values may be average values in a mixed product. The preferred
products, as commercially prepared, are mixtures of 'a number of compounds of varying oxyethylene
chain lengths, the average of which is in the range stated above.
The hydroxy polyoxyethylene ethers can be made in a number of different ways which will be
apparent to those skilled in the art. It is preferred, however, first to make the partial ester by a 65
customary esterification procedure and then react the partial ester with ethylene oxide in the
presence of an alkaline catalyst, such as sodium methylate. To prepare the hexitan and hexide
esters it is 70 preferable to react a hexitol and the fatty acid (or fat or oil) under high temperature
conditions which produce anhydridization of the hexitol to the hexitan or hexide concurrently with the
esterificae, 75 tion. It has been found that the products made in this way have a useful heterogeneity
which makes them more, efficient as solubilizing, and dispersing agents for essential' oils. 80 This
invention is broadly applicable to essential oils as a class, both natural and synthetic types.
Representative members of this class which have been employed in the invention are benzaldehyde,
85 eucalyptol, oil of orange, terpineol, oil of spearmint, oil of lemon, oil of cassia, oil of clove, oil of
cedar leaf oil of peppermint, tea tree oil, oil o{ chenopodium, Siberian pine needle oil, methyl
salicylate and benzyl acetate.
The composition of essential oil and hydroxy polyoxyethylene ether is prepared by dissolving the
essential oil in a quantity of the ether. Some of the 95 hydroxy polyoxyethylene ethers are very
viscous or soft solids at room temperature and in such cases they should be warmed to liquify them
before dissolving the essential oil therein. The essential oils and 100 said ethers are soluble in each.
other so that compositions of varying concentrations can be made.
The compositions of essential oil and ether are clear, extended essential oil 105 solutions which can
be kept for an indefinite period without separation. In this form the compositions are highly useful for
flavouring, perfuming, or the like.
506/1651
The ethers are not volatile and actually 110 dissolve and hold the essential oil, redneing its volatility.
Many of the extended essential oil compositions are to be used to introduce, the essential oil into
aqueous media. To 115 produce stable fine dispersions or solutions the extended compositions
should have at least as much of the hydroxy polyoxyethylene ether as essential oil by volume and
preferably several times as 1'.0 much ether as essential oil. For example, a composition containing 4
to 6 or more parts of the ether to, 1 part of essential oil is useful in preparing a. highly diluted
aqueous dispersion or solution of the oil. 125 Aqueous dispersions or solutions of essential oils can
be made also by mixing the hydroxy polyoxyethylene ether, the ) 57;,78,9 essential oil and the water
in various sequences without first making a solution of the essential oil in ithe ether.
The compositions of the, invention find application wherever the essential oils are needed or
customarily employed. Flavouring concentrates are useful in the customary wmay in cooking and
candy-making practice. Perfume and deodorant oils are useful for making toilet waters, cosmetics,
laundry aids, and the like. A modern use for the perfume oil compositions is in the field of so-called
theatre sprays in which the essential oil dispersed in. water is sprayed either into the air Example
Ebsential Number. Oil. I 1 Benzaldehyde 2 Eucalyptol 3 Oil of Orange 4 Terpineol Oil of Spearmint 6
Oil of Lemon 7 Oil of Cassia 8 Olive of Clove 9 Oil of Cedar Leaf Oil of Peppermint 11 Tea Tree Oil
(Ti-tree) 12 Siberian Pine Needle Oil 13 Methyl Salicylate 14 Benzyl Acetate 1.5 Oil of Cassia 16 Oil of
Orange 17 Oil of Cassia, 18 Oil of Orange 19 Oil of Cassia 20 Oil of Orange....
21 Oil of Cassia 2'2 Oil of Orange 23 Oil of Cassia stream of an air-conditioning system or freely into
the theatre.
The following examples are illustrative of extended essential oil compositions that oan be made
according to the invention. In each case the essential oil and solvent indicated were mixed forming
clear solutions. The solvents were all liquids at room temperature with the exception of the ethylene
glycol derivatives 26 used in Examples 23 and 24. In the case of these two examples the ingredients
were warmed above the melting point of the solvent before mixing.
Solvent.
Parts.
1.
507/1651
1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 )arts.
1 mannitan mono-laurate hydroxy polyoxyethylene ether (20 oxyethylene groups per mol.) 1 do 1 do
1 do, 1 do 1 do 1 do 1 do 1 do 1 do 1 do 1 do 1 do 1 do 1 pentaerythritol monolaurate hydroxy
polyoxyethylene ether (20 oxyethylene groups per mol.) 1 do 1 glycerol monolaurate hydroxy
polyoxyethylene ether (20 oxyethylene groups per mol.) 1 do 1,glycerol monooleate hydroxy
polyoxyethylene ether (20-oxyethylene groups per mol.) 1 do 1 glycerol monostearate hydroxy
polyoxythylene ether (20 oxyethylene groups per mol.) 1 do ethylene glycol monolaurate hydroxy
polyoxyethylene ether (20 oxyethylene groups per meol'.) 3 Example Essential Number. Oil.
4 Oil of Orange 2 Oil of Orange 2a Oil of Orange A Oil of Orange Parts.
Solvent.
1 do 1 sorbitan monolaurate hydroxy polyoxyethylene ether (8 oxyethyleen groups per mol.) 1
sorbitan monolaurate hydroxy polyoxyethylene ether (20 oxyethylene groups per mol.) 1 minannitann
monolaurate hydroxy polyethylene ether (60 oxyethylene gToups per mol.) The following examples
are illustrative of aqueous dispersion or solutions of essential oils in accordance with the invention. In
each case a solution of essential oil and solvent was made first and then mixed thoroughly with the
water.
Ex. Essential No. Oil.
Chalracter Water of Parts. Solvent. Parts. Parts. Dispersion.
28 Oil of Orange 29 Oil of Orange 3,5 Oil of Cassia 31 Oil of Orange 32 Oil of Cassia 1 mannitan
monolaurate hydroxy polyoxyethylene ether (20 oxyethylene groups per mol.) 1 1 glycerol m
onolaurate hydroxy polyoxyethylene ether (20 oxyethylene groups per meolt,) 4 95 cloudy but stable
6 93 slightly cloudy but stable
7 9 clear 6 9 clear 7 9 clear ExaarrLs 33.
508/1651
1 part of oil of orange was shaken with 9 parts of water. 6 partes of manrlitan monolaurate hydroxy
polyoxyethyleni ether (20 oxyethylene units per mol.) were slowly added with agitation. When first
prepared the composition was a slightly turbid stable dispersion which became clear on standing
for.5 days.
EXAMPLF 34. 55 A mixture of 1 part of oil of oiange and 9 parts of water was agitated and to this 3
parts of mannitan monolaurate hydroxy pclyoxyet.hylene ether (20 oxyethylene units per mol.) were
added and 60 thoroughly mixed. Finally another 3 parts of the same ether were added and
thoroughly mixed in the composition. The 1a rts.
1 a-,sv'9 resulting composition was clear and stable.
From the foregoing description and exuamnples many other essential oil coirepositions will be
apparent to those skilled in the art. It will be understood that mixtures of different essential oils can be
used in these compositions.
Having now particularly described and ascertained the nature of my said invention, and in what
manner the same is to be performed (as communicated to me by my foreign correspondents), I
declareClaims:
that what I claim is:1. An essential oil composition, Comprising an essential oil, and at least an equal quantity of a
water-soluble hydroxy polyoxyethylene ether of a partial higher fatty acid ester of a low molecular
weight polyhydroxylic compound.
2. An essential oil composition, comprising an essential oil, and at least an equal quantity of a
water-soluble hydroxy poliyoxyethylene ether of a partial, ester of a higher fatty acid and a low
molecular weight polyhydroxylic compound selected from polyhydric alcohols and their internal and
external ethers.
3. A composition according to Claim 1 or 2, in which said water-soluble etherester is a mannitan.
monolaurate hydroxy polyoxyethylene ether.
4. A composition according to Claim 1 or 2, in which said water-soluble etherester is a mannitan
monopahlitate hydroxy polyoxyethylene ether.
509/1651
5. A composition according to, Claim 1 or 2, in which said water-soluble etherester is a
pentaerythritol monolaurate hydroxy polyoxyethylene ether.
6. A composition according to Claim 1 or 2, in which said water-soluble etherester is a glycerol
monolaurate hydroxy polyoxyethylene ether.
7. A composition according to Claim 1 or 2, in which said water-soluble etherester is a glycerol
mono-oleate hydroxy poly oxyethylene ether.
8. A composition according to Claim 1 or 2, in which said water-soluble etherester is a glycerol
monostearate hydroxy l)olyoxyethylene ether.
9. A composition according to' Claim 1 or 2, in which said water-soluble etherester is an ethylene
glycol monolaurate 66 hydroxy polyoxyethylene ether.
10). A composition according, to (Clain, 1 or 2, in which said water-soluble etherester is a sorbitan
monolaurate hydroxy polyoxyethylene ether. 60 11. A composition according to? any of the
preceding Claims, in which said water-soluble ether-ester contains front 6 to 60 oxyethylene units per
mol.
1'2. A composition according to. any of 65 the preceding Claims, in which the fatty acid of said
higher fatty acid partial ester is a fatty acid having from 12 to 18 carbon atoms.
13. An essential oil composition, coinprising an essential oil, and at least an equal quantity of a
water-soluble hydroxy polyoxyet.lhylene ether of a partial ester of a hexitan with a fatty acid having
from 12 to 16 carbon atoms, said hydroxy polyoxyethylene ether having from 6 to 60 oxyethyllene
units per mol.
14. An essential oil composition according to any of Claims 1 to 13, including water and in the form
of an aqueous dispersion or solution of the essential oil.
15. A method of making the composition according to Claim 14, in which the essential oil and etherester are first, mixed and water is then added. 85 16.. A method of nmaking the composition
510/1651
'according to Claim 14, in which water is first added to the essential oil and/or the ether-ester before
admixture thereof.
17. An essential oil composition according to any of Claims 1 to 13, containing a suitable essential
oil for use as a flavouring or perfumnling composition.
18. Essential oil compositions, substantially as hereinbefore described with reference to the
Examples.
Dated this 7th day of April, 1943.
For: ARTIHUR HIAROLD STEVENS:
Stevens, Langner, PalTy & Rollinson, Chartered Patent Agents, 5/9, Quality Court, Chancery Lane,
London, W.C.2, and at 120, East 41st Street, New York, United States of America.
1.eaniriington Spa: Printed The Patent 0ffil price
511/1651
79. GB633210 - 12.12.1949
MACHINE FOR RECOVERING ESSENTIAL OIL FROM THE RIND OF CITRUS FRUIT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=GB633210
Applicant(s):
TAGLITH LTD (--)
E Class: A23L1/222B; A23N1/00B
Application Number:
GB19470031130 (19471124)
Priority Number: ILX633210 (19470519)
Family: GB633210
Abstract:
IN A MACHINE FOR THE RECOVERY OF THE ESSENTIAL OIL CONTAINED IN THE PEEL OF
CITRUS FRUIT BY MEANS OF ROTATING CYLINDERS 7 PROVIDED WITH PINS OR THE LIKE
PROTUBERANCES ADAPTED TO PIERCE AND OPEN THE VESICLES OF THE PEEL OF THE FRUIT,
THE CYLINDERS ARE ARRANGED HORIZONTALLY AND PARALLEL TO EACH OTHER WITH THEIR
AXES IN AN ASCENDING PLANE, THE ROTATION OF THE CYLINDERS BEING SUCH AS TO
CAUSE THE FRUIT DURING TREATMENT TO CLIMB UPWARDS ACROSS THE ROTATING
CYLINDERS FROM A LOWER CYLINDER TO A NEXT HIGHER ONE. THE CYLINDERS ARE
JOURNALLED IN TWO OPPOSITE SIDES OF A FRAME, THE OTHER TWO SIDES 1A, 1B BEING
SUPPORTED ON STANDARDS 2, 3. THE SIDE 1A IS PIVOTALLY ATTACHED TO THE STANDARD 2
AND THE SIDE 1B IS COMBINED WITH A DEVICE FOR TILTING THE FRAME, SUCH AS AN
APERTURED STAY 4 ENGAGING WITH A PIN 6 PROVIDED ON THE STANDARD 3, OR A SCREWBOLT, TURNBUCKLE, C. THE CYLINDERS ARE DRIVEN IN THE SAME DIRECTION THROUGH
BELT PULLEYS AND GEARING KEYED TO THE ENDS OF THE AXLES OF THE CYLINDERS
PROJECTING THROUGH THE SIDE FRAMES. A FEEDING SHOOT 16 IS PROVIDED, PREFERABLY
INCLINED IN A DIRECTION INVERSE TO THE INCLINATION OF THE ASCENDING PLANE OF THE
AXES OF THE CYLINDERS 7. THE PEEL OF THE FRUIT IS THOROUGHLY RASPED IN ITS PASSAGE
UP THE INCLINED BANK OF CYLINDERS AND THE ESSENTIAL OIL IS WASHED OUT BY SPRAYS
OF WATER FROM NOZZLES 15, THE MIXTURE OF WATER AND OIL COLLECTING IN A TROUGH
512/1651
12 FASTENED TO THE UNDERSIDE OF THE FRAME FOR REMOVAL THROUGH AN OPENING 13
AND SUBSEQUENT SEPARATION. THE SHOOT MAY BE SUB-DIVIDED BY PARALLEL WALLS AND
THE AREA OF THE CYLINDERS MAY BE SUB-DIVIDED BY A REMOVABLE WALL 19 ARRANGED
ACROSS THEM.Description:
iz -: A
I
633,210 Application Date (in United Kingdom): Nov 24, 1947 No 31130/47.
Complete Specification Accepted: Dec 12, 1949.
Index at acceptance:-Class 91, ib:
COIV 01 PLETE SPECIFICATION
Machine for recovering essential oil -from the rind of citrus-fruit We, TAG Li TH LIMTED, a Company
organised under the laws of Palestine, of 25, Rothschild Boulevard, Tel Aviv, Palestine, do hereby
declare the nature of this invention 'and in what manner the same is to be performed, to be
particularly described and ascertained in and by the following statement: This invention relates to a machine for the recovery of the essential oil contained in the peel of citrus
fruit having rotating cylinders provided with pins or the like which are adapted to pierce and open the
vesicles of the flavedo of the fruit.
The essential oils contained in the vesicles of the flavedo of citrus fruit are recovered by opening the
vesicles, subjecting the fruit to a water spray and finally separating the oil from the water 'The
vesicles are opened by manually'operated rasping devices or by mechanically rotated cylinders In
the latter case the cylinders are provided on their circumference with pins or the like pointed
protuberances which during the rotation of the cylinders bruise the ilavedo of the fruit which is
passed by gravity or otherwise from one end of the cylinders to the other end Hereby the membranes
of the vesicles are pierced and disrupted Two co-operating cylinders or several pairs of such
cylinders have been used, the fruit being caused to travel along the cylinders from one end to the
other end thereof, and in the case of several pairs of cylinders in a serpentine way from one pair to a
succeeding one In order that the fruit may be rasped all round, the cylinders, if there is one pair only,
should be of considerable length On the other hand, in case of several parallel pairs used, the pairs
513/1651
must be separated from each other by partition walls to prevent the fruit from jumping from one pair
on to the other prior to completing its way along the whole length of one pair of cylinders.
According to the invention, the cylinders are arranged horizontally and -parallel to each other with
thei axes in an ascending (PRICE 2/-) plane, the rqtation of -the yliniiers 'b eijpg in a ldikecjioulto
cuise the fruit dpring treatment -to climb upwrds -across the rotating cy Jiixners fromn a lowe
_cylinder to the next bigher cylinder The fruit moves across tb@ syjiderssjn contradgstction to the
known jmqveement along the cylinders.
All cy Jin Iers,t Qtge in she same direction and -the frnit fed to the lowermost cylindexrs Oagsed 'to
climb upwards to-the higher cyliners -by the pins or pfotuberainces of the cylinders and also by
being pushed forward by the fresh fruit fed to the lowermost cylinder from an inclined chuite, thie
inclination _of the latter being inversejy directed to the-slope of the plane of the cylinders Said slope may vary between about 5-15 ' depending uponi the weight of the fruit and on the results obtained by
experience.
-The invention is -illustrated by way of example and in a schematical manner in the annexed
drawing, wherein Fig 1 represents a vertical section, -Fig 2 a plan view of the new machine.
A four-sided quadrangular frame rests -at two opposite sides ra, ib, on standards or supports 2, 3
Support 3 '-is higher than support 2,links or stays 4 of an adjustable length being interposed between
support 3 and frame by means of which the inclination of the frame can-be changed The links 4 are
provided with several holes 5 any one of which can be engaged by a horizontal pin 6 provided on
support 3.
Link 4 can of course be substituted by some other common device for raising the frame, e g some
screw-bolt, turnbuckle or the like Side la is pivotally attached to support 2.
In the two other opposite sides IC, id of the frame are journalled, in parallelism to and slightly
spaced from each other, cylinders or rollers 7 provided on their circumference with pins adapted to
pierce and disrupt the vesicles of the flavedo containing the essential oil On the ends of the axles of
the cylinders projecting out of the side Ic of the frame are keyed belt pulleys Perice 4 S ad L_ k,, As,
L-2-5 a }8 (see Fig 2 upper part) for driving all cylinders in the same direction For the same purpose
there may be fastened a belt pulley 9 on one axle only (see lower part of Fig 2) and the movement be
transmitted to the other axles by means of spur gears fixed on them, and intermediate gears 11 To
514/1651
the underside of the frame is fastened a trough 12 with an opening 13 in its bottom On the sides lc, id
of the frame is erected a vaulted roof 14 open at the sides la, lb of the frame Underneath the roof 14
are arranged several nozzle pipes 15 adapted to direct water sprays onto the cylinders 7 In front of
the machine there is arranged a chute 16 reaching to the lowermost cylinder 7 and inversely inclined
to the plane of the cylinders The chute is divided by walls 17 into several parts, through all or some of
which the ъruit can be fed down to the said lowermost cylinder In the lower edge of the chute 16 are
cut out incisions lo in prolongation of the partition walls 17, corresponding incisions 191 being
provided in the side lb A board -19 can be inserted on edge in any of the incisions 18 and in an
opposite incision 191 in side lb of the frame The machine operates as follows: The fruit-is supplied to
the chute 16 in any appropriate way wherefrom it slides down to the lowermost of the rotating
cylinders 7 The pins of the latter pick up the fruit penetrating its skin, and carry the fruit upwards
towards the next higher cylinder, which on its part feeds the fruit to the next higher cylinder and so on
until the fruit falls down from the last and highest cylinder This upward-trend of the fruit across the
cylinder -is assisted by the pressure exerted by the fruit sliding down the chute on the fruit already on
the cylinders While the fruit is thus pulled and pushed-upwards it is also rotated around its centre
and is rasped all round During-the transport -of the fruit across the cylinders the open vesicles are
washed out by the water-spray-and the mixture of water and oil is collected in the trough 12,
wherefrom it-is drained off for further treatment in the known manner For fruit of a lighter weight the
frame Will be given a greater inclination than for a fruit of a heavier weight If the machine built for a
certain output is to be used for a smaller output it is advisable to insert the partition wall 19 and to
allow the fruit to pass over the cylinders only on the right or left side of this wall.
HAVING NOW particularly described and ascertained the nature of our said invention and the
manner in which the same is to be performed, we declare that whatClaims:
we claim is:1 Machine for the recovery of the essential oil contained in the peel of citrus fruit by means of rotating
cylinders provided with pins or the like protuberances adapted to pierce and open the vesicles of the
flavedo of the fruit, characterised in that the cylinders are arranged horizontally and parallel to each
other with their axes in an ascending plane, -the rotation of the cylinders being so as to cause the
fruit during treatment to climb upwards across the rotating cylinders from a lower cylinder to a next
higher one.
515/1651
2 Machine as claimed in claim 1, characterised therein that a chute is provided for feeding fruit to the
lowermost cylinder 3 Machine as claimed in claim 2, characterised in that the chute is inclined in a
direction inverse to the inclination of the ascending plane.
4 Machine as claimed in claim 1, wherein the inclination of the ascending plane can be adjusted by
the cylinders being journalled in a frame which can be raised and lowered at one side.
Machine as claimed in claim 1, characterised by a removable wall arranged across the cylinders and
dividing the active area of the cylinders into areas of a smaller extension.
6 Machine for the recovery of the essential oil contained in the peel of citrus fruit substantially as
hereinbefore described and shown in the annexed drawing.
Dated this 24th day of November, 1947.
For the Applicants:
GILL, JENNINGS AND EVERY, Chartered Patent Agents, 51/52, Chancery Lane, London, W C 2.
Printed for H M Stationery Office by A Quick & Co, Ltd, Clacton-on-Sea -39-243-1948 Published at
The Patent Office, 25, Southampton Buildings, London, W C 2, from which copies price 2 s Od each
(inland), 2 s ld (abroad) may be obtained.
633,210
516/1651
80. IL42715 - 04.02.1975
MACHINE AND PROCESS FOR SIMULTANEOUSLY EXTRACTING THE JUICE AND ESSENTIAL OIL
OF CITRUS FRUIT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=IL42715
Inventor(s):
INDELICATO CARMELO (--); INDELICATO PAOLO (--)
Applicant(s):
INDELICATO PAOLO (--); INDELICATO CARMELO (--)
IP Class 4 Digits: B30B; A47J
IP Class:
B30B9/02; A47J19/02
E Class: A47J19/02
Application Number:
US19730373662 (19730626)
Priority Number: IT19730067840 (19730323)
Family: US3863560
Equivalent:
IT980680; ZA7304370
Abstract:
A MACHINE AND PROCESS FOR SIMULTANEOUSLY EXTRACTING THE JUICE AND ESSENTIAL
OIL OF CITRUS FRUIT, COMPRISING FEEDING THE CITRUS FRUIT INTO A GAP FORMED
BETWEEN A PAIR OF PARALLEL OPPOSITELY ROTATING CYLINDERS, CUTTING THE CITRUS
FRUIT INTO HALVES BY A CUTTING BLADE ARRANGED IN SAID GAP, FEEDING AND SQUEEZING
SAID HALVES ALONG A NARROWING GAP FORMED BETWEEN THE PERIPHERY OF EACH OF
SAID CYLINDERS AND AN ADJACENT PERFORATED METAL SHEET, COLLECTING THE JUICE
BELOW SAID PERFORATED METAL SHEET, CUTTING THE MEMBRANES AND MESOCARP OF THE
CITRUS FRUIT FROM THE PEELS, COLLECTING THE ESSENTIAL OIL ADHERING TO THE
517/1651
PERIPHERIES OF SAID CYLINDERS BY A PAD OF ABSORBENT MATERIAL AND SEPARATELY
COLLECTING THE CUT MEMBRANES AND MESOCARP AND THE CUT PEELS.Description:
This invention relates to a machine and process for simultaneously extracting the juice and essential
oil of citrus fruit and for simultaneously removing the mesocarp from the epicarp.
Machines for extracting the juice from citrus fruit are already known and machines for extracting the
essential oil from citrus fruit are also known. These two types of machines occupy much space and
perform two different working cycles, thus increasing production cost and reducing production
output.
Machines for the continuous extraction of the juice and the essential oil from citrus fruit are also
known. These machines comprise a combination of two units, i.e., an essential oil extractor and a
juice squeezer, arranged in tandem or cascade fashion. Such a machine is described in Italian Pat.
No. 912,325 filed on May 11, 1970 by the present applicants and issued on Mar. 15, 1972.
This invention provides an improved machine of the latter type in which the rasping unit for the
extraction of the essential oil is eliminated. The invention also provides a new process for
simultaneously extracting the juice and essential oil of citrus fruit with the aid of this improved
machine. According to this process the whole citrus fruit is introduced between a pair of straight
tubular adjacent cylinders having a vertical central cutting blade therebetween for cutting the citrus
fruit into two halves which are fed and squeezed together with the peel by the cutting blade into two
opposed gaps formed between the cutting blade and the periphery of the cylinders. The juice of the
citrus fruit is collected in a basin located centrally below the two cylinders whereas the peel is
squeezed and deformed in the progressively narrowing gaps to break up the oil vesicles contained
in the outer surface of the peel or epicarp and thus extract the essential oil contained in those
vesicles. The essential oil penetrates into the outer surface of the cylinders where it is retained due to
its viscosity and the effect of the peel which acts as a screen. Located downstream of the narrowest
portion of the gaps is a knife for separating the membranes from the mesocarp and the mesocarp
from the peel. The mesocarp then drops into a conveyor screw collector arranged therebelow and
the epicarp later drops into another conveyor screw collector, the collection of the mesocarp and
epicarp being assisted by jets of water fed into the two collectors for washing the peels, membranes
and mesocarps which together with the essential oil then form an emulsion which is fed to a
centrifugal separator. Upstream of the screw conveyors along the periphery of the cyclinders there is
located a pad or roller or absorbent material which is slightly biased against the periphery of the
518/1651
associated cylinder and absorbs the essential oil still adhering thereto, cleaning the cylinder and
discharging the essential oil dripping from the absorbent material to an exhaust duct.
The preferred embodiments of the invention will now be described by way of example and with
reference to the accompanying drawings in which:
FIG. 1 is a partially schematic cross-sectional view of a machine for extracting juice and essential oil
of citrus fruit according to the invention, and
FIG. 2 is a fragmentary view similar to a portion of FIG. 1, showing a modified form of absorbent
material, mounted on a rotating roller positioned adjacent the rotating cylinder.
Referring to the drawing, the machine proposed by the present invention for simultaneously
extracting the juice and essential oil of citrus fruit comprises a frame 1 supporting a pair of parallel
adjacent straight tubular cylinders 2 mounted for idling movement in the frame 1, the peripheries of
the cylinders 2 being spaced from each other by an amount slightly smaller than the diameter of the
smallest citrus fruit to be treated. The axes A of the cylinders 2 are parallel and located in a horizontal
plane and the peripheries of the cylinders 2 are rugged, for example, have outwardly projecting
points produced by embossing or punching from inside, so that the citrus fruit is gripped by the
cylinders and due to their rotation in opposite direction moved downwardly toward and through the
center line therebetween where a vertical cutting blade 3 is arranged which intercepts the citrus fruit
and cuts it into two halves. The two halves thus obtained are fed by the vertical cutting blade 3 in
cooperation with the pair of rotating cylinders 2 into two opposed curved gaps 4 each forming a
citrus fruit conveying channel. The inner surface of each of the gaps 4 is defined by the periphery of
the cylinder 2 while the outer surface of each gap 4 is defined by a perforated metal sheet 5 which
extends from the vertical cutting blade 3 downwardly in a curve which progressively approaches the
periphery of the cylinder 2, so that the gap 4 is restricted in cross section toward its outlet end. Due
to this restriction the mesocarp moved by the cylinders 2 is progressively crushed until all the juice is
squeezed out of the citrus fruit halves. The juice passes through the holes in the perforated metal
sheet 5 and is collected in a basin 6 arranged therebelow. Further, due to the deformation of the
curvature of the citrus fruit peel the essential oil is also extracted.
519/1651
The perforated metal sheet 5 is supported by a housing 7 having a pair of rectangular slots 8
extending in parallel to the axes of the cylinders 2. A pair of shafts 9 is located in the slots 8 and the
latter have an upper surface supported by the shafts 9. The shafts 9 are mounted eccentrically with
respect to their axle on the frame 1 of the machine. By rotating the eccentric shafts 9 the vertical
position of the perforated metal sheet 5 and thus the width of the gap 4 along which the citrus fruit
halves are moved can be adjusted. In this manner the width of the gap 4 can be adjusted to the
thickness of the mesocarp so that the latter is completely squeezed out.
While the citrus fruit is being cut and squeezed the oil vesicles in the outer surface of the mesocarp
are broken due to the deformation and flattening of the mesocarp. The oil flowing out of the vesicles
penetrates into the outer surface of the cylinders 2 but remains between the epicarp and the cylinder
surface. Thus the essential oil is extracted simultaneously with the cutting and squeezing of the citrus
fruit.
The mesocarp from which the juice and essential oil has been removed arrives at the outlet 10 of the
gaps 4 with the membranes still connected to the mesocarp. For detaching the membranes a pair of
steel blades or knives 20 supported by shafts 9' are provided, the knives 20 being located with their
cutting edge near the outlet opening 10 of the gaps 4 to remove the membranes from the mesocarp,
if desired, together with a portion of the mesocarp itself. The shafts 9' are firmly secured to the knives
20 so that by rotating the shafts 9' the angle of incidence of the knives on the mesocarp can be
adjusted, if desired even in such a manner that the knives do not even touch the mesocarp. A screw
conveyor 11 is arranged below the opening 10 to receive the removed cellulose and mesocarp and
discharge them from the machine.
A pump 12 is provided to feed jets of water through a pipe 13 to a second screw conveyor 14 for
discharging the peels and also to the screw conveyor 11 for discharging the membranes and
mesocarp. A basin 15 is arranged below the two screw conveyors 11 and 14 to collect the emulsion
of essential oil and the water admitted for washing the peels, membranes and mesocarp, this
emulsion being fed to a centrifugal separator (not shown).
Downstream of the knife 20 each of the cylinders 2 contacts a pad 16 of absorbent material slightly
biased toward the periphery of the adjacent cylinder 2 along an arc B of the circumference of the
cylinder and retained in position by a fixed wall 17 and a wall 18 which serves as a cover and can be
opened to permit the absorbent material 16 to be exchanged.
520/1651
So the essential oil on the outer surface of the cylinder 2 penetrates into and all over the abosorbent
material 16 and when the absorbent material is saturated with essential oil the latter starts to drip
down therefrom and is collected in an exhaust channel 19 provided on the wall 17 and is discharged
out of the machine.
Alternatively, the pad 16 may be replaced by at least one roller of absorbent material, referring to
roller 21 shown in FIG. 2. The roller 21 is mounted on a shaft 22 for rotation in a direction opposite to
the direction of rotation of the adjacent cylinder 2 and engages the periphery of the latter under slight
pressure.
During rotation of the cylinder 2 the essential oil on its outer surface penetrates into the absorbent
material of the roller 21 at the pinch point 20. An arcuate collecting duct 24 is provided adjacent the
roller 21 in a position opposite the pinch point 20 and engages the periphery of the roller 21 with a
perforated inner surface 23 under a pressure sufficient to squeeze the essential oil out of the roller 21
and through the perforated inner surface 23 into the collecting duct 24 which conducts the essential
oil out of the machine.
The machine and process according to the invention afford the following advantages:
a. The juice can be extracted from citrus fruit of any size.
b. The membranes and a portion of the mesocarp are cleaned.
c. The essential oil is extracted from the peel by deforming the latter rather than rasping it as in the
conventional machines, together with the extraction of the juice. In this manner a better quality of the
products is achieved.
d. The essential oil is obtained automatically without the use of water as a vehicle by means of the
cylinders with associated absorbent foam material and simultaneously the peels, membranes and
mesocarp are washed to extract the juice all with the use of only one relatively simple machine.
Altough a preferred embodiment of the invention has been described herein in detail and illustrated
in the accompanying drawing it is to be understood that the invention is not limited to this precise
embodiment and that numerous changes and modifications obvious to one skilled in the art may be
made therein without departing from the scope of the invention.
521/1651
Claims:
We claim:
1. A machine for simultaneously extracting the juice and essential oil of citrus fruit, comprising a
frame; a pair of parallel straight tubular cylinders mounted horizontally for rotation in opposite
directions on said frame; said parallel straight tubular cylinders having rugged peripheries adapted
to grip the citrus fruit and being separated from each other by a gap slightly smaller than the
diameter of the smallest citrus fruit to be treated; a vertical cutting blade arranged centrally in the
gap between the pair of cylinders for cutting the citrus fruit into two halves; a pair of perforated metal
sheets each extending from said vertical cutting blade downwardly in a curve progressively
approaching the periphery of an adjacent one of said pair of cylinders; a juice collecting basin below
said perforated metal sheets; a first pair of conveyor screw collectors at the downstream end of said
perforated metal sheets for collecting and discharging the cut membranes and mesocarp of the
citrus fruit; a knife at the downstream end of each of said perforated metal sheets for separating the
membranes of the citrus fruit from the mesocarp; absorbent material biased against the periphery of
each of said cylinders in an upper portion thereof for collecting essential oil adhering to the periphery
of said cylinders; an essential oil exhaust channel at the lower end of said absorbent material; a
second pair of conveyor screw collectors adjacent said knives and cylinders for discharging the cut
citrus fruit peels and an essential oil and water collecting basin below each of said second pair of
conveyor screw collectors.
2. A machine as claimed in claim 1, further comprising a pump and pipe means for feeding water to
each of said conveyor screw collectors to assist in discharging the membranes and mesocarp, and
the peels, respectively, of the citrus fruit.
3. A machine as claimed in claim 1, wherein said perforated metal sheets are adjustably mounted to
permit the width of the gap formed between each of said perforated metal sheets and an adjacent
one of said pair of cylinders to be adjusted.
4. A machine as claimed in claim 1, wherein each of said knives is secured to a rotatable shaft so
that the angle of incidence of the knife relative to the periphery of an adjacent one of said cylinders
can be adjusted by rotating the shaft.
5. A machine as claimed in claim 1, wherein said absorbent material is arranged in a pad on a fixed
wall mounted on said frame with one end thereof adjacent the periphery of each of said cylinders
522/1651
and supporting said pad of absorbent material from below while the top of said pad of absorbent
material is retained by another wall serving as a cover adapted to be opened to permit the pad of
absorbent material to be replaced.
6. A machine as claimed in claim 1, wherein said absorbent material is in the form of a roller of
absorbent material rotatably mounted adjacent the periphery of each of said pair of cylinders.
7. A process for simultaneously extracting the juice and essential oil of citrus fruit, comprising the
step of feeding the citrus fruit into a gap formed between a pair of parallel straight tubular cylinders
mounted horizontally for rotation in opposite directions; cutting the citrus fruit into two halves by a
vertical cutting blade arranged in the gap between said pair of cylinders; feeding, deforming and
squeezing the cut citrus fruit halves along a progressively narrowing gap formed between the
periphery of each of said cylinders and an adjacent perforated metal sheet; allowing the juice of the
cut citrus fruit halves to pass through said perforated metal sheet and collecting the juice in a basin;
cutting the membranes and mesocarp from the peels of the citrus fruit halves and collecting and
discharging the cut membranes and mesocarp; collecting and discharging the cut peels separately;
collecting the essential oil adhering to the peripheries of said cylinders by a pad of absorbent
material arranged adjacent said cylinders and collecting the essential oil dripping from said pad of
absorbent material in an exhaust channel.
523/1651
81. IN185741 - 21.04.2001
A COMPOSITION USEFUL FOR HYBRIDIZATION OF PALMAROSA (CYMBOPOGON MARTINII) FOR
INCREASED HERBAGE AND ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=IN185741
Inventor(s):
-)
KRISHNA SRIVASTAVA HARI (--); KUMAR SATPUTE GYANESH (--); AJAY MISRA (-
Applicant(s):
COUNCIL SCIENT IND RES (--)
IP Class 4 Digits: A01C
IP Class:
A01C21/00
Application Number:
IN1997DE02135 (19970731)
Priority Number: IN1997DE02135 (19970731)
Family: IN185741
524/1651
82. IT1179658 - 16.09.1987
APPTS. EXTRACTING ESSENTIAL OIL FROM PLANTS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=IT1179658
Inventor(s):
INDELICATO CARMELO (--); INDELICATO PAOLO (--)
Applicant(s):
INDELICATO SRL FLLI (IT)
IP Class 4 Digits: A23N
IP Class:
A23N
Application Number:
IT19840067479 (19840511)
Priority Number: IT19840067479 (19840511)
Family: IT1179658
Abstract:
PIXEL IMAGE DATA INCLUDING DEPTH DATA, PREFERABLY REPRESENTING A SPHERE OR
COLUMN, ARE GENERATED AND STORED IN A MAPPING MEMORY. WHEN THE SPHERE OR
COLUMN IS TO BE DISPLAYED ON A DISPLAY SCREEN, THE IMAGE DATA ARE READ OUT FROM
THE MAPPING MEMORY TO A PREDETERMINED REGION OF A FRAME MEMORY. HIDDEN
SURFACE REMOVAL IS PERFORMED IN ACCORDANCE WITH THE DEPTH DATA AND ONLY
VISIBLE DATA IS WRITTEN INTO THE FRAME MEMORY. SPHERES AND COLUMNS ARE USED TO
REPRESENT CHEMICAL STRUCTURES.
525/1651
83. IT1204934 - 10.03.1989
ESSENTIAL OIL EXTRACTION EQUIPMENT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=IT1204934
Inventor(s):
DECIO GIOVANNI (--)
Applicant(s):
BERTUZZI SPA (IT)
IP Class 4 Digits: A23N
IP Class:
A23N
Application Number:
IT19870019685 (19870313)
Priority Number: IT19870019685 (19870313)
Family: IT1204934
Abstract:
STORAGE VESSELS FILLED WITH WASTE RADIOACTIVE MATERIAL ARE TAKEN UNDERGROUND
USING THE ENTRANCE OF AN OPERATING OR ABANDONED MINE. THE VESSELS ARE
DEPOSITED IN CHAMBERS CUT INTO PREVIOUSLY UNDISTURBED ROCK BELOW THE `KARST'
WATER LEVEL. THE CHAMBERS ARE FILLED AND EACH CHAMBER, SECTION AND THE WHOLE
`FIELD' IS SEALED OFF AGAINST WATER. TRANSPORT IS ALWAYS CARRIED OUT AGAINST THE
FLOW OF VENTILATION AIR. THE UNDERGROUND STORAGE AREA IS LOCATED BELOW THE
`KARST' WATER LEVEL, IN ROCK FORMATION WITH A MAX. OF 10 POWER(-6) CM/SEC. WATER
LEAKAGE, AT LEAST 100 METRES FROM THE BOUNARY OF THE FORMATION, AND AT LEAST
300 METRES FROM ROCK, WHICH IS ALREADY DISTURBED. THE STORAGE AREA HAS A MAX.
OF TWO CONNECTIONS TO THE SURFACE, THESE ARE FOR INWARD TRANSPORT AND TIE-IN.
THE STORAGE AREA IS DIVIDED INTO SECTIONS IN WHICH ACCESS ROADS AND STORAGE
CHAMBERS ARE CUT. EACH CHAMBER IS SURROUNDED BY PROTECTIVE ROCK. FULL
CHAMBERS AND SECTORS ARE SEALED WITH WATER TIGHT STRUCTURES
526/1651
84. IT1227275 - 28.03.1991
ANTI OXIDATION LEMON ESSENTIAL OIL, RELATIVE PREPARATION PROCESS FORMULAS
CONTAINING IT AS ACTIVE INGREDIENT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=IT1227275
Inventor(s):
RIZZA VICTOR (--); SCAPAGNINI UMBERTO (--)
Applicant(s):
T ASSOCIATED BIO TECHNOLOGIES (IT)
IP Class 4 Digits: A61K
IP Class:
A61K
Application Number:
IT19880022172 (19881004)
Priority Number: IT19880022172 (19881004)
Family: IT1227275
Abstract:
THE PRESENT INVENTION CONCERNS AN EXTRACT DERIVING FROM LEMON PERICARP, SAID
LEMON HAVING REACHED A PARTICULAR RIPENESS STADIUM, IN WHICH LEMON PERICARP
BECOMES GREEN. IN ORDER TO OBTAIN SAID EXTRACT, THE LEMON PERICARP IS FIRST
SQUEEZED AND THEN CENTRIFUGED; FINALLY, VACUUM DISTILLATION AND PREPARATION
CHROMATOGRAPHY FOLLOW. THE OBTAINED EXTRACT HAS ANTI OXIDATION PROPERTIES,
USEFUL IN THERAPIES.
527/1651
85. JP1023000 - 25.01.1989
CONVERSION OF VEGETABLE ESSENTIAL OIL TO BE EASILY SOLUBLE IN WATER
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP1023000
Inventor(s):
NAKADA TATSUO (--)
Applicant(s):
KAMEYA MINAMI CHAIN:KK (--)
IP Class 4 Digits: A61K; C11B; B01F
IP Class:
C11B9/00; A61K7/26; B01F17/30
Application Number:
JP19870179489 (19870717)
Family: JP1023000
Abstract:
PURPOSE:TO CONVERT A LARGE AMOUNT OF AN ESSENTIAL OIL OF VEGETABLES SUCH AS
HIBA ARBORVITAE, PINE OR HINOKI CYPRESS INTO AN EASILY WATER-SOLUBLE OIL WITHOUT
LOSING THE FRAGRANCE NOR CAUSING THE PROBLEM OF TOXICITY, ETC., BY ADDING
WATER AND A PROTEIN (OR MODIFIED PROTEIN) TO THE ESSENTIAL OIL.
CONSTITUTION:AN ESSENTIAL OIL SUCH AS HIBA OIL, TURPENTINE OIL OR OLIVE OIL
PRODUCED BY THE STEAM DISTILLATION OR DRY DISTILLATION OF A PLANT SUCH AS HIBA
ARBORVITAE, PINE OR HINOKI CYPRESS IS ADDED WITH WATER AND A (MODIFIED) PROTEIN
SUCH AS CASEIN SODIUM AND, AS NECESSARY, FURTHER WITH A CYCLODEXTRIN AS AN
ASSISTANT TO MAKE EASILY SOLUBLE IN WATER. THE OBTAINED ESSENTIAL OIL
COMPOSITION IS USEFUL AS A BATHING AGENT, FLAVOR AND AROMATIC AGENT.
528/1651
86. JP10316991 - 02.12.1998
PREPARATION OF NATURAL ESSENTIAL OIL WHICH DOES NOT CONTAIN PSORALEN
COMPOUND
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP10316991
Inventor(s):
AWANO KENICHI (--)
Applicant(s):
T HASEGAWA CO LTD (--)
IP Class 4 Digits: C11B
IP Class:
C11B9/02
Application Number:
JP19970139176 (19970515)
Family: JP10316991
Abstract:
PROBLEM TO BE SOLVED: TO REMOVE PSORALEN COMPDS. FROM A NATURAL ESSENTIAL OIL
CONTG. THE SAME INDUSTRIALLY EASILY WITHOUT ADVERSELY AFFETING THE YIELD, THE
PERFUME COMPONENT BALANCE OF THE OIL, ETC., BY FRACTIONATING THE PSORALEN
COMPDS. WITH CARBON DIOXIDE IN THE SUBCRITICAL OR SUPERCRITICAL STATE AS A FLUID
AND WITH A SUPERCRITICAL CARBON DIOXIDE EXTRACTION COLUMN CHROMATOGRAPH
APPARATUS FILLED WITH A POROUS POLYMERIC RESIN.
SOLUTION: AN EXTRACTION CONTAINER/SEPARATION COLUMN 5 IS FILLED WITH A POROUS
POLYMERIC RESIN HAVING A SPECIFIC SURFACE AREA OF 300-700 M<2> /G, A MICROPROE
VOL. OF 0.7-1.1 ML/G, AND A MICROPORE RADIUS OF 50-1,300 ANGST . THEN, CARBON
DIOXIDE IN A SUBCRITICAL OR SUPERCRITICAL STATE AT 31 DEG.C OR LOWER UNDER A
PRESSURE OF 75 KG/CM<2> OR HIGHER IS SUPPLIED TOGETHER WITH A NATURAL ESSENTIAL
OIL CONTG. PSORALEN COMPDS. FROM A BOMB 1 THROUGH A SPARE COIL 2, AN INDICATOR
3, AND A SIX-WAY VALVE 6 TO THE SEPARATION COLUMN IN ORDER TO CAUSE THE POROUS
POLYMERIC RESIN TO ADSORB THE PSORALEN COMPDS. TO FRACTIONATE AND REMOVE
529/1651
THEM. THE ESSENTIAL OIL DISSOLVED IN CARBON DIOXIDE AND CONTG. NO PSORALEN
COMPD. IS SEPARATED FROM CARBON DIOXIDE IN THE GAS-LIQ. SEPARATION COLUMN 5.
530/1651
87. JP10338630 - 22.12.1998
ESSENTIAL OIL-CONTAINING AGENT TO PREVENT FUNGAL INFECTION/SPREAD
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP10338630
Inventor(s):
INOUE SHIGEHARU (--); WATANABE MASANORI (--); TAKEO KANJI (--); AKAO
MITSUTARO (--); NISHIYAMA YAYOI (--); YAMAGUCHI HIDEYO (--)
Applicant(s):
MEIJI SEIKA KAISHA LTD (--); INOUE SHIGEHARU (--)
IP Class 4 Digits: A61K; C11B; A01N
IP Class:
A61K35/78; C11B9/00; A01N65/00; A01N27/00; A01N31/02; A01N35/02;
A61K31/045; A01N31/04; A01N31/08; A01N35/06; A01N37/02; A61K31/11
Application Number:
JP19970148744 (19970606)
Family: JP10338630
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN THE SUBJECT AGENT HAVING LOW TOXICITY AGAINST
WARM-BLOODED ANIMALS, INHIBITING SPORE-FORMING ACTIVITY OF SPOROGENIC FUNGI,
TERMINATING GROWTH OF ITS MYCELIUM AND RE-GROWTH OF IT, AND HENCE APPLICABLE
TO SICKROOMS WHICH HOUSE EASILY INFECTIONS PATIENTS, BY INCLUDING ESSENTIAL OIL
LAND SO ON.
SOLUTION: THIS AGENT IS OBTAINED BY INCLUDING AN ESSENTIAL OIL SUCH AS PERILLA OIL,
PIECES OF A PLANT (E.G. LEAF OF GREEN PERILLA) CONTAINING AN ESSENTIAL OIL, OR MAIN
COMPONENTS OF AN ESSENTIAL OIL SUCH AS CARVACROL AND TIMOR. A FUNGUS SUCH AS
ASPERGILLUS FUMIGATUS IS EXPOSED TO THE AGENT AT 1-400 MG/L IN A SEALED SPACE BY
HEAT EVAPORATION AND SO ON, PREFERABLY FOR 2-3 DAYS TO PREVENT SPOREFORMATION OR FOR 10-30 MIN TO SUPPRESS GROWTH OF ITS MYCELIUM AND RE-GROWTH
OF IT. OTHER APPLICABLE PLACES INCLUDE ONES TO STORE CROP/FOOD AND BATH ROOM.
531/1651
88. JP11061091 - 05.03.1999
RESONANCE MAGNETIC FIELD WATER INTO WHICH ESSENTIAL OIL HAS BEEN DROPPED
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP11061091
Inventor(s):
SUZUKI KIYOKAZU (--); LEE H LORENZEN (--)
Applicant(s):
IHM:KK (--)
IP Class 4 Digits: A61K; A61L; A01N; C09K
IP Class:
A61K35/78; A61L9/01; A01N65/00; C09K3/00; A61K7/00; A01N25/02
Application Number:
JP19970262597 (19970822)
Family: JP11061091
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE WATER WHICH IS EFFECTIVE IN KEEPING AND
IMPROVING HUMAN HEALTH AND IN CLEANING AIR, TO STABILIZE THE MIXTURE OF WATER
AND AN ESSENTIAL OIL, AND TO SOLVE THE PROBLEM WITH THE STORABILITY OF AN
ESSENTIAL OIL BY ADDING A MINUTE AMT. OF AN ESSENTIAL OIL TO RESONANCE MAGNETIC
FIELD WATER.
SOLUTION: IF NECESSARY, 3-10% ALCOHOL (E.G. ETHANOL), 1-5% GLYCERIN, OR 0.05-2%
POLYSORBATE 80 OR LECITHIN IS ADDED TO RESONANCE MAGNETIC FIELD WATER, A
PRODUCT DEVELOPED BY DR LIE H. LORENTZEN. THEN, ABOUT 1-2 DROPS (0.05-0.01 ML) OF
AN ESSENTIAL OIL IS ADDED TO 100 ML OF THIS RESONANCE MAGNETIC FIELD WATER,
WHICH IS THEN VIBRATED TO GIVE A BLEND. THIS BLEND IS DILUTED ABOUT 200 TIMES WITH
WATER BEFORE BEING USED. IN THIS CASE, THE ESSENTIAL OIL IS DILUTED ABOUT 400,000800,000 TIMES AND HENCE A MILD EFFECT IS ACHIEVED AT A LOW COST. THUS, THE
IRRITATIVE PROPERTIES OF AN ESSENTIAL OIL ISELF IS WEAKENED AND THE PROBLEM WITH
STORABILITY IS SOLVED BY THE CHARACTERISTICS OF MICROCLUSTER WATER.
532/1651
89. JP11118739 - 30.04.1999
COMPUTERIZED MAGNETIC RESONANCE ANALYZER, AND MEASUREMENT METHOD BY USING
ANALYTICAL INSTRUMENT HAVING EQUAL EFFICIENCY TO THE SAME FOR SPECIFYING
MATERIAL, AND BLEND RATIO OF ESSENTIAL OIL BLEND FOR SPECIFIC USE, AND ITS
APPLICATION
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP11118739
Inventor(s):
SUZUKI KIYOKAZU (--)
Applicant(s):
IHM:KK (--)
IP Class 4 Digits: A61K; C11B; A23L; G01N; A61B
IP Class:
G01N24/00
A61K35/78; C11B9/00; A61K7/00; A23L1/222; A23L1/30; G01N24/08; A61B5/055;
Application Number:
JP19970310980 (19971008)
Family: JP11118739
Abstract:
PROBLEM TO BE SOLVED: TO SELECT AN ESSENTIAL OIL EFFECTIVE TO IMPROVE A SPECIFIC
ITEM OF A PARTICULAR PERSON, BY USING A COMPUTERIZED MAGNETIC RESONANCE
ANALYZER AND AN ANALYTICAL INSTRUMENT HAVING EQUAL EFFICIENCY TO THE ANALYZER.
SOLUTION: ACCORDING TO THIS METHOD, A MUTUAL ACTION OF MINUTE MAGNETIC
RESONANCE PATTERNS IS JUDGED BY A COMPUTERIZED MAGNETIC RESONANCE ANALYZER
AND AN ANALYTICAL INSTRUMENT HAVING EQUAL PERFORMANCE TO THE ANALYZER. AN
EFFECTIVE COMBINATION AND A PROPER BLEND RATIO ARE OBTAINED FROM CONGENIALITY
RELATIONSHIPS OF HUMAN CONSTITUTIONS AND VARIOUS MATERIAL AND OF VARIOUS
MATERIALS. THE COMPUTERIZED MAGNETIC RESONANCE ANALYZER REPRODUCES NORMAL
PATTERNS OF THE MINUTE MAGNETIC RESONANCE PATTERNS OF HUMAN BODIES AND
SUBSTANCES APPROXIMATELY AND OBTAINS AN ECHO FROM A BODY TO BE ANALYZED. FOR
INSTANCE, A PERSON'S HAND (B) TO BE ANALYZED AND A CANDIDATE SUBSTANCE (C)
533/1651
(ESSENTIAL OIL) EXPECTED TO BE USEFUL FOR IMPROVEMENT ARE PLACED AND MEASURED
ON A MEASUREMENT PLATE (A) OF THE COMPUTERIZED MAGNETIC RESONANCE ANALYZER.
A REACTION AS A RESULT OF THE MEASUREMENT IS EXPRESSED BY SOUND OR A CHART
GRAPH.
534/1651
90. JP11209212 - 03.08.1999
ANTIMICROBIAL COMPOSITION CONTAINING ESSENTIAL OIL OF MOSLA CHINENSIS MAXIM AS
ACTIVE INGREDIENT, AND ANTIMICROBIALLY PROCESSED PRODUCT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP11209212
Inventor(s):
FURUYA TSUTOMU (--)
Applicant(s):
MURATA MAKOTO (--); FURUYA TSUTOMU (--)
IP Class 4 Digits: A01N
IP Class:
A01N65/00; A01N25/02
Application Number:
JP19980012721 (19980126)
Family: JP11209212
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN AN ANTIMICROBIAL COMPOSITION UTILIZING AN
ANTIMICROBIAL COMPONENT INCLUDED IN THE PLANT MOSLA CHINENSIS MAXIM
BELONGING TO THE GENUS MOSLA, AND FURTHER TO OBTAIN AN ANTIMICROBIALLY
PROCESSED PRODUCT.
SOLUTION: THIS ANTIMICROBIAL COMPOSITION IS OBTAINED BY CARRYING OUT STEAM
DISTILLATION OF MOSLA CHINENSIS MAXIM TO PROVIDE AN ESSENTIAL OIL, AND DILUTING
THE ESSENTIAL OIL WITH A SUITABLE DILUENT, TYPICALLY WATER OR ETHANOL. THE
ANTIMICROBIALLY PROCESSED PRODUCT IS OBTAINED BY ALLOWING THE ESSENTIAL OIL TO
BE IMPREGNATED INTO A SUITABLE CARRIER, E.G. A FIBER PRODUCT, A PAPER, A CLOTH AND
A PLASTIC FILM, OR COATING THE ESSENTIAL OIL ON THE FIBER PRODUCT, THE PAPER, THE
CLOTH AND THE PLASTIC FILM SO AS TO BE HELD THEREON.
535/1651
91. JP11209294 - 03.08.1999
PARASYMPATHOMIMETIC AGENT CONTAINING ESSENTIAL OIL AS ACTIVE INGREDIENT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP11209294
Inventor(s):
KARITA TAKESHI (--)
Applicant(s):
KARITA TAKAHISA (--)
IP Class 4 Digits: A61K
IP Class:
A61K35/78; A61K9/70
Application Number:
JP19980008858 (19980120)
Family: JP11209294
Abstract:
PROBLEM TO BE SOLVED: TO PREPARE A PARASYMPATHOMIMETIC AGENT HAVING
MITIGATING ACTIONS ON ABNORMAL MYOTONIA BY ADMINISTRATION THEREOF TO A PATIENT
IN A WAKEFULNESS STATE WITHOUT CAUSING ADVERSE EFFECTS.
SOLUTION: THIS PARASYMPAYTHOMIMETIC AGENT CONTAINS AT LEAST ONE OR MORE KINDS
OF ESSENTIAL OILS, PREFERABLY A MIXTURE OF AN ESSENTIAL OIL OF THE FAMILY
RUTACEAE WITH A EUCALIPTUS OIL AND A THYME OIL OR A MIXTURE OF THE ESSENTIAL OIL
OF THE FAMILY RUTACEAE WITH THE EUCALYPTUS OIL, THYME OIL AND/OR AN ESSENTIAL OIL
OF THE FAMILY LABIATAE OTHER THAN THE THYME OIL AS AN ACTIVE INGREDIENT. THE
AGENT FOR THE PARASYMPATHETIC NERVOUS SYSTEM IS READILY APPLICABLE AND
CAPABLE OF RAPIDLY STOPPING THE MEDICATION DUE TO A SHEETLIKE PREPARATION FOR
EXTERNAL USE THEREOF.
536/1651
92. JP11226578 - 24.08.1999
SPECIAL FUNCTION WATER TO WHICH MAGNETIC RESONANCE PATTERN OF ESSENTIAL OIL IS
TRANSFERRED
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP11226578
Inventor(s):
SUZUKI KIYOKAZU (--)
Applicant(s):
IHM:KK (--)
IP Class 4 Digits: A61K; C02F
IP Class:
C02F1/48; A61K33/00
Application Number:
JP19980065992 (19980210)
Family: JP11226578
Abstract:
PROBLEM TO BE SOLVED: TO PUT BODY CONDITIONING FUNCTION TO PRACTICAL USE AND
TO ENABLE THE SAFE DRINKING AND INTERNAL USE OF WATER BY TRANSFERRING THE
MAGNETIC RESONANCE PATTERN POSSESSED BY AN ESSENTIAL OIL TO RESONANCE
MAGNETIC FIELD WATER OR OTHER WATER SUBJECTED TO MICROCLUSTERING TREATMENT
TO USE THE SAME.
SOLUTION: FOR EXAMPLE, A GLASS BOTTLE HOUSING A MIXTURE OF LAVENDER OIL,
FRANKINCENSE OIL AND ROSEMARY OIL IS PLACED IN THE IN-WELL OF AN MRA IMPRINTER
AND A GLASS BOTTLE HOUSING RESONANCE MAGNETIC FIELD WATER IS ARRANGED IN THE
OUT-WALL THEREOF. THE TRANSFER MODE OF THE MRA IMPRINTER IS SET TO THE IN-WELL
AND THE OUT-WELL AND A TRANSFER BUTTON IS PUSHED TO PERFORM TRANSFER.
THEREAFTER, THE GLASS BOTTLE HOUSING THE RESONANCE MAGNETIC FIELD WATER IS
WELL VIBRATED. DISTILLED WATER IS CHARGED IN A GLASS BOTTLE AND THIS BOTTLE IS
SURROUNDED BY FAR INFRARED RAY EMITTING CERAMIC PELLETS. THEN, FENNEL OIL AND
JUNIPER OIL ARE PLACED IN THE IN-WELL OF THE MRA IMPRINTER AND A GLASS BOTTLE
HOUSING WATER IS PLACED IN THE OUT-WALL TO PERFORM TRANSFER TREATMENT.
537/1651
93. JP11246383 - 14.09.1999
ESSENTIAL OIL LIQUID WHICH CAN BE SPRAYED OR APPLIED
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP11246383
Inventor(s):
HASHIGUCHI OSAMU (--)
Applicant(s):
HASHIGUCHI OSAMU (--); HASHIGUCHI HAJIME (--)
IP Class 4 Digits: A61K; C11B; D06M; B01J
IP Class:
A61K7/46; C11B9/00; D06M13/00; B01J13/02; D06M23/12
Application Number:
JP19980063964 (19980227)
Family: JP11246383
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN AN ESSENTIAL OIL LIQUID IN WHICH A SMALL AMOUNT
OF AN ESSENTIAL OIL IS MICROCAPSULATED AND DILUTED FOR STORAGE, AND WHICH CAN
BE SPRAYED TO FIBERS AND SO ON, WHEN DESIRED, AS 'MICROCAPSULE SPRAY'.
SOLUTION: THIS LIQUID IS OBTAINED BY ADDING AN AQUEOUS HINDER TO A SLURRY
PREPARED BY MICROCAPSULATING AN ESSENTIAL OIL FOLLOWED BY DILUTING WITH AN
AQUEOUS SOLUTION SO AS TO BE ABLE TO BE SPRAYED OR APPLIED TO FIBERS AND SO ON.
THE MICROCAPSULE OF THE ESSENTIAL OIL CAN BE A NON-POROUS OR POROUS
MICROCAPSULE, OR A MIXTURE OF THESE. AS THE ESSENTIAL OIL, A PLURALITY OF
ESSENTIAL OILS CAN BE USED IN VARIOUS COMPOSITIONS DEPENDING ON ITS PURPOSE. THE
FIBERS INCLUDE (UNWOVEN) CLOTHES SUCH AS DRESS, BEDDING, PERSONAL EFFECTS, AND
CUSHION IN THE SHOE. THE LIQUID CAN BE SPRAYED ALSO TO A PART OF THE HUMAN BODY.
538/1651
94. JP11279583 - 12.10.1999
ESSENTIAL OIL OF HORTICULTURAL PLANT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP11279583
Inventor(s):
NAGAI SHIGEHIRO (--); GOTO KANAE (--); HAN TADASHI (--); HASEBE AKIO (--)
Applicant(s):
JUMOKU SEIRI KINOUSEI BUSSHITSU GIJUTSU KENKYU KUMIAI (--)
IP Class 4 Digits: C11B; A01N
IP Class:
C11B9/00; A01N65/00
Application Number:
JP19980102208 (19980330)
Family: JP11279583
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE AN ESSENTIAL OIL OF A HORTICULTURAL PLANT
WHICH CAN BE PREPARED BY MEANS OF NO FOREST RESOURCES AS THE ESSENTIAL OIL
RAW MATERIAL, OF WHICH PLANNED PRODUCTION AND CONTROLLED PRODUCTION ARE
POSSIBLE, AND OF WHICH MASS PRODUCTION IS POSSIBLE, REQUIRING A SMALL LABOR AND
A LOW COST.
SOLUTION: THE ESSENTIAL OIL IS PREPARED FROM HORTICULTURAL PLANT BELONGING TO
THE SPECIES MACROCARPA OF THE GENUS CUPRESUS. THE ESSENTIAL OIL IS PREF. A
GOLDCREST ESSENTIAL OIL CONTG., AS THE MAIN COMPONENTS, SABINENE, 4-TERPINEOL,
AND CITRONELLOL, BESIDES MORE PREF. THE GOLD CREST ESSENTIAL OIL CONTG., BASED
ON THE ESSENTIAL OIL COMPONENTS, 15-30 WT.% OF SABINENE, 10-25 WT.% OF 4TERPINEOL, AND 5-10 WT.% OF CITRONELLOL.
539/1651
95. JP1247095 - 02.10.1989
PRODUCTION OF ESSENTIAL OIL COMPONENTS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP1247095
Inventor(s):
SUZUKI CHIHIRO (--); others: 06 (--)
Applicant(s):
NAKANO VINEGAR CO LTD (--)
IP Class 4 Digits: C11B; C12N; C12P
IP Class:
C11B9/00; C12P1/00; C12N5/00
Application Number:
JP19880073144 (19880329)
Family: JP1247095
Abstract:
PURPOSE:TO SIMPLY AND EFFICIENTLY PRODUCE ESSENTIAL OIL BY PROLIFERATING
NUCELLUS CALLUSES INDUCED FROM NUCELLUSES OF A PLANT IN CITRUS FRUITS AND
DIFFERENTIATING ADVENTITIOUS NUCELLUS EMBRYOS, AND ALLOWING THE EMBRYOS TO
GROW BY TISSUE CULTURE.
CONSTITUTION:NUCELLUS CALLUSES ARE INDUCED FROM THE NUCELLUSES OF A PLANT IN
CITRUS FRUITS OR FORTUNELLA AND PROLIFERATED BY THE SHAKING CULTURE OR AEROBIC
CULTURE. THE PROLIFERATED CALLUSES ARE SHAKE-CULTURED OR AERATION-CULTURED IN
A LIQUID MEDIUM FOR THE ADVENTITIOUS NUCELLUS EMBRYO MULTIPLICATION TO
DIFFERENTIATE AND INDUCE ADVENTITIOUS NUCELLUS EMBRYOS. THEN, THE EMBRYOS ARE
SUBJECTED TO SHAKING CULTURE OR AERATION CULTURE IN A LIQUID MEDIUM FOR
ADVENTITIOUS NUCELLUS EMBRYOS AND THE ESSENTIAL OIL IS OBTAINED FROM THE
ADVENTITIOUS NUCELLUS EMBRYOS GROWN THROUGH THREE STEPS.
540/1651
96. JP2000140081 - 23.05.2000
ESSENTIAL OIL FRAGRANCE EMITTING MACHINE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2000140081
Inventor(s):
ORIGASA NOBORU (--)
Applicant(s):
PHOTO KOGEI:KK (--)
IP Class 4 Digits: A61L
IP Class:
A61L9/12; A61L9/01
Application Number:
JP19980353740 (19981106)
Family: JP2000140081
Abstract:
PROBLEM TO BE SOLVED: TO AUTOMATICALLY PERFORM THE EMISSION OF A FRAGRANCE
AND THE STOP, AND EASILY AND QUICKLY ENJOY THE FRAGRANCE, AND AT THE SAME TIME,
PROPERLY PREVENT A WASTEFUL EMISSION OF THE FRAGRANCE FROM OCCURRING, AND
IMPROVE THE ECONOMIC PROPERTY BY ROTATING/STOPPING A FAN MOTOR ACCOMPANYING
AN ON/OFF OPERATION OF A SWITCH, AND AT THE SAME TIME, OPENING/CLOSING A LID.
SOLUTION: A FRAGRANCE EMITTING MACHINE MAIN BODY 1 IS MADE OF A RESIN OR WOOD,
AND A FELT 4 IS PASSED THROUGH AN INTERNAL LID 3 OF AN ESSENTIAL OIL BOTTLE 2
WHICH IS HOUSED IN THE FRAGRANCE EMITTING MACHINE MAIN BODY 1, AND AN ESSENTIAL
OIL IN THE ESSENTIAL OIL BOTTLE 2 IS SUCKED UP BY USING A CAPILLARY TUBE
PHENOMENON. ALSO, A FRAGRANCE LID 10 IS DISPOSED AT THE UPPER PART OF AN
ESSENTIAL OIL INSERT 7 TO WHICH THE ESSENTIAL OIL BOTTLE 2 IS ATTACHED, AND THE
FRAGRANCE LID 10 IS VERTICALLY MOVED BY A SOLENOID VALVE 11. IN ADDITION, WHEN THE
FRAGRANCE LID 10 IS LIFTED, A FAN MOTOR 8 IS ROTATED, AND THE FRAGRANCE IS EMITTED
FROM A FRAGRANCE PORT 12. IN THE MEANTIME, WHEN THE FRAGRANCE LID 10 IS LOWERED
THROUGH THE SOLENOID VALVE 11 BY A SWITCH 9, THE FAN MOTOR 8 IS STOPPED. BY THIS
CONSTITUTION, THE FRAGRANCE IS EMITTED BY A SIMPLE SWITCH OPERATION, AND AT THE
541/1651
SAME TIME, A WASTEFUL EMISSION OF THE FRAGRANCE IS PREVENTED FROM OCCURRING,
AND THE ECONOMIC PROPERTY IS IMPROVED.
542/1651
97. JP2000169823 - 20.06.2000
ADHESIVE USING RESIN OR ESSENTIAL OIL EXTRACTED FROM WOOD AND PRODUCTION OF
THE ADHESIVE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2000169823
Inventor(s):
HASHIMOTO YOTAROU (--); TAKECHI HIDEHIRO (--)
Applicant(s):
EIWA:KK (--); TAKECHI HIDEHIRO (--)
IP Class 4 Digits: C09J; B27M
IP Class:
C09J193/00; B27M3/00
Application Number:
JP19980345930 (19981204)
Family: JP2000169823
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN AN ADHESIVE BY USING A BY-PRODUCT ON A GASEOUS
PHASE TREATMENT FOR TREATING WOOD WITH THE VAPOR OF A SOLUTION CONSISTING
MAINLY OF WATER AND METHYLENE CHLORIDE.
SOLUTION: A RESIN EXTRACTED FROM WOODS WITH A SOLVENT CONSISTING MAINLY OF
WATER AND METHYLENE CHLORIDE IS USED AS AN ADHESIVE FOR COMPILING WOODS. THE
METHYLENE CHLORIDE MAY BE REPLACED WITH ONE OF OTHER CHLORINATED ORGANIC
SOLVENTS. THE METHYLENE CHLORIDE MAY BE REPLACED WITH A HALOGENATED ORGANIC
SOLVENT. A WATER-RECOVERING TANK 5 AND A RECOVERY TANK 3 FOR RECOVERING A
SOLUTION PORTION OOZED FROM THE WOODS, OR THE LIKE, ARE DISPOSED TO RECOVER
THE EXTRACT OF THE WOOD. THE RESIN EXTRACTED FROM THE WOODS WITH A WATERMETHYLENE CHLORIDE CLUSTER PRODUCED IN THE AZEOTROPIC STATE IS USED AS AN
ADHESIVE FOR COMPILING WOODS.
543/1651
98. JP2000212589 - 02.08.2000
PLANT ESSENTIAL OIL-CONTAINING AQUEOUS SOLUTION AND ITS PRODUCTION
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2000212589
Inventor(s):
NISHIMOTO TETSUO (--)
Applicant(s):
COSMO ACE:KK (--)
IP Class 4 Digits: C11B; A61L; A01N; C09K; B01D
IP Class:
C11B9/00; A61L9/01; A01N65/00; C11B9/02; C09K3/00; A01N25/02; B01D47/06
Application Number:
JP19990012129 (19990120)
Family: JP2000212589
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN THE SUBJECT AQUEOUS SOLUTION HAVING NO
TOXICITY, EXCELLENT IN SAFETY AND CAPABLE OF ADSORBING FLOATING PARTICULATE
MATERIALS SUCH AS VARIOUS MICROORGANISMS AND POLLEN PRESENT IN THE INTERIOR OF
A HOUSE BY MIXING A PLANT ESSENTIAL OIL AND A WATER-SOLUBLE FRACTION, OBTAINED
BY A STEAM DISTILLATION, AND WATER IN A SPECIFIC PROPORTION, AND TREATING THE
OBTAINED MIXTURE UNDER A SPECIFIED CONDITION.
SOLUTION: THIS PLANT ESSENTIAL OIL-CONTAINING AQUEOUS SOLUTION IS OBTAINED BY
STEAM-DISTILLING A PLANT SELECTED FROM JAPANESE CYPRESS BORN IN AOMORI
PREFECTURE, CHAMAECYPARIS TAIWANENSIS, TEA PLANT, GINKGO BILOBA,
PHYLLOSTACHYS PUBESCENS, PHYLLOSTACHYS BAMBUSOIDES, SASA ALBO-MARGINATA,
SASA KURILENSIS AND LAVANDULA VERA, MIXING THE PLANT ESSENTIAL OIL AND THE
WATER-SOLUBLE FRACTION OBTAINED BY THE STEAM DISTILLATION WITH WATER IN A
WEIGHT RATIO OF (0.5-2)/(2-4)/(4-8) BY USING A STIRRER, STIRRING THE OBTAINED MIXTURE
WHILE BLOWING A GAS HAVING >=10 VOL.% OXYGEN CONTENT AND JETTING THE MIXTURE
TO PROVIDE A MIXED LIQUID, AND JETTING THE OBTAINED MIXED LIQUID FROM PLURAL
JETTING MEANS SO AS TO COLLIDE WITH EACH OTHER TO PROVIDE THE OBJECTIVE PLANT
544/1651
ESSENTIAL OIL-CONTAINING AQUEOUS SOLUTION. THE MIXED LIQUID OBTAINED BY STIRRING
WHILE JETTING THE LIQUID IS PREFERABLY FURTHER MIXED BY USING THE STIRRER.
545/1651
99. JP2000229121 - 22.08.2000
METHOD FOR CONTROLLING CONCENTRATION OF PLANT ESSENTIAL OIL IN SPACE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2000229121
Inventor(s):
TAKAHASHI YUMIE (--); TAKAHASHI KENICHI (--)
Applicant(s):
ISLAND MAGIC:KK (--)
IP Class 4 Digits: A61L
IP Class:
A61L9/01; A61L9/04
Application Number:
JP19990032861 (19990210)
Family: JP2000229121
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE A METHOD FOR CONTROLLING CONCN. OF A PLANT
ESSENTIAL OIL IN A SPECIFIED SPACE WHICH MAKES THE CONCN. OF THE PLANT ESSENTIAL
OIL TO A SPECIFIED CONCN. IN THE SPECIFIED SPACE BY PREVENTING THE PLANT ESSENTIAL
OIL FROM BEING DECOMPOSED AND CHANGED IN QUALITY CAUSED BY HEATING AND
WARMING AND CONTROLLING ACCURATELY AMT. OF EVAPORATION OF THE PLANT
ESSENTIAL OIL PER UNIT TIME IN ACCORDANCE WITH VOL. OF THE SPACE, VENTILATION
SPEED, ABSORBING SPEED, OR THE LIKE.
SOLUTION: IN THIS METHOD, A PLANT ESSENTIAL OIL DISSOLVED IN A WATER-SOLUBLE
ALCOHOL IS EVAPORATED BY USING AN ULTRASONIC OSCILLATOR AND THE PLANT
ESSENTIAL OIL IS EVAPORATED FROM AN EMULSION LIQ. OF THE PLANT ESSENTIAL OIL OBTD.
BY A METHOD WHEREIN WATER IS INCORPORATED AND THE MIXTURE IS AGITATED AT HIGH
SPEED AND THE PLANT ESSENTIAL OIL IS EVAPORATED BY OPENING A SEALED CONTAINER
WHEREIN A MIXED MATERIAL IN WHICH THE PLANT ESSENTIAL OIL OBTD. IS ADSORBED AND
IMPREGNATED BY USING AT LEAST TWO KINDS OF MATERIALS SELECTED FROM A PLURALITY
OF POROUS MATERIALS AND FIBROUS MATERIALS WITH DIFFERENT ADSORBING AND
IMPREGNATING ABILITIES TO A SPECIFIED PLANT ESSENTIAL OIL IS STORED.
546/1651
100. JP2000239178 - 05.09.2000
PLANT ESSENTIAL OIL COMPOSITION HAVING ANTI-TYPE I ALLERGIC EFFECT AND PREVENTIVE
AND/OR THERAPEUTIC AGENT FOR TYPE I ALLERGY CONTAINING THE COMPOSITION AS
ACTIVE INGREDIENT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2000239178
Inventor(s):
KARITA TAKESHI (--)
Applicant(s):
KARITA TAKAHISA (--)
IP Class 4 Digits: A61K; A61P
IP Class:
A61K35/78; A61P43/00
Application Number:
JP19990334203 (19991125)
Family: JP2000239178
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN A PREVENTIVE AND/OR THERAPEUTIC AGENT FOR TYPE I
ALLERGY WHICH HAS NO ADVERSE DRUG REACTIONS SUCH AS THOSE OF MEDICINES USED
IN THE PAST AND SHOWS HIGH SAFETY.
SOLUTION: THE PLANT ESSENTIAL OIL COMPOSITION HAVING ANTI-TYPE I ALLERGIC EFFECT
IS OBTAINED BY INCLUDING AN ESSENTIAL OIL OBTAINED FROM AT LEAST ONE KIND OF
PLANT BELONGING TO THE FAMILY MYRTACEAE, AN ESSENTIAL OIL OBTAINED FROM AT
LEAST TWO KINDS OF PLANTS BELONGING TO THE FAMILY LABIATAE AND AN ESSENTIAL OIL
OBTAINED FROM AT LEAST ONE KIND OF PLANT BELONGING TO THE FAMILY RUTACEAE. THE
PREVENTIVE AND/OR THERAPEUTIC AGENT FOR TYPE I ALLERGY CONTAINING THIS
COMPOSITION AS AN ACTIVE INGREDIENT IS CAPABLE OF EFFECTIVELY CARRYING OUT
PREVENTION AND/OR TREATMENT FOR TYPE I ALLERGY, BECAUSE THE SYNTHESIS OF LTC4
OR LTD4 IS INHIBITED AND THE SIGNAL TRANSMISSION DUE TO CHEMICAL MEDIATORS
CAUSING TYPE I ALLERGIC REACTION FROM MAST CELLS, OR THE LIKE, IS ALSO INHIBITED.
547/1651
FURTHER, AS THIS THERAPEUTIC AGENT IS A PERCUTANEOUS ABSORBENT, THE DRUG
ADMINISTRATION CAN BE EASILY STOPPED.
548/1651
101. JP2000355545 - 26.12.2000
ESSENTIAL OIL COMPOSITION FOR SLEEP SUPPLEMENTATION AND/ OR INTRODUCTION, AND
AGENT FOR SLEEP SUPPLEMENTATION AND/OR INTRODUCTION
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2000355545
Inventor(s):
KARITA TAKESHI (--)
Applicant(s):
KARITA TAKAHISA (--)
IP Class 4 Digits: A61K; A61P
IP Class:
A61K35/78; A61K9/70; A61K47/04; A61K47/10; A61K47/32; A61K47/36;
A61K47/38; A61P25/20
Application Number:
JP19990163890 (19990610)
Family: JP2000355545
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN THE SUBJECT COMPOSITION AND AGENT CAPABLE OF
QUICKLY IMPROVING A LEVEL OF SLEEP PREPARATORY STATE WITHOUT CAUSING ANY SIDE
EFFECT.
SOLUTION: THIS COMPOSITION IS SUCH AS TO BE COMPOSED OF LAVENDER OIL OR
LAVANDIN OIL, AT LEAST TWO KINDS OF ESSENTIAL OILS SELECTED FROM THE GROUP
CONSISTING OF NEROLI OIL, ORANGE OIL, LEMON OIL AND MANDARIN OIL, AND AT LEAST
ONE KIND OF ESSENTIAL OIL SELECTED FROM THE GROUP CONSISTING OF HOP OIL,
EUCALYPTUS OIL, AMBRETT SEED OIL, GREEN TEA OIL AND JASMINE OIL. THE ESSENTIAL OIL
COMPOSITION AND AGENT EACH FOR SLEEP SUPPLEMENTATION AND/OR INTRODUCTION AS
VAPOROUS PHARMACEUTICAL PREPARATION HAVING AS ACTIVE INGREDIENT AN ESSENTIAL
OIL DERIVED FROM PLANTS CAN QUICKLY DEVELOP AN EFFECT SINCE THEY ARE GIVEN
THROUGH PERCUTANEOUSLY ABSORBING ROUTE AND ALSO QUICKLY STOP A MEDICATION.
FURTHERMORE, THEY ARE HIGHLY SAFE WITHOUT CAUSING ANY SIDE EFFECT BECAUSE THE
ACTIVE INGREDIENT THEREOF IS AN ESSENTIAL OIL COMPOSITION.
549/1651
102. JP2001031515 - 06.02.2001
COMPOSITION INCLUDING FRAGRANT ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2001031515
Inventor(s):
ECHIGO KEIKO (--); ISHII TETSUYA (--); TAKOSHI HIROTAKA (--)
Applicant(s):
SHOWA DENKO KK (--)
IP Class 4 Digits: C11B; A01N
IP Class:
C11B9/00; A01N65/00; A01N27/00; A01N25/02; A01N25/10; A01N25/22;
A01N25/30; A01N31/02; A01N35/02
Application Number:
JP19990201417 (19990715)
Family: JP2001031515
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN A REPELLENT CAPABLE OF EASILY HANDLING,
RETAINING ITS REPELLENT ACTION FOR A LONG TIME ON A NOXIOUS ANIMAL ESPECIALLY TO
CATS, AND THE LIKE, BY USING A COMPOSITION INCLUDING A FRAGRANT ESSENTIAL OIL.
SOLUTION: THIS REPELLENT COMPRISING A COMPOSITION INCLUDING A FRAGRANT
ESSENTIAL OIL COMPRISES (A) A (CO)POLYMER OR A CROSSLINKED PRODUCT OF THE
(CO)POLYMER OBTAINED FROM A MONOMER EXPRESSED BY THE FORMULA: CH2=CH-NR1COR2 (R1 AND R2 ARE INDEPENDENTLY H, METHYL OR MECTUALLY BOND TO FORM A 3-5C
ALKYLENE GROUP), (B) A TERPENOID COMPOUND AND (C) A SURFACTANT AND/OR A WATERSOLUBLE ORGANIC SOLVENT.
550/1651
103. JP2001031579 - 06.02.2001
ESSENTIAL OIL COMPOSITION FOR PREVENTION OF EDEMA AND EDEMA PREVENTING AGENT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2001031579
Inventor(s):
KARITA TAKESHI (--)
Applicant(s):
KARITA TAKAHISA (--)
IP Class 4 Digits: A61K; C11B
IP Class:
A61K35/78; C11B9/00; A61K9/70; A61K31/00
Application Number:
JP19990202605 (19990716)
Family: JP2001031579
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN AN ESSENTIAL OIL COMPOSITION FOR PREVENTION OF
EDEMA OF HIGH EFFECTIVENESS WITHOUT SIDE-EFFECT AND AN EDEMA PREVENTING AGENT.
SOLUTION: THE OBJECTIVE ESSENTIAL OIL COMPOSITION HAVING AN EFFECT OF EDEMA
PREVENTION IS PREPARED BY USING AT LEAST ONE ESSENTIAL OIL SELECTED FROM
LAVENDER, LAVANDIN, EUCALYPTUS, MANDARINE, ORANGE AND LEMON OILS, FURTHER,
VIOLET OIL OR SANDAL OIL. THE EDEMA PREVENTING AGENT COMPRISING ESSENTIAL OIL
COMPOSITION IS A HIGH-SAFETY EVAPORATIVE PREPARATION INCLUDING VEGETABLE
ESSENTIAL OILS.
551/1651
104. JP2001098296 - 10.04.2001
DETERGENT USING AROMATIC ESSENTIAL OIL-CONTAINING COMPOSITION
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2001098296
Inventor(s):
ECHIGO KEIKO (--); ISHII TETSUYA (--); TAKOSHI HIROTAKA (--)
Applicant(s):
SHOWA DENKO KK (--)
IP Class 4 Digits: C11D
IP Class:
C11D7/50
C11D3/50; C11D3/18; C11D3/20; C11D3/37; C11D7/24; C11D7/26; C11D7/32;
Application Number:
JP19990278720 (19990930)
Family: JP2001098296
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE A DETERGENT USING A NOVEL AROMATIC ESSENTIAL
OIL-CONTAINING COMPOSITION WHICH IS POSSIBLE TO EASILY HANDLE THE DETERGENT
AND TO SHOW EFFECTIVE DETERGENCY TO AN OILY STAIN OR THE LIKE TO BE HARD TO
COME OUT.
SOLUTION: THIS DETERGENT COMPRISES (A) A (CO)POLYMER AND/OR A CROSSLINKED
PRODUCT OF THE (CO)POLYMER OBTAINED FROM A MONOMER REPRESENTED BY THE
FOLLOWING GENERAL FORMULA: CH2=CH-NR1-COR2 (WHEREIN R1 AND R2 ARE
INDEPENDENTLY HYDROGEN, A METHYL GROUP OR A 3-5C ALKYLENE GROUP), (B) A TERPENE
COMPOUND AND (C) A SURFACTANT AND/OR A WATER-SOLUBLE ORGANIC SOLVENT AS
EFFECTIVE COMPONENTS.
552/1651
105. JP2001114619 - 24.04.2001
ESSENTIAL OIL FOR AROMATHERAPY AND METHOD FOR USING THE SAME
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2001114619
Inventor(s):
MORITA ATSUKO (--); SHIMANO KAZUHIRO (--)
Applicant(s):
ST LOUIS INTERNATIONAL INC (--); SHIMANO:KK (--)
IP Class 4 Digits: A01N
IP Class:
A01N65/00; A01N63/00; A01N25/00; A01N25/06
Application Number:
JP19990292102 (19991014)
Family: JP2001114619
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN AN ESSENTIAL OIL FOR AROMATHERAPY, CAPABLE OF
EXHIBITING NOT ONLY HEALING AND RELAXATION EFFECTS OF BODY AND SPIRIT BY THE
PERFUME OF THE ESSENTIAL OIL BUT ALSO ANTIMICROBIAL EFFECTS SUFFICIENTLY, AND
FURTHER TO PROVIDE A METHOD FOR USING THE ESSENTIAL OIL WHEN SCATTERING THE
ESSENTIAL OIL IN A ROOM.
SOLUTION: THIS ESSENTIAL OIL FOR THE AROMATHERAPY IS PREPARED BY ADDING A
NATURAL EXTRACTED ANTIMICROBIAL AGENT COMPRISING PHYTOALEXIN, PRODUCED BY A
PLANT BY USING A CHITIN OR A CHITOSAN AS AN ELICITOR, TO A NATURAL VEGETABLE
ESSENTIAL OIL. THE ESSENTIAL OIL IS ATOMIZED TO FINE PARTICLE SHAPE HAVING 1-5 MU M
AVERAGE PARTICLE DIAMETER BY USING A DEFUSER OR THE LIKE OF AN ULTRASONICALLY
VIBRATING AND ATOMIZING TYPE, AND SCATTERING THE ATOMIZED FINE PARTICLES IN THE
ROOM.
553/1651
106. JP2001137608 - 22.05.2001
METHOD AND DEVICE FOR EXTRACTING ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2001137608
Inventor(s):
UEDA MAKIKO (--)
Applicant(s):
SHIKOKU ELECTRIC POWER CO INC (--); SHIKOKU RES INST INC (--)
IP Class 4 Digits: B01D
IP Class:
B01D9/04; B01D9/02; B01D17/025
Application Number:
JP19990325009 (19991116)
Family: JP2001137608
Abstract:
PROBLEM TO BE SOLVED: TO EXTRACT AN ESSENTIAL OIL EVEN AT A LOW TEMP. WITHOUT
USING A SOLVENT.
SOLUTION: THE ESSENTIAL OIL IS EXTRACTED BY FREEZING A LIQUID RAW MATERIAL 1
CONTAINING THE ESSENTIAL OIL HAVING A MELTING POINT OF <0 DEG.C AT A FREEZING
TEMPERATURE BETWEEN 0 DEG.C TO THE MELTING POINT OF THE ESSENTIAL OIL,
DEFROSTING THE FROZEN RAW MATERIAL 1 AND UTILIZING THE DIFFERENCE OF THE
SPECIFIC GRAVITY BETWEEN THE DEFROSTED ESSENTIAL OIL AND RAW MATERIAL POTION 7.
554/1651
107. JP2001139488 - 22.05.2001
ANALGESIC ESSENTIAL OIL COMPOSITION AND ANALGESIC
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2001139488
Inventor(s):
KARITA TAKESHI (--)
Applicant(s):
KARITA TAKAHISA (--)
IP Class 4 Digits: A61K; A61P
IP Class:
A61K35/78; A61P29/02
Application Number:
JP19990322645 (19991112)
Family: JP2001139488
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE AN ANTIPHLOGISTIC SEDATIVE AGENT NOT HAVING
ADVERSE EFFECTS SUCH AS GASTROINTESTINAL DISTURBANCE AND DRUG DEPENDENCE
WHICH ANTIPYRETIC ANALGESICS AND MORPHINE-LIKE ANALGESICS WHICH HAVE BEEN
USED HITHERTO HAVE.
SOLUTION: THIS ANTIPHLOGISTIC SEDATIVE AGENT RAPIDLY EXHIBITING EFFECT ON PAIN
CAUSED BY VARIOUS DISEASES AND HAVING HIGH SAFETY IS PROVIDED BY FORMING AN
ANALGESIC ESSENTIAL OIL COMPOSITION COMPRISING AT LEAST ONE KIND OF ESSENTIAL
OIL SELECTED FROM A GROUP CONSISTING OF ORANGE OIL, GRAPEFRUIT OIL, MANDARINE
OIL AND LEMON OIL, AT LEAST ONE KIND OF ESSENTIAL OIL SELECTED FROM A GROUP
CONSISTING OF LAVENDER OIL, LAVANDIN OIL AND ROSEMARY OIL AND AT LEAST ONE KIND
OF ESSENTIAL OIL SELECTED FROM A GROUP CONSISTING OF EUCALYPTUS OIL, CHAMOMILE
OIL, TAIWAN HINOKI AND MUGWORT OIL INTO A SHEET-LIKE PARMACEUTICAL PREPARATION.
555/1651
108. JP2001151602 - 05.06.2001
POLYMERIC MICRO PARTICLE CONTAINING ESSENTIAL OIL OF TREE AND WAX COMPOSITION
INCLUDING THE SAME
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2001151602
Inventor(s):
INUI HAJIME (--)
Applicant(s):
NIPPON PAPER INDUSTRIES CO LTD (--); PAL CO LTD (--)
IP Class 4 Digits: A01N; C08J; C08L
IP Class:
C08L101/00
A01N65/00; A01N3/04; A01N25/24; A01N27/00; C08J3/12; C08L91/06;
Application Number:
JP20000247254 (20000817)
Family: JP2001151602
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN A WAX COMPOSITION MAINTAINING SEVERAL EFFECTS
OF ESSENTIAL OIL COMPONENT FOR LONG TIME.
SOLUTION: THIS POLYMERIC PARTICLE 1 IS OBTAINED BY IMPREGNATING AND MAINTAINING
DIFFERENT ESSENTIAL OILS OF TREES IN VINYL ACETATE-BASED POLYMERIC PARTICLE 4 AND
5 AND PREFERABLY FORMING A SHELL 2 AT OUTSIDE OF THE PARTICLE WHEREIN THE
ESSENTIAL OILS HAVE SAME OR RESEMBLING MOLECULAR WEIGHT AND MOLECULAR
FORMULA AND DIFFERENT STRUCTURE AND ANOTHER SUBJECT WAX COMPOSITION IS AN
ACRYLIC RESIN-BASED WAX OBTAINED BY ADDING AND MIXING THE POLYMERIC PARTICLE.
556/1651
109. JP2001213701 - 07.08.2001
ESSENTIAL OIL CONTAINING DRY ICE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2001213701
Inventor(s):
HENMI MAKOTO (--); YAMASAKI SATOSHI (--)
Applicant(s):
EKIKA TANSAN KK (--)
IP Class 4 Digits: A61L; A01N
IP Class:
A61L9/01; A01N65/00; A01N1/00; A01N59/04
Application Number:
JP20000022292 (20000131)
Family: JP2001213701
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE AN ANTIBACTERIAL DEODORANT APPLICABLE TO
WASTE FROM ORGANISM, EXCREMENT AND CARCASS OF ANIMAL AND CORPSE OF HUMAN
BEING WHICH TURN INTO A BAD SMELL GENERATION SOURCE THROUGH DECOMPOSITION.
SOLUTION: THE ANTIBACTERIAL DEODORANT WHEREIN AN ESSENTIAL OIL HAVING
ANTIBACTERIAL PROPERTY AGAINST BACTERIA IS INVOLVED IN DECOMPOSITION, IS
CONTAINED IN DRY ICE.
557/1651
110. JP2002038187 - 06.02.2002
METHOD FOR MODIFYING ESSENTIAL OIL OF PLANT BELONGING TO GENUS MENTHA OF
FAMILY LABIATAE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2002038187
Inventor(s):
HARADA YASUHIRO (--); OBARA HITOSHI (--); NISHIMURA OSAMU (--)
Applicant(s):
OGAWA and CO LTD (--)
IP Class 4 Digits: A61K; C11B; A23L; A23G
IP Class:
C11B9/02; A23L1/221; A61K47/44; A61K7/00; A23L2/38; A23G3/30; A23L2/00
Application Number:
JP20000228857 (20000728)
Family: JP2002038187
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE A METHOD FOR MODIFYING FLAVOR OF MINT
ESSENTIAL OILS COLLECTED FROM PLANTS BELONGING TO THE GENUS MENTHA OF THE
FAMILY LABIATAE BY STEAM DISTILLATION METHOD IN ORDER TO USE THESE OILS FOR
FOODS, FRAGRANCES AND COSMETICS AND MEDICINES WITHOUT GIVING A SENSE OF
IMCOMPATIBILITY.
SOLUTION: THIS METHOD FOR MODIFYING AN ESSENTIAL OIL OF A PLANT BELONGING TO
THE GENUS MENTHA OF THE FAMILY LABIATAE COMPRISES CARRYING OUT MOLECULAR
DISTILLATION OF ESSENTIAL OIL OF THE PLANT BELONGING TO THE GENUS MENTHA OF THE
FAMILY LABIATAE COLLECTED BY A STEAM DISTILLATION METHOD. IN THE ABOVE METHOD,
THE LIQUID TO BE TREATED IS PREFERABLY VAPORIZED IN A THICKNESS OF THIN FILM OF
0.05-5.0 MM AT 40-100 DEG.C UNDER 0.001-10.0 MM HG PRESSURE FOR 0.1-5.0 SEC HEATING
TIME.
558/1651
111. JP2002114605 - 16.04.2002
METHOD FOR BIODEGRADABLE MICROENCAPSULATION OF NATURAL VEGETABLE ESSENTIAL
OIL AND BIODEGRADABLE MICROENCAPSULATED FORMULATION
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2002114605
Inventor(s):
TEI SHOSO (--); BUN ZENCHU (--); KO SHOICHI (--); KIM YONIKKU (--); LEE
SAIKYU (--); KIM YOKYU (--); SEI SHUNKI (--)
Applicant(s):
BIG:KK (--)
IP Class 4 Digits: A01N; C05G
IP Class:
A01N65/00; A01N25/10; A01N25/28; C05G3/00; C05G3/02
Application Number:
JP20010250006 (20010821)
Family: JP2002114605
Equivalent:
KR2000072238
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN A FORMULATION CAPABLE OF REDUCING THE LOSS OF
A CHEMICAL DUE TO VOLATILIZATION, MASKING A PECULIAR SMELL, IMPROVING THE
USABILITY, REGULATING THE RELEASE, RETAINING EFFICACIES FOR A LONG PERIOD, HAVING
FUNGICIDAL AND INSECTICIDAL ACTIONS AND SIMULTANEOUSLY ACTING ALSO AS A
FERTILIZER AFTER BIODEGRADATION BY APPLYING A MICROENCAPSULATING METHOD TO A
NATURAL BIOTIC AGROCHEMICAL.
SOLUTION: THIS METHOD FOR BIODEGRADABLE MICROENCAPSULATION OF A NATURAL
VEGETABLE ESSENTIAL OIL COMPRISES A STEP OF PREPARING AN AQUEOUS SOLUTION OF
STARCH SUBJECTED TO SUBSTITUTION TREATMENT WITH N-OCTENYL SUCCINATE AND
HAVING 50,000-150,000 MOLECULAR WEIGHT, A STEP OF ADDING THE NATURAL VEGETABLE
ESSENTIAL OIL WHICH IS A FUNGICIDAL AND INSECTICIDAL INGREDIENT IN AN AMOUNT OF
0.1-100 PTS.WT. BASED ON 100 PTS.WT. OF THE AQUEOUS SOLUTION OF THE SUBSTITUTED
559/1651
STARCH, EMULSIFYING THE ESSENTIAL OIL AND PREPARING AN EMULSION, A STEP OF
ADDING A CROSSLINKING AGENT TO THE RESULTANT EMULSION, CARRYING OUT
POLYMERIZING REACTION AND PROVIDING A MICROCAPSULE SLURRY AND A STEP OF
CONTINUOUSLY SPRAY-DRYING THE SLURRY. THE MICROCAPSULE FORMULATION IS
OBTAINED BY THIS METHOD.
560/1651
112. JP2002308715 - 16.10.2002
MITICIDAL ESSENTIAL OIL MIXTURES AND MITICIDAL SPRAY
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2002308715
Inventor(s):
OHTA HIDEAKI (JP); SUETOMI AKITAKA (JP); MISHIMA YASUTAKA (JP)
Applicant(s):
TAKASAGO PERFUMERY CO LTD (JP); UBE MATERIAL IND LTD (JP)
IP Class 4 Digits: A01N
IP Class:
A01N65/00
E Class: A01N65/00; A01N65/00+M
Application Number:
EP20020290895 (20020410)
Priority Number: JP20010112185 (20010411)
Family: EP1249167
Equivalent:
US2002176899
Cited Document(s):
EP0737479; DE19824683; WO0101782; CH688787; JP4305505;
JP2002053415; JP2251669; JP2001031508
Description:
FIELD OF THE INVENTION
561/1651
[0001] This invention relates to a miticide which contains natural essential oil as the active
ingredient.
BACKGROUND OF THE INVENTION
[0002] It is known that certain aromatic raw materials and natural essential oils and terpene
compounds contained therein have mite-repelling effect or miticide effect.
[0003] For example, JP-A-5-178712 discloses mite-repelling effect by aromatic raw materials such
as benzyl formate, benzyl acetate, benzyl propionate, benzyl butyrate, benzyl valerate, benzyl
caproate, benzyl phenyl ketone and benzophenone, terpene compounds such as linalool and
limonene, and natural essential oils such as lemongrass oil, geranium oil, rosemary oil, laurel oil,
peppermint oil, spearmint oil, lavender oil, caraway oil, cassia oil, calamus oil, fennel oil and thyme oil.
[0004] Since natural essential oils are substances having extremely high safety for human bodies, it
is desirable if mites can be controlled using natural essential oils. However, according to studies
carried out by the present inventors, it was revealed that when a natural essential oil is applied to a
habitat of mites in an amount by which high miticide effect can be obtained, the smell of the natural
essential oil in its surroundings becomes extremely strong which causes a tendency to give its user
and those around the site unpleasant feeling.
SUMMARY OF THE INVENTION
[0005] An object of the invention is to provide a miticide which hardly gives unpleasant feeling to
users when it is applied in an amount by which sufficient miticide effect can be obtained.
[0006] The present invention provides the following invention.
(1) An essential oil mixture for miticide, which comprises
eucalyptus oil or rosemary oil or a mixture thereof and
a mint oil
562/1651
in amounts within a range of from 1:4 to 1:99 by mass ratio.
(2) The essential oil mixture for miticide
according to (1) above, wherein the mint oil is peppermint oil.
(3) A miticide composition which comprises an essential oil mixture for miticide comprising
eucalyptus oil or rosemary oil or a mixture thereof and
a mint oil
in amounts within a range of from 1:4 to 1:99 by mass ratio.
(4) The miticide composition according to (3) above, wherein the mint oil is peppermint oil.
(5) A miticide composition which comprises a solvent and an essential oil mixture for miticide
dissolved in said solvent, said essential oil mixture for miticide comprising
eucalyptus oil or rosemary oil or a mixture thereof and
a mint oil
in amounts within a range of from 1:4 to 1:99 by mass ratio.
(6) The miticide composition according to (5)
above, wherein a content of the essential oil mixture for miticide is within a range of from 3 to 20%
by mass based on the total amount of the miticide composition.
(7) The miticide composition according to (5) above, wherein the mint oil is peppermint oil.
(8) A spray for miticide, which comprises a closed container having a spray nozzle and the miticide
composition of any one of (3) to (7) above packed therein.
DETAILED DESCRIPTION OF THE INVENTION
[0007] The essential oil mixture for miticide of the invention is characterized in that it contains
eucalyptus oil or rosemary oil or a mixture thereof, and a mint oil. That is, it is characterized in that it
contains a mint oil which has excellent miticide effect, among natural essential oils, and eucalyptus
oil and/or rosemary oil which promote the miticide effect of the mint oil.
[0008] A mixing ratio of the eucalyptus oil or rosemary oil or a mixture thereof with the mint oil is
within a range of from 1:4 to 1:99 (eucalyptus oil or rosemary oil or a mixture thereof:mint oil) by mass
ratio, preferably within a range of from 1:4 to 1:30, more preferably within a range of from 1:5 to 1:25.
563/1651
[0009] A mixing ratio in the case of using eucalyptus oil and rosemary oil may be selected in the
appropriate range.
[0010] As the mint oil, peppermint oil, a distilled oil (an essential oil obtained by distilling mint), a
dementholized oil (an essential oil after precipitation of menthol from the distilled oil), spearmint oil
and the like can be used alone or as a mixture of two or more. Among these mint oils, it is desirable
to use peppermint oil or spearmint oil, and particularly desirable to use peppermint oil.
[0011] The essential oil mixture for miticide of the invention may contain a natural essential oil other
than the above natural essential oils and a terpene compound.
[0012] Examples of the natural essential oil include almond bitter oil, caraway oil, ho oil, bay oil,
clove oil, cassia oil, ylang-ylang oil, geranium oil, fennel oil, sage oil, perilla oil, bois de rose oil and
the like.
[0013] Examples of the terpene compound include linalool, anethole, carvone, benzaldehyde,
benzyl alcohol, eugenol, dihydromyrcenol, cineol, camphor, methyl anthranilate, geraniol, limonene,
thymol, paraisopropylanisole, citral, borneol and the like.
[0014] When the essential oil mixture for miticide of the invention is applied to a habitat of mites, it
is desirable to apply it by dissolving in a medium.
[0015] Examples of the medium include solvents and the like.
[0016] As the solvent, one or more of alcohols such as ethyl alcohol, isopropyl alcohol, ethylene
glycol, glycerol, propylene glycol, dipropylene glycol and 1,3-butylene glycol, or a mixed solution of
these solvents with water, can be used.
[0017] The content of the essential oil mixture for miticide of the invention to be contained in the
solvent is generally within a range of from 3 to 20% by mass, preferably within a range of from 5 to
20% by mass, more preferably within a range of from 9 to 12% by mass (based on the total amount
of the composition).
[0018] The solvent containing the essential oil mixture for miticide of the invention, that is, miticide
composition is generally used by packing in a closed container having a spray nozzle such as spray
564/1651
can. Known gas such as methyl fluoride, isobutane, carbon dioxide, liquefied petroleum gas or
dimethyl ether can be used as the propellant.
EXAMPLE 1
[0019] The miticide effect was evaluated on the following essential oil solutions (A) to (C).
(1) Essential oil solution (A)
An essential oil mixture was obtained by mixing eucalyptus oil and peppermint oil at a weight ratio of
1:5. Next, 12 parts by mass of this essential oil mixture was mixed with 88 parts by mass of 95% by
volume ethanol aqueous solution to obtain the essential oil solution (A).
(2) Essential oil solution (B)
An essential oil mixture was obtained by mixing rosemary oil and peppermint oil at a weight ratio of
1:5. Next, 12 parts by mass of this essential oil mixture was mixed with 88 parts by mass of 95% by
volume ethanol aqueous solution to obtain the essential oil solution (B).
(3) Essential oil solution (C)
[0020] An essential oil solution (C) was obtained by mixing 13 parts by mass of peppermint oil with
87 parts by mass of 95% by volume ethanol aqueous solution.
Evaluation method of miticide effect
[0021] A total of 50 individuals of the mite to be tested (belonging to Dermatophagoides: female)
were allowed to crawl on a 10 cm x 10 cm filter paper (mfd. by Advantech, No. 5C). Each of the
essential oil solutions was sprayed on the filter surface side where the mite individuals to be tested
were allowed to crawl. Immediately after the spraying, weight of the filter paper was weighed and the
increased weight was used as the sprayed amount of the essential oil solution. Next, the filter paper
was folded in two, and the opening three sides were fastened with eye clips. After 30 minutes or 24
565/1651
hours of the spraying of the essential oil solution, the filter paper was opened to count the number of
resting mite individuals (knocked down numbers).
[0022] After counting knocked down numbers after 24 hours, the resting mite individuals were
transferred onto another filter paper free from the essential oil solution. Thereafter, knocked down
numbers after 24 hours of resting (the number of mite individuals still under resting state) were
counted to be used as the number of deaths. During the testing period, the temperature in the test
room was from 23.9 to 27.8 DEG C (24.6 DEG C in average) and the humidity was from 52 to 64%
RH (57.3% RH in average). In a control plot, the same operation was carried out except that the
essential oil solution was not sprayed on the filter paper. In this connection, the test was carried out
three times.
[0023] The sprayed amount of essential oil solution in each test and the knockdown ratio (%), death
rate and average death rate (%) calculated based on the following formulae are shown in Table 1.
Knockdown ratio (%) = knocked down numbers/the number
of mites tested (50 individuals) x 100
Death rate (%) = the number of deaths/ the number of
mites tested (50 individuals) x 100
Id=TABLE 1 Columns=7
Head Col 1 AL=L: Essential oil solution
Head Col 2: Test No.
Head Col 3: Sprayed amount of essential oil solution (g)
Head Col 4 to 5: Knockdown ratio (%)
Head Col 6: Death rate (%)
Head Col 7: Average death rate (%)
SubHead Col 1:
SubHead Col 2:
SubHead Col 3:
SubHead Col 4: after 30 min
SubHead Col 5: after 24 hr
Essential oil solution (A) (mint oil-eucalyptus oil solution)10.4631009696
566/1651
20.3981009494
30.424100969695.3
Essential oil solution (B) (mint oil-rosemary oil solution)10.4121009494
20.3981009898
30.418100909094.0
Essential oil solution (C) (mint oil solution)10.4401009494
20.431100100100
30.436100909094.7
Control plot1-000
2-000
3-0020.7
EXAMPLE 2
[0024] Sensory test of the essential oil solutions (A) to (C) prepared in Example 1 was carried out.
[0025] The sensory test was carried out by asking five testers (A, B, C, D and E) to decide ranking
of smells of the essential oil solutions (A) to (C) in preferred order, and the results were evaluated by
the total of the ranking (smaller total means superior result). The results are shown in Table 2.
Id=TABLE 2 Columns=7
Head Col 1 AL=L: Essential oil solution
Head Col 2 to 6: Ranking decided by testers
Head Col 7: Total ranking
SubHead Col 1:
SubHead Col 2: A
SubHead Col 3: B
SubHead Col 4: C
SubHead Col 5: D
SubHead Col 6: E
Essential oil solution (A) (mint oil-eucalyptus oil solution)212319
567/1651
Essential oil solution (B) (mint oil-rosemary oil solution)131128
Essential oil solution (C) (mint oil solution)3232313
EXAMPLE 3
[0026] An essential oil mixture was obtained by mixing eucalyptus oil and peppermint oil at a
weight ratio of 1:23. Next, 12 parts by mass of this essential oil mixture was mixed with 88 parts by
mass of 95% by volume ethanol aqueous solution to obtain an essential oil solution (D). When the
miticide effect of this essential oil solution (D) was evaluated, similar effect of the essential oil
solutions (A) to (C) was obtained. Also, as a result of the sensory test carried out by five testers, four
testers answered that it smelled sweeter than the essential oil solution (C) (mint oil solution).
EXAMPLE 4
[0027] An essential oil mixture was obtained by mixing eucalyptus oil and peppermint oil at a
weight ratio of 1:11. Next, 12 parts by mass of this essential oil mixture was mixed with 88 parts by
mass of 95% by volume ethanol aqueous solution to obtain an essential oil solution (E). When the
miticide effect of this essential oil solution (E) was evaluated, similar effect of the essential oil
solutions (A) to (C) was obtained. Also, as a result of the sensory test carried out by five testers, four
testers answered that it smelled sweeter than the essential oil solution (C) (mint oil solution).
EXAMPLE 5
[0028] An essential oil mixture was obtained by mixing rosemary oil and peppermint oil at a weight
ratio of 1:11. Next, 12 parts by mass of this essential oil mixture was mixed with 88 parts by mass of
95% by volume ethanol aqueous solution to obtain an essential oil solution (F). When the miticide
effect of this essential oil solution (F) was evaluated, similar effect of the essential oil solutions (A) to
568/1651
(C) was obtained. Also, as a result of the sensory test carried out by five testers, four testers
answered that it smelled sweeter than the essential oil solution (C) (mint oil solution).
[0029] Though examples of the use of peppermint oil as a mint oil have been described in the
foregoing, similar effect can also be obtained when a mint-distilled oil, a dementholized oil or
spearmint oil is used instead of peppermint oil.
[0030] Since the essential oil mixture and miticide composition of the invention use natural essential
oils as the active ingredients, they have high safety for human bodies and hardly give users
unpleasant feeling when used until exerting the miticide effect. Accordingly, the essential oil mixture
for miticide and miticide composition of the invention can be used suitably for exterminating mites
inhabiting places such as mats, rugs, carpets, sofas, mattresses and bedclothes which contact
directly with human bodies.
[0031] The term "mass", "by mass ratio", and "part(s) by mass" as used in this specification has the
same meaning with "weight", "by weight ratio", and "part(s) by weight", respectively.
[0032] While the invention has been described in detail and with reference to specific
embodiments thereof, it will be apparent to one skilled in the art that various changes and
modifications can be made therein without departing from the scope thereof.Claims:
1. An essential oil mixture for miticide, which comprises
eucalyptus oil or rosemary oil or a mixture thereof and
a mint oil
in amounts within a range of from 1:4 to 1:99 by mass ratio.
2. The essential oil mixture for miticide according to claim 1, wherein the mint oil is peppermint oil.
3. A miticide composition which comprises an essential oil mixture for miticide comprising
eucalyptus oil or rosemary oil or a mixture thereof and
a mint oil
in amounts within a range of from 1:4 to 1:99 by mass ratio, and at least an appropriate medium.
569/1651
4. The miticide composition according to claim 3, wherein the mint oil is peppermint oil.
5. A miticide composition which comprises a solvent and an essential oil mixture for miticide
dissolved in said solvent, said essential oil mixture for miticide comprising
eucalyptus oil or rosemary oil or a mixture thereof and
a mint oil
in amounts within a range of from 1:4 to 1:99 by mass ratio.
6. The miticide composition according to claim 5, wherein a content of the essential oil mixture for
miticide is within a range of from 3 to 20% by mass based on the total amount of the miticide
composition.
7. The miticide composition according to claim 5 or 6, wherein the mint oil is peppermint oil.
8. A spray for miticide, which comprises a closed container having a spray nozzle and the miticide
composition of any one of claims 3 to 7 packed therein.
570/1651
113. JP2002322023 - 08.11.2002
ESSENTIAL OIL-REMOVED ALPINIA URAIENSIS HAY LIQUID AND METHOD FOR PRODUCING
THE SAME
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2002322023
Inventor(s):
GUSHIKEN TSUTOMU (--); MOROKIDA SAKAE (--); NAGO TOMOKAZU (--); HIGA
YOSHIHIRO (--)
Applicant(s):
GUSHIKEN TSUTOMU (--); HIGA HIDETO (--)
IP Class 4 Digits: A61K
IP Class:
A61K7/00
Application Number:
JP20010125936 (20010424)
Family: JP2002322023
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN AN ESSENTIAL OIL-REMOVED ALPINIA URAIENSIS HAY
LIQUID PRODUCED BY EFFECTIVELY REMOVING THE ESSENTIAL OILS AND THE FLAVOR
COMPONENTS FROM A DISTILLATE OF THE TERRESTRIAL PART OF ALPINIA URAIENSIS HAY, TO
PROVIDE A METHOD FOR PRODUCING THE SAME, AND APPLICATION TO COSMETICS, OR THE
LIKE.
SOLUTION: THE ALPINIA URAIENSIS HAY DISTILLATE IS OBTAINED FROM THE TERRESTRIAL
PARTS OF ALPINIA URAIENSIS HAY THROUGH A METHOD SUCH AS CARBONIZATION,
DISTILLATION UNDER REDUCED PRESSURE OR STEAM DISTILLATION, AND THE VOLATILE
PART IS SEPARATED BY A SEPARATING FUNNEL, AN OIL SEPARATOR, OR THE LIKE.
SUCCESSIVELY, THE FLAVOR COMPONENT IS REMOVED BY ABSORPTION WITH ACTIVE
CARBON, OR THE LIKE FROM THE ESSENTIAL OIL-REMOVED LIQUID. ALTERNATIVELY, BY
ADDING AN ALCOHOL TO THE LIQUID AND HEATING THE MIXTURE, THE REMAINING
ESSENTIAL OILS AND FLAVOR COMPONENTS ARE DISSIPATED TOGETHER WITH THE ALCOHOL.
571/1651
114. JP2003183690 - 03.07.2003
METHOD FOR EXTRACTING MATERIAL HAVING HIGH CONTENT OF PERICARP ESSENTIAL OIL
OF SHEKWASHA (CITRUS DEPRESSA HAYATA) AND POWDER THEREOF
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2003183690
Inventor(s):
KANESHIRO EMIKO (--)
Applicant(s):
OGIMISON (--)
IP Class 4 Digits: C11B; A23L
IP Class:
C11B9/02; A23L1/222; A23L1/30; C11B15/00
Application Number:
JP20020005831 (20020115)
Family: JP2003183690
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE A METHOD FOR EXTRACTING MATERIAL HAVING A
HIGH SONTENT OF A PERICARP ESSENTIAL OIL OF SHEKWASHA BY WHICH THE PERICARP
ESSENTIAL OIL IS INEXPENSIVELY EXTRACTED IN HIGH CONCENTRATION FROM A FRUIT OF
THE SHEKWASHA IN A SHAPE USABLE AS A FOOD ADDITIVE.
SOLUTION: THE FRUIT OF THE SHEKWASHA IS CLEANED AND SQUEEZED, AND THE SQUEEZED
RESIDUE IS REMOVED. THE SEPARATED SQUEEZED JUICE IS SUBJECTED TO CENTRIFUGAL
SEPARATION BY A CENTRIFUGAL SETTLING TYPE SEPARATOR, AND A VISCOUS ATTACHMENT
ATTACHED TO A TREATING VESSEL AND A SEPARATION WALL OF THE SEPARATOR IS
COLLECTED AS THE MATERIAL HAVING THE HIGH CONTENT OF THE PERICARP ESSENTIAL OIL
OF THE SHEKWASHA.
572/1651
115. JP2003190267 - 08.07.2003
PERSISTENT ESSENTIAL OIL AROMATIC COMPOSITION
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2003190267
Inventor(s):
KANEMATSU SHINICHIRO (--); KAKINUMA FUMIKO (--)
Applicant(s):
GURITTA:KK (--)
IP Class 4 Digits: A61K; C11B; A61L; C08L
IP Class:
A61K7/46; C11B9/00; A61L9/01; A61L9/02; A61L9/04; C08L25/04; C08L91/00
Application Number:
JP20010396552 (20011227)
Family: JP2003190267
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE A MEANS CAPABLE OF STABLY AND ECONOMICALLY
EMITTING AROMA OF ESSENTIAL OIL TO THE INDOOR SPACE OVER A LONG PERIOD OF TIME.
SOLUTION: ESSENTIAL OIL IS MIXED WITH COMPOSITION MANUFACTURED BY MIXING A
SOFTENER AND/OR PLASTICIZER WITH STYRENE BASE PLASTIC ELASTOMER TO PREPARE
UNIFORM JELLY COMPOSITION. THE JELLY COMPOSITION IS USED BY AN ORDINARY USE
METHOD WHERE THE ESSENTIAL OIL IS USED SINGLY, WHEREBY THE DURATION OF AROMA
CAN BE REMARKABLY PROLONGED AS COMPARED WITH THE CASE OF SINGLE USE.
573/1651
116. JP2003210560 - 29.07.2003
AROMATIC ESSENTIAL OIL ODORIZING DEVICE USING DISPOSABLE BODY WARMER AS
THERMAL SOURCE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2003210560
Inventor(s):
WATANABE KAZUHIKO (--)
Applicant(s):
WATANABE KAZUHIKO (--)
IP Class 4 Digits: A61L
IP Class:
A61L9/03
Application Number:
JP20020047163 (20020118)
Family: JP2003210560
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE AN AROMATIC ESSENTIAL OIL ODORIZING DEVICE IN
WHICH A DISPOSABLE BODY WARMER IS USED AS A THERMAL SOURCE FOR VOLATIZING
AROMATIC ESSENTIAL OIL.
SOLUTION: THE MAIN BODY 2 OF THE AROMATIC ESSENTIAL OIL ODORIZING DEVICE IS
PARTITIONED WITH AN ALUMINUM PLATE 3. THE ALUMINUM PLATE 3 IS PROVIDED WITH A
SHEET OF A FILTER PAPER 1 CONTAINING THE AROMATIC ESSENTIAL OIL PLACED ON THE
UPPER PART THEREOF, AND A MIDDLE CONTAINER 8 SEALING THE DISPOSABLE BODY
WARMER 4 ON THE LOWER PART THEREOF. THE ALUMINUM PLATE 3 IS HEATED THROUGH
THE HEAT GENERATION BY THE DISPOSABLE BODY WARMER 4, THUS THE SHEET OF FILTER
PAPER 1 CONTAINING THE AROMATIC ESSENTIAL OIL IS WARMED, SO THAT THE AROMATIC
ESSENTIAL OIL IS EVAPORATED.
574/1651
117. JP2003265152 - 24.09.2003
ANTIBACTERIAL AGENT COMPRISING ESSENTIAL OIL OF ARTEMISIA CAPILLARIS, METHOD OF
PRODUCTION FOR THE SAME AND FOOD PRESERVATIVE
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2003265152
Inventor(s):
TSUDA HIDEYUKI (--); KATABAMI TADASHI (--)
Applicant(s):
DAINIPPON INK and CHEM INC (--)
IP Class 4 Digits: A01N; A23L
IP Class:
A01N65/00; A23L3/3472
Application Number:
JP20020071952 (20020315)
Family: JP2003265152
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE AN ANTIBACTERIAL AGENT COMPRISING AN
ESSENTIAL OIL OF ARTEMISIA CAPILLARIS USED FOR A FOOD PRESERVATIVE BY REDUCING
CONTENT OF AN UNPLEASANT PECULIAR ODOR AND TO PROVIDE A METHOD OF
PRODUCTION FOR THE SAME AND TO PROVIDE THE FOOD PRESERVATIVE CONTAINING THE
ESSENTIAL OIL OF THE ARTEMISIA CAPILLARIS AS THE PRINCIPAL INGREDIENT AND TO
PROVIDE FOODS AND DRINKS CONTAINING THE FOOD PRESERVATIVE COMPRISING THE
ESSENTIAL OIL OF THE ARTEMISIA CAPILLARIES.
SOLUTION: THE ESSENTIAL OIL OF THE ARTEMISIA CAPILLARIS HAS <12% OF PEAK AREAS OF
MORE THAN ONE PEAKS APPEARING IN 0-40 MIN OF RETENTION TIME PER PEAK AREAS OF
MORE THAN ONE PEAKS APPEARING IN 0-85 MIN OF THE RETENTION TIME CHARACTERIZED
BY A CAPILLARY GAS CHROMATOGRAPHY WITH A SPECIFIED ANALYTICAL CONDITION SUCH
AS A COLUMN, FLOW RATE OF CARRIER GAS, ETC., AND HAS >=0.5% OF PEAK AREAS OF THE
PEAK OF CAPILLENE APPEARING CLOSE TO 50 MIN OF RETENTION TIME PER PEAK AREAS OF
MORE THAN ONE PEAKS APPEARING IN 0-85 MIN OF THE RETENTION TIME.
575/1651
118. JP2003327992 - 19.11.2003
ESSENTIAL OIL COMPOSITION AND PATCH
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2003327992
Inventor(s):
YAMAMOTO YOSHIKO (--); SANO HIKOJIRO (--); KAWAHARA KAZUYO (--);
SHIZU KOICHI (--); NODA KUNIMOTO (--); KADOTA HIROAKI (--)
Applicant(s):
YAMAMOTO YOSHIKO (--); SANO INTERNATIONAL:KK (--); EGREDIOR KK (--)
IP Class 4 Digits: A61K; C11B; A61P
IP Class:
A61K35/78; C11B9/00; A61K9/70; A61K31/125; A61K31/343; A61P3/00; A61P43/00
Application Number:
JP20020132827 (20020508)
Family: JP2003327992
Abstract:
PROBLEM TO BE SOLVED: TO OBTAIN AN ESSENTIAL OIL COMPOSITION CAPABLE OF
REDUCING FATIGUE FEELING BY EASILY REDUCING SWELLING WITHOUT CARRYING OUT
MASSAGE.
SOLUTION: THE ESSENTIAL OIL COMPOSITION IS OBTAINED BY ALLOWING A BASE MATERIAL
COMPRISING A HYDROPHILIC POLYMER TO ADSORB AN ESSENTIAL OIL. THE TISSUAL LIQUID
AND LYMPHATIC LIQUID EXCESSIVELY STORED IN A CELL, THE EXTERIOR OF THE CELL, OR
THE LIKE, ARE EXCRETED TO THE EXTERIOR OF HUMAN BODY TO BE ABSORBED BY THE BASE
MATERIAL BY ALLOWING THE ESSENTIAL OIL COMPOSITION TO BE ABSORBED
PERCUTANEOUSLY TO ACT ON THE BODY BY BRINGING THE ESSENTIAL OIL COMPOSITION
NEAR TO OR INTO CONTACT WITH THE BODY. AROMATHERAPEUTIC EFFECTS CAN BE
OBTAINED BY BREATHING AROMA CAUSED BY THE EVAPORATION OF THE ESSENTIAL OIL.
576/1651
119. JP2003339841 - 02.12.2003
HEATING UNIT OF AROMATIC ESSENTIAL OIL AND VOLATILIZING CONTAINER OF ESSENTIAL
OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2003339841
Inventor(s):
HAMAZAKI MASABUMI (--); HAMAZAKI MASANOBU (--)
Applicant(s):
HAMA CORPORATION:KK (--); HAMMERS INC (--)
IP Class 4 Digits: A61L
IP Class:
A61L9/12; A61L9/01
Application Number:
JP20020158580 (20020531)
Family: JP2003339841
Abstract:
PROBLEM TO BE SOLVED: TO REDUCE THE FIRE DANGER.
SOLUTION: THIS HEATING UNIT 10 COMPRISES A MIXTURE 12 AND A BAG BODY 14. THE
MIXTURE 10 IS COMPOSED OF AN EXOTHERMIC AGENT 16 GENERATING HEAT BY HYDRATION
REACTION AND A POROUS AGENT 16 CAPABLE OF HOLDING THE AROMATIC ESSENTIAL OIL
AQUEOUS SOLUTION W. THE BAG BODY 14 IS USED TO ACCOMMODATE THE MIXTURE 12,
AND CONFIGURATED BY A WATER-PERMEABLE BAG BODY 20 AND A NON-WATER PERMEABLE
BAG BODY 22 SURROUNDING AN OUTER PERIPHERY OF THE WATER- PERMEABLE BAG BODY
20. IN ORDER TO GENERATE THE AROMA BY HEATING THE AROMATIC ESSENTIAL OIL BY THE
HEATING UNIT 10, MOISTURE-PROOF FUNCTION OF A MOISTURE-PROOF MEANS OF THE BAG
BODY 14 IS LOST, AND THEN THE AQUEOUS SOLUTION W OF THE AROMATIC ESSENTIAL OIL IS
SUPPLIED TO THE MIXTURE 12. WHEN THE AQUEOUS SOLUTION W OF THE AROMATIC
ESSENTIAL OIL IS SUPPLIED, THE AQUEOUS SOLUTION W IS BROUGHT INTO CONTACT WITH
THE EXOTHERMIC AGENT 12, AND THE HYDRATION REACTION IS GENERATED, WHEREBY THE
EXOTHERMIC AGENT 16 GENERATES THE HEAT, THE AROMATIC ESSENTIAL OIL INCLUDED IN
577/1651
THE AQUEOUS SOLUTION W IS HEATED, AND ITS AROMA IS VOLATILIZED AND DIFFUSED TO
THE OUTSIDE.
578/1651
120. JP2004018737 - 22.01.2004
METHOD FOR EXTRACTING ESSENTIAL OIL FROM FILTRATION RESIDUE OF CITRUS FRUIT
JUICE WITH VIBRATING SCREEN
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2004018737
Inventor(s):
KITAMOTO SHIYUUBIN (--)
Applicant(s):
UMAJIMURA NOGYO KYODO KUMIAI (--)
IP Class 4 Digits: C11B; A23L
IP Class:
C11B9/00; C11B9/02; A23L1/222
Application Number:
JP20020177408 (20020618)
Family: JP2004018737
Abstract:
PROBLEM TO BE SOLVED: TO EFFICIENTLY AND EASILY EXTRACT ESSENTIAL OIL AND FLORAL
WATER FROM SQUEEZED RESIDUE OF CITRUS FRUIT BY TREATING THE RESIDUE WITH A
REDUCED-PRESSURE DISTILLATION APPARATUS.
SOLUTION: WATER IS ADDED TO A SQUEEZED RESIDUE OF CITRUS FRUITS, THE MIXTURE IS
SUBJECTED TO ENZYMATIC TREATMENT WITH CELLULASE OR PECTINASE, ETC., AND THE
TREATED PRODUCT IS DISTILLED BY REDUCED-PRESSURE DISTILLATION TO EFFICIENTLY AND
EASILY EXTRACT THE ESSENTIAL OIL AND FLORAL WATER. FOODS, COSMETICS, QUASIDRUGS AND AROMATHERAPY GOODS UTILIZING EXPENSIVE AND PRECIOUS ESSENTIAL OIL
AND FLORAL WATER OF CITRUS FRUIT CAN BE PRODUCED BY THE METHOD.
579/1651
121. JP2004067523 - 04.03.2004
APOPTOSIS INDUCER AND EXTERNAL PREPARATION FOR SKIN AND METHOD FOR USING
CITRUS ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2004067523
Inventor(s):
HATA CHINA (--); SAKAGUCHI IKUYO (--); IKEDA NORIKAZU (--); KATO
TAKAYOSHI (--); MINAMINO YOSHINORI (--)
Applicant(s):
CLUB COSMETICS CO LTD (--)
IP Class 4 Digits: A61K; A61P
IP Class:
A61K35/78; A61P43/00; A61P17/00
Application Number:
JP20020225081 (20020801)
Family: JP2004067523
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE A NEW AND USEFUL APOPTOSIS INDUCER.
SOLUTION: THE APOPTOSIS INDUCER COMPRISES A CITRUS ESSENTIAL OIL EXTRACTED FROM
A RUTACEOUS PLANT SUCH AS AN ORANGE ESSENTIAL OIL, A GRAPEFRUIT ESSENTIAL OIL
OR A LEMON ESSENTIAL OIL AS AN ACTIVE INGREDIENT. A FRACTION OBTAINED BY
ADSORBING THE CITRUS ESSENTIAL OIL ON A NEUTRAL ALUMINA, THEN DISTILLING OFF AN
ELUTION SOLVENT FROM A FRACTION ELUTED WITH N-HEXANE OR ETHER MAY BE USED AS
THE ACTIVE INGREDIENT. THE RESULTANT APOPTOSIS INDUCER PROMOTES METABOLISM OF
SKIN, PROMOTES TREATMENT OF BACTERIAL INFECTION AND CAN BE UTILIZED AS THE
EXTERNAL PREPARATION FOR THE SKIN.
580/1651
122. JP2004099535 - 02.04.2004
SANITARY INSECT PEST REPELLENT OF NATURAL ESSENTIAL OIL AND APPLICATION THEREOF
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2004099535
Inventor(s):
KOMAI KOICHIRO (--); HAYASE TOMOKO (--); HAYASE MANABU (--); MIWATA
MASAYASU (--); SAKURAI OSAMU (--); KUROKI OSAMU (--); MIZUGUCHI MASAAKI (--)
Applicant(s): HAYASE TOMOKO (--); RIFURE:KK (--); DAIHO KORYO KK (--); SUZUKI YUSHI
KOGYO KK (--)
IP Class 4 Digits: C11B; A01N; A01M; C09D; C09J
IP Class:
C09J11/06
C11B9/00; A01N65/00; A01M29/00; C09J201/00; C09D11/00; C09J7/00;
Application Number:
JP20020264399 (20020910)
Family: JP2004099535
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE AN ADHESIVE AND STICKING AGENT, AN INK, A RESIN
PELLET, A RESIN PRODUCT, A SHEET AND A FILM, HAVING EFFECTS OF REPELLENT ACTIVITIES
CAUSED BY ORGANIC MACROMOLECULAR FINE PARTICLES CARRYING A REPELLENT ACTIVE
MATERIAL OVER A LONG PERIOD.
SOLUTION: THE DISPERSION CONTAINS THE NATURAL ESSENTIAL OIL HAVING SANITARY
INSECT PEST-REPELLENT ACTIVITIES, CONSISTING OF COPAIBA OIL AND/OR ONE OR MORE
KINDS OF CARYOPHYLLENE, VETIVER OIL, ELEMI OIL AND "ELEMIRIDINOID", ORANGE FLOWER
OIL, GERANIUM OIL, PEIGNEE ROYAL OIL, NEEM OIL AND THE LIKE AS AN ACTIVE INGREDIENT.
THE DISPERSION CAN CONTAIN A PRECIPITATION-PREVENTING AGENT BESIDES THEM. THE
ADHESIVE AND STICKING AGENT, THE INK, THE RESIN PELLET, THE RESIN PRODUCT, THE
SHEET, THE FILM AND THE APPARATUS HAVING THE SANITARY INSECT PEST-REPELLENT
ACTIVITIES CONTAIN THE FINE PARTICLES.
581/1651
123. JP2004099536 - 02.04.2004
SANITARY INSECT PEST REPELLENT OF NATURAL ESSENTIAL OIL AND APPLICATION THEREOF
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2004099536
Inventor(s):
KOMAI KOICHIRO (--); HAYASE TOMOKO (--); HAYASE MANABU (--); MIWATA
MASAYASU (--); SAKURAI OSAMU (--); KUROKI OSAMU (--); MIZUGUCHI MASAAKI (--)
Applicant(s): HAYASE TOMOKO (--); RIFURE:KK (--); DAIHO KORYO KK (--); SUZUKI YUSHI
KOGYO KK (--)
IP Class 4 Digits: C11B; A01N; A01M; C09D; C09J
IP Class:
C09J201/00
C11B9/00; A01N65/00; A01N25/10; A01M29/00; C09D11/02; C09J9/00;
Application Number:
JP20020264404 (20020910)
Family: JP2004099536
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE AN ADHESIVE AND STICKING AGENT, AN INK, A RESIN
PELLET, A RESIN PRODUCT, A SHEET, A FILM AND A DEVICE, HAVING EFFECTS OF REPELLENT
ACTIVITIES CAUSED BY ORGANIC MACROMOLECULAR FINE PARTICLES CARRYING A
REPELLENT ACTIVE MATERIAL OVER A LONG PERIOD.
SOLUTION: THE ORGANIC MACROMOLECULAR FINE PARTICLE CONTAINS THE NATURAL
ESSENTIAL OIL HAVING SANITARY INSECT PEST-REPELLENT ACTIVITIES, CONSISTING OF
COPAIBA OIL AND/OR ONE OR MORE KINDS OF CARYOPHYLLENE, VETIVER OIL, ELEMI OIL
AND "ELEMIRIDINOID", ORANGE FLOWER OIL, GERANIUM OIL, PEIGNEE ROYAL OIL, NEEM OIL
AND THE LIKE AS AN ACTIVE INGREDIENT. THE DISPERSION OF THE FINE PARTICLES
CONTAINS ONLY THE FINE PARTICLES, OR THE FINE PARTICLES AND A PRECIPITATIONPREVENTING AGENT. THE ADHESIVE AND STICKING AGENT, THE INK, THE RESIN PELLET, THE
RESIN PRODUCT, THE SHEET, THE FILM AND THE DEVICE, HAVING SANITARY INSECT PESTREPELLENT ACTIVITIES CONTAIN THE FINE PARTICLES.
582/1651
124. JP2004099594 - 02.04.2004
NEW USE OF TEA TREE ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2004099594
Inventor(s):
KAWAGUCHI TOMIHISA (--); ISHIDAKA KOJI (--); KOBAYASHI TATSUYA (--);
YAMAMOTO SHOKO (--); IMAI SHIN (--); KIDA NORIHIRO (--)
Applicant(s):
KYOUWA YAKUHIN KK (--)
IP Class 4 Digits: A61K; A61P; A23K
IP Class:
A61P37/04
A61K35/78; A61P3/00; A61P31/04; A23K1/16; A23K1/18; A61P7/00; A61P35/02;
Application Number:
JP20030195751 (20030711)
Family: JP2004099594
Abstract:
PROBLEM TO BE SOLVED: TO PROVIDE VARIOUS COMPOSITIONS FOR SOLVING PROBLEMS
SUCH THAT CONVENTIONALLY, VARIOUS DISEASES OF FISHES ARE TREATED WITH
ANTIBIOTICS, VACCINES AND VARIOUS IMMUNO-AUGMENTING AGENT, ETC., BUT FOR THE
ANTIBIOTICS, THERE ARE MANY PROBLEMS IN FOOD HYGIENE SUCH AS THE APPEARANCE OF
DRUG RESISTANT BACTERIA, ETC., ON THE OTHER HAND, FOR THE VACCINE AND VARIOUS
IMMUNO AUGMENTING AGENT, MANY OF THEM LACK PRACTICALITY IN POINTS OF ECONOMIC
PROPERTY, EFFECTIVENESS, SAFETY, LABOR OR AVAILABILITY, ETC., AND ALSO IN THE
PRESENT FISHERY BREEDING, IT IS DIFFICULT TO GROW CULTURED FISHES IN A GOOD
EFFICIENCY CAUSED BY A HYPER OVER-CONGESTED BREEDING.
SOLUTION: THIS IMMUNO-ACTIVATING COMPOSITION CONTAINS A TEA TREE ESSENTIAL OIL.
BY FEEDING IT TO FISHES, THE IMMUNO-ACTIVATING EFFECT, ANTIBACTERIAL EFFECT,
VACCINE EFFECT-AUGMENTING EFFECT AND/OR BODY-INCREASING EFFECT OF THE
COMPOSITION ARE CUMULATIVELY OR SINERGISTICALLY EXHIBITED, AND IT IS POSSIBLE TO
583/1651
CONTROL VARIOUS DISEASES OF FISHES AND/OR IMPROVE THE BREEDING RESULTS OF THE
FISHES.
584/1651
125. JP2078613 - 19.03.1990
SOFT CAPSULE CONTAINING ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2078613
Inventor(s):
others: 04 (--); KOMATA KAZUOKI (--)
Applicant(s):
others: 01 (--); TAISHO PHARMACEUT CO LTD (--)
IP Class 4 Digits: A61K
IP Class:
A61K9/48
Application Number:
JP19880229538 (19880913)
Family: JP2078613
Equivalent:
JP1970915; JP7000550
Abstract:
PURPOSE:TO OBTAIN A CAPSULE RESISTANT TO THE LOWERING OF SOLUBILITY AND
DISCOLORATION WITH TIME, COMPOSED OF GELATIN AND A POLYPEPTIDE AND CONTAINING
AN ALDEHYDE-CONTAINING NATURAL VEGETABLE OIL SUCH AS CINNAMON OIL OR ANISE OIL
AND AN ESSENTIAL OIL EXTRACT REACTIVE TO THE AMINO GROUP OF GELATIN.
CONSTITUTION:THE SOFT GELATIN CAPSULE IS COMPOSED OF A CAPSULE WALL MADE OF
GELATIN COMPOUNDED WITH 15-70WT.% (PREFERABLY 20-50WT.%) OF A POLYPEPTIDE AND
IS FILLED WITH AN OIL SUCH AS CINNAMON OIL, ANISE OIL, CLOVE OIL, PEPPERMINT OIL,
GINGER OIL, CARDAMOM OIL, LEMON OIL, CITRUS OIL OR L-MENTHOL. PREFERABLY, THE
POLYPEPTIDE HAS A MOLECULAR WEIGHT OF 5,000-10,000 AND IS USED IN THE FORM OF
POWDER. THE GELATIN WALL OF THE CAPSULE PRODUCED BY THE ABOVE PROCESS IS
RESISTANT TO THE LOWERING OF SOLUBILITY AND THE DISCOLORATION WITH TIME. THE
CAPSULE IS PRODUCED BY MIXING GELATIN WITH A POLYPEPTIDE, SWELLING THE MIXTURE
WITH PURIFIED WATER AND FORMING A CAPSULE BY A CAPSULE-FORMING MACHINE USING
CINNAMON OIL, ETC., AS A CONTACT.
585/1651
126. JP2180997 - 29.10.1991
PROCESS FOR THE REMOVAL OF TERPENES FROM ESSENTIAL OILS
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP2180997
Inventor(s):
VOLLBRECHT HEINZ-RUEDIGER (DE); CULLY JAN (DE); SCHUETZ ERWIN (DE)
Applicant(s):
SUEDDEUTSCHE KALKSTICKSTOFF (DE)
IP Class 4 Digits: B01D
IP Class:
B01D15/00
E Class: C11B9/02B
Application Number:
US19890419643 (19891011)
Priority Number: DE19883834988 (19881014)
Family: JP2180997
Equivalent:
DE3834988; EP0363971; ES2070877; GR3015902; JP2541670; MX171557;
SU1769761; ZA8907691
Abstract:
TERPENES ARE REMOVED FROM ESSENTIAL OILS BY (A) CONTACTING TERPENE-CONTAINING
ESSENTIAL OILS WITH A POLAR SOLID (ADSORBENT); (B) SEPARATING THE LOADED
ADSORBENT FROM THE LIQUID PHASE ENRICHED WITH TERPENES; AND (C) SUBJECTING THE
ADSORBENT LOADED WITH ESSENTIAL OILS TO AN EXTRACTION WITH COMPRESSED CARBON
DIOXIDE.Description:
FIELD OF THE INVENTION
The present invention is concerned with a process for the removal of terpenes from essential oils in a
three-step process.
586/1651
BACKGROUND OF THE INVENTION
Essential oils are important aroma substances in the foodstuff industry. Thus, for example, coldpressed oils from citrus fruits are used to a large extent for the production of essences for the
beverage industry, as well as for the aromatization of bakery products. These essential oils frequently
contain terpene hydrocarbons of the mono- and sesquiterpene series which have only a limited
storage stability and are thermolabile and, in addition, display a smaller aroma intensity than the
actual aroma material which is preponderantly composed of volatile oxygen-containing compounds,
such as aldehydes, ketones, esters, acids, phenols, alcohols and lactones. For these reasons, the
removal of the terpenes is an important step for the improvement of the storage stability and for
intensifying the aroma intensity of essential oils.
Furthermore, by the removal of the non-polar terpene hydrocarbons, the water-solubility of the
essential oils is improved, which is of particular importance for the beverage industry.
A number of processes are known for the removal of terpenes from of essential oils which, for the
separation of the terpenes, utilize differences in the vapor pressure, in the polarity or in the solubility
of the terpene components in comparison with the oxygen-containing compounds. All these
processes possess certain disadvantages which manifest themselves either in the quality of the
product, in the process costs or in the yields. Thus, for example, there has been described the
dissolving of essential oils in aqueous alcohols, the terpenes thereby separating out, followed by the
recovery of the desired aroma fractions by salting out or by liquid-liquid extraction. In the case of this
process, the separation action and the yields are not satisfactory. Furthermore, depending upon the
nature of the extraction agent used, technical or environmental problems can arise.
Chromatography is a further known method, for example for the enrichment of citrus oils. These
processes are very laborious and expensive since it is necessary to work with very dilute solutions.
Furthermore, in the case of the subsequent evaporation of the solutions, there is a danger of the
thermal decomposition of the sensitive component materials or of the loss of the low boiling aroma
materials.
The removal of terpenes by means of rectification or distillation in a vacuum, as well as steam
distillation, are also widely used methods. These processes do not provide high quality products
since the aroma components are considerably damaged by the thermal stressing.
587/1651
In contradistinction thereto, processes of high pressure extraction for the enrichment of essential oils,
which recently became known, are substantially more gentle. Thus, for example, in Chem. Ing. Tech.,
56, 794/1984, there is described a process for the removal of terpenes from citrus oils in which the
citrus oils are subjected to a countercurrent extraction with carbon dioxide at 70 to 90 bar and at
about 55 DEG to 85 DEG C. in a counterflow column to which is applied a temperature gradient. With
the help of countercurrent extraction there can be achieved either high rates of enrichment or high
yields but not both together (cf. Food Technology, 6, 145/1988) since either the selectivity of the
process is small or the loading of the carbon dioxide with terpenes is low.
Finally, in U.S. Pat. No. 4,647,466, there is described a process for the extraction of readily volatile
oxygen-containing materials, such as ethyl butyrate or hexanal, from citrus oils with the help of
compressed gases, limonene thereby being enriched. However, since citrus oils, for example orange
oils, consist of up to 95% limonene, very large amounts of carbon dioxide or long extraction times are
necessary for carrying out the process in order to remove from the aroma oil a high proportion of
limonene with the necessary selectivity.
OBJECTS OF THE INVENTION
Therefore, it is an object of the present invention to provide a process for the removal of terpenes
from essential oils which does not display the disadvantages of the prior art but rather, with low
technical expense and under mild conditions, makes possible a selective enrichment of the essential
oils with good yields.
DESCRIPTION OF THE INVENTION
Thus, according to the present invention, there is provided a process for the removal of terpenes
from essential oils, wherein
a) the terpene-containing essential oils are contacted with a polar solid (adsorbent),
b) the loaded adsorbent is separated from the liquid phase enriched with terpenes and
c) the adsorbent loaded with essential oils is subjected to an extraction with compressed carbon
dioxide.
Surprisingly, we have found that in this way a substantial removal of the terpenes is achieved and, at
the same time, the essential oils can be obtained in high yield and with good quality.
588/1651
The process according to the present invention comprises at least three steps. In the first step a), the
terpene-containing essential oils are contacted with a polar solid (adsorbent). In the scope of the
present invention, in principle there can be used all terpene-containing essential oils. In particular,
citrus oils can be used which have been obtained from citrus fruits, for example, oranges, lemons,
tangerines, citrons, limes, grapefruit and cravos. However, other aromatic oils, such as hop,
carnation, laurel, ginger, peppermint and cedar wood oils can also be used. Instead of the pure
essential oils, there can also be used carbon dioxide extracts or oleoresins. Depending upon their
nature and origin, the essential oils have terpene contents of up to 95%.
The loading of the adsorbent with the essential oils can take place according to known methods, for
example by simple mixing. As polar adsorbents, there can be used the solid materials conventional
for this purpose, for example silica gel, aluminum oxide, kieselguhr, cellulose, bentonite, magnesium
silicates and the like. Silica gel and aluminum oxide have thereby proved to be especially
advantageous.
The amount of the polar adsorption agent can be varied within wide limits but it is preferred to use 10
to 60% by weight of polar adsorbent, referred to the initial amount of essential oils. In the case of this
loading of the adsorbent according to step a), the greater part of the oxygen-containing aroma
materials are adsorbed on the solid material, whereas the terpenes remain substantially in the liquid
phase. Depending upon the nature of the aroma oil used and the amount of adsorbent employed,
about 60 to 95% of the aroma materials are adsorbed.
In the second step b) of the process according to the present invention, there then takes place the
separation of the adsorbent loaded with the aroma materials from the terpenes remaining in the liquid
phase. The methods which are usual for the separation of solid materials from liquids can thereby be
used. Because of the rapid and complete separation, there is hereby preferably used centrifuging.
However, in the case of this step, other separation processes, for example filtration, can readily be
employed. In this way, as a rule the main amount of the terpenes contained in the essential oils can
already be removed without it resulting in noticeable losses of the valuable aroma materials.
In general, the adsorbent can be used several times for the adsorption. In the case of the adsorption,
it is possible to increase the yield of aroma materials by first mixing the adsorbent with the terpene
fraction of a previous batch and then separating off as described above. In this case, the mixture of
589/1651
terpene fraction and adsorbent can be filled into a column and the essential oils to be enriched
passed therethrough in the manner of column chromatography.
In the following step c), the adsorbent loaded with aroma components is subjected to a high
pressure extraction with compressed carbon dioxide, the aroma materials thereby being desorbed or
extracted. The high pressure extraction should take place at pressures above 70 bar and at a
temperature of from 10 DEG to 80 DEG C. in order to achieve a complete extraction of the aroma
materials. Preferred extraction conditions are to be regarded as being pressures of >100 bar and
especially of 200 to 300 bar and temperatures of from 30 DEG to 70 DEG C. because, under these
conditions, the aroma materials can be obtained especially quickly and gently. It is clear that, in the
case of this high pressure extraction, apart from the desired aroma materials, the residue of terpenes
is also co-extracted which was co-adsorbed on the polar adsorbent in the first step.
Therefore, if it is desired to achieve a practically complete removal of the terpenes from the essential
oils, in a preferred embodiment of the process according to the present invention, before the high
pressure extraction (step c)) for obtaining the aroma materials, there is carried out a pre-extraction in
which the residual terpenes are first removed from the adsorption agent. This pre-extraction is also
carried out with compressed carbon dioxide but, in contradistinction to the process conditions of
step c) (main extraction), at pressures below 100 bar and preferably at 70 to 90 bar.
The temperature range for the pre-extraction is from 30 DEG to 80 DEG C. and preferably 50 DEG to
70 DEG C. Under these process conditions, a substantially selective extraction of the terpenes takes
place, whereas the aroma materials remain behind on the adsorbent. The terpene hydrocarbon
content of these pre-extracts generally lies above the terpene content of the starting oil. Then, as
already described, this pre-extraction is followed by the main extraction (step c)) in which the
oxygen-containing aroma materials can then be obtained under gentle conditions. The carbon
dioxide aroma extracts obtained in this way can then be completely separated from the carbon
dioxide in the usual manner by lowering the density of the carbon dioxide. In this way, it is possible to
obtain highly concentrated extracts of essential oils with low terpene contents (reduction of the
terpenes by 95%) in high yields, which display a very good quality because of the gentle treatment.
Since the main amount of the terpenes has already been removed before the carbon dioxide
extraction, only comparatively small amounts of carbon dioxide are necessary for the extraction of
the important aroma materials.
The following Examples are given for the purpose of illustrating the present invention:
590/1651
EXAMPLE 1
Obtaining of lemon peel oil concentrate with a low terpene content.
3 kg. of lemon oil with a limonene content of 64.1% was intimately mixed with 1 kg. silica gel at
ambient temperature for 90 minutes by stirring. Thereafter, the loaded silica gel was separated from
the liquid phase by centrifuging and, in a high pressure extraction plant, subjected to a preextraction at 70 bar and 50 DEG C. with 80 kg. carbon dioxide. After removal of the terpene-rich
fraction from the separator, the main extraction was carried out at 280 bar and 50 DEG C., the
adsorbed aroma materials thereby being extracted from the silica gel with 40 kg. carbon dioxide.
As extract, there were obtained 30 g. of concentrate with a limonene content of 6.7%. The specific
carbon dioxide requirement amounted in all to 40 kg. carbon dioxide per kg. of starting oil.
EXAMPLE 2
Obtaining of orange peel oil concentrate with a reduced terpene content.
5 kg. of orange oil with a limonene content of 95.7% were, corresponding to Example 1, stirred with 1
kg. silica gel at ambient temperature for 120 minutes.
Thereafter, the loaded silica gel was separated from the liquid phase by centrifuging and extracted
in a high pressure extraction plant with 40 kg. carbon dioxide at 280 bar and 35 DEG C.
As extract there were obtained 625 g. of concentrate with a limonene content of 89.6%. The specific
carbon dioxide consumption was 8 kg. carbon dioxide per kg. of starting oil.
EXAMPLE 3
Obtaining of lemon peel oil concentrate with a reduced terpene content.
3 kg. of lemon oil with a limonene content of 64.1% were stirred with 1 kg. active aluminum oxide at
ambient temperature for 90 minutes. Subsequently, the loaded aluminum oxide was separated from
591/1651
the liquid phase by centrifuging and subjected to a pre-extraction in a high pressure extraction plant
with 30 kg. carbon dioxide at 90 bar and 70 DEG C. After removal of the separated terpene-rich
fraction from the separator, the main extraction was carried out at 280 bar and 70 DEG C. and the
adsorbed aroma materials extracted from the aluminum oxide with 40 kg. carbon dioxide.
As extract, there were obtained 230 g. of concentrate with a limonene content of 41.9%. The specific
carbon dioxide consumption was, in all, 23 kg. of carbon dioxide per kg. of starting oil.
Claims:
We claim:
1. The method of removing terpenes from a terpene-containing essential oil, which comprises (a)
contacting the terpene-containing essential oil with a polar adsorbent such that the adsorbent
becomes loaded with essential oil and a liquid phase enriched with terpene is produced, (b)
separating the loaded adsorbent from the liquid phase enriched with terpenes, and (c) subjecting
the adsorbent loaded with essential oil to an extraction with compressed carbon dioxide.
2. The method of claim 1, wherein the adsorbent is silica gel.
3. The method of claim 1, wherein the adsorbent is aluminum oxide.
4. The method of claim 1, wherein the amount of adsorbent used is 10 to 60% by weight, based on
the amount of terpene-containing essential oil contacted in step (a).
5. The method of claim 1, wherein the separation of the loaded adsorbent from the liquid phase is
carried out by centrifuging.
6. The method of claim 1, wherein the extracted adsorbent is recycled to step (a).
7. The method of claim 1, wherein the adsorbent is contacted with a terpene fraction from a previous
process batch, the mixture of the loaded adsorbent and terpene enriched liquid phase is introduced
into a column and, after draining off the liquid phase, passing the essential oil through the column.
8. The method of claim 1, wherein the carbon dioxide extraction is carried out at a pressure of >70
bar and at a temperature of 10 DEG to 80 DEG C.
592/1651
9. The method of claim 8, wherein the carbon dioxide extraction is carried out at a pressure of 200 to
300 bar and at a temperature of 30 DEG to 70 DEG C.
10. The method of claim 1, wherein, before step (c), the loaded adsorbent is subjected to a preextraction with compressed carbon dioxide at a pressure of <100 bar.
11. The method of claim 10, wherein the pre-extraction takes place at a pressure of 70 to 90 bar and
at a temperature of 30 DEG to 80 DEG C.
12. The method of claim 11, wherein the pre-extraction takes place at a temperature of 50 DEG to 70
DEG C.
593/1651
127. JP3028300 - 06.02.1991
ESSENTIAL OIL AND PERFUME CONTAINING SAME ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP3028300
Inventor(s):
others: 02 (--); KUBOTA MASAO (--)
Applicant(s):
KANEBO LTD (--)
IP Class 4 Digits: A61K; C11B
IP Class:
A61K35/78; A61K7/46; C11B9/02
Application Number:
JP19890163231 (19890626)
Family: JP3028300
Abstract:
PURPOSE:TO PROVIDE AN ESSENTIAL OIL HAVING AN EXCELLENT STRESS RELIEVING EFFECT,
EMITTING STRONG FRAGRANCE AND BEING SUITABLE FOR MANUFACTURING PERFUMES BY
USING A LOW B.P. COMPONENT FRACTIONATED FROM A SANDALWOOD OIL AND HAVING A
SPECIFIED PROPERTY AS AN ACTIVE INGREDIENT.
CONSTITUTION:A SANDALWOOD OIL IS FRACTIONATED BY GAS CHROMATOGRAPHY UNDER
SUCH CONDITIONS THAT A GAS CHROMATOGRAPH GC-6AM MANUFACTURED BY SHIMADZU
CORPORATION AND A COLUMN PEG20M (WITH THE INNER DIAMETER OF 0.25MM AND THE
LENGTH OF 50CM) MANUFACTURED BY GASCHRO INDUSTRIES CO., LTD. ARE USED AND
NITROGEN GAS IS USED AS A CARRIER GAS UNDER THE OPERATING CONDITIONS OF A
CARRIER GAS FLOW RATE OF 1ML/MIN, A COLUMN TEMP. OF 80-200 DEG.C AND A COLUMN
TEMP. RISE RATE OF 2 DEG.C/MIN USING F.I.D AS A DETECTOR. A LOW B.P. COMPONENT OF
THE SANDALWOOD OIL WITH A RETENTION TIME OF 5-55MIN IS FRACTIONATED. THEN AN
ESSENTIAL OIL IS PREPD. BY USING THIS LOW B.P. COMPONENT AS AN ACTIVE INGREDIENT
AND, IF NECESSARY, INCORPORATING A FIXER AGENT (E.G. TRIMETHYL CITRATE), ETC. THE
SANDALWOOD OIL IS OBTD. BY PERFORMING STEAM DISTILLATION OF ROOTS, HEARTWOOD,
ETC., OF AN INDIAN SANDALWOOD.
594/1651
128. JP3061001 - 15.03.1991
MANUFACTURE OF PLYWOOD CONTAINING NATURAL ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP3061001
Inventor(s):
others: 02 (--); ANDO SHIGERU (--)
Applicant(s):
SANYO KOKUSAKU PULP CO LTD (--)
IP Class 4 Digits: C09J; B27D
IP Class:
B27D5/00; C09J11/08
Application Number:
JP19890197703 (19890728)
Family: JP3061001
Equivalent:
JP2874768
Abstract:
PURPOSE:TO CONTRIVE IMPROVEMENTS IN EXCELLENT BREEDING CONTROL AND EVASION
EFFECT OF COCKROACH, BY A METHOD WHEREIN A MULTI-LAYER-CONSTRUCITON EMULSION
IS MIXED INTO A FORMALDEHYDES ADHESIVE FOR ADHESION OF VENEERS IN A SPECIFIC
QUANTITY WITHOUT SPOILING THE ADHESION THEREBETWEEN.
CONSTITUTION:INFILTRATION AND RATION OF AN EFFECTIVE INGREDIENT OF A MEDICIENE
INTO POLYMER PARTICLES OBTAINED BY AN EMULSION POLYMERIZATION OF A MONOMER
HAVING UNSATURATED DOUBLE CONSTRUCTION ARE PERFORMED AS THE MULTI-LAYERCONSTRUCTION EMULSION. THEN THE MONOMER HAVING UNSATURATED DOUBLE BOND
CONTAINING AN OIL-SOLUBLE POLYMERIZATION INHIBITOR IS POLYMERIZED ON THE
SURFACE OF A POLYMER RETAINING THE EFFECTIVE INGREDIENT OF THE MEDICINE. ACRYLIC
ACID OR VINYL ACETATE AND BENZOYL PEROXIDE ARE USED RESPECTIVELY AS AN
UNSATURATED MONOMER AND THE OIL-SOLUBLE POLYMERIZATION INHIBITOR. A NATURAL
VOLATILE OIL INGREDIENT SUCH AS A TERPENE GROUP IS USED AS THE NATURAL LESENTIAL
OIL INGREDIENT. A FORMALDEHYDE ADHESIVE SUCH AS UREA MELAMINE RESIN CAN BE
595/1651
USED AS ADHESIVE AND MULTI-LAYER-CONSTRUCTION EMULSION IS ADDED TO AND MIXED
WITH THE ADHESIVE AS LOADINGE OF THE SAME TO THE ADHESIVE SO THAT THE LOADINGS
BECOME 100G/M<2>-300G/M<2> TO PLYWOOD.
596/1651
129. JP3111493 - 13.05.1991
TRANQUILIZING ESSENTIAL OIL AND PERFUMES CONTAINING IT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP3111493
Inventor(s):
KUBOTA MASAO (--); others: 03 (--)
Applicant(s):
KANEBO LTD (--)
IP Class 4 Digits: A61K; C11B
IP Class:
A61K35/78; A61K7/46; C11B9/02
Application Number:
JP19890248464 (19890925)
Family: JP3111493
Abstract:
PURPOSE:TO ENHANCE (AND PROLONG THE DURATION OF) THE TRANQUILIZING EFFECT AND
THE FRAGRANCE DIFFUSIBILITY OF A LAVENDER OIL BY REMOVING A HIGH BOILING
COMPONENT THEREFROM.
CONSTITUTION:A LAVENDER OIL (E.G. A LAVENDER ESSENTIAL OIL) IS HEATED SLOWLY TO 25
TO 70 DEG.C UNDER A REDUCED PRESSURE OF 0.1 TO 0.3MMHG TO REMOVE A HIGH BOILING
COMPONENT THEREFROM. AS A RESULT, THERE IS OBTAINED AN ESSENTIAL OIL FOR
TRANQUILIZATION CONTAINING AS MAIN COMPONENTS MYRCENE, 1,8-CINEOLE, OCIMENE,
CAMPHOR, LINALOOL AND LINALYL ACETATE AS CONFIRMED BY A GAS-CHROMATOGRAPHIC
CHROMATOGRAM [APPARATUS: 5980A PRODUCED BY HEWLETT PACKARD; COLUMN: DBWAX PRODUCED BY JW (INNER DIAMETER: 0.25MM, HEIGHT: 60M); CARRIER GAS: NITROGEN;
CARRIER GAS FLOW RATE: 1ML/MIN; COLUMN TEMPERATURE; 70-200 DEG.C; COLUMN
TEMPERATURE ELEVATING RATE: 2 DEG.C/MIN; DETECTOR: F.I.D.] PERFORMED WITH A
RETENTION TIME OF 0 TO 30 MINUTES, AND AT A SPECIFIC GRAVITY D<20> OF 0.860 TO 0.900
AND A REFRACTIVE INDEX OF 1.4063 TO 1.4073.
597/1651
130. JP4091768 - 25.03.1992
PRODUCTION OF HEALTHY BEVERAGE OF CRUDE MEDICINAL ACTIVE HERBAL ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP4091768
Inventor(s):
YAMADA TOSHIO (--)
Applicant(s):
others: 01 (--); MASAHARU SAITO (--)
IP Class 4 Digits: C11B; A23L
IP Class:
C11B9/02; A23L2/38; A23L1/30; A23L2/00
Application Number:
JP19900207380 (19900803)
Family: JP4091768
Abstract:
PURPOSE:TO PRODUCE A HEALTHY BEVERAGE OF A CLEAR LIQUID.CRUDE MEDICINAL
HERBAL ESSENTIAL OIL INTACTLY CONTAINING ACTIVE INGREDIENTS OF THE CRUDE DRUGS
WITHOUT ANY CLOUDING AND PRECIPITATES BY EXTRACTING PARTS READILY AFFECTED BY
HEAT IN THE CRUDE DRUGS AT AMBIENT TEMPERATURE, THEN DECOCTING PARTS OF MARCS
AND EXTRACTING THE DECOCTED MARCS.
CONSTITUTION:INGREDIENTS OF CRUDE DRUGS SUCH AS GINSENG, CORK TREE BARK OR
LICORICE ARE LEACHED WITH A SUITABLE LEACHING AGENT SUCH AS METHANOL OR
PETROLEUM ETHER AND THE SOLVENT IS THEN DISTILLED AWAY TO CONCENTRATE THE
LEACHATE. THEREBY, AN EXTRACT AGENT IS PREPARED. THE REMAINING MARCS OF THE
CRUDE DRUGS ARE THEN DECOCTED AT A PRESCRIBED TEMPERATURE FOR A PRESCRIBED
TIME, E.G. 70-95 DEG.C FOR 30-90MIN AND THE RESULTANT FILTRATE IS ADDED TO THE
AFOREMENTIONED EXTRACT AGENT. THE PREPARED MIXTURE IS SUBSEQUENTLY FREEZEDRIED OR DRY SPRAYED TO PROVIDE A DRY EXTRACT, WHICH IS THEN ADDED TO A
BEVERAGE BASE.
598/1651
131. JP4108707 - 09.04.1992
VERMIN-REPELLENT CONTAINING ESSENTIAL OIL OF JAPANESE CYPRESS AS ACTIVE
COMPONENT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP4108707
Inventor(s):
WATANABE KEISUKE (--); others: 04 (--)
Applicant(s):
SUMITOMO CHEM CO LTD (--)
IP Class 4 Digits: A01N
IP Class:
A01N65/00
Application Number:
JP19900226223 (19900827)
Family: JP4108707
Abstract:
PURPOSE:TO OBTAIN A VERMIN-REPELLENT HAVING HIGH SAFETY AND LOW RESIDUAL
TOXICITY AND EFFECTIVE FOR MOSQUITO, GNAT, STOMOXYS CALCITRANS, SANDFLY,
CERATOPOGONID, COCKROACH, ETC., BY EXTRACTING ESSENTIAL OIL FROM JAPANESE
CYPRESS E.G. BY THE STEAM-DISTILLATION OF THE WOOD AND LEAF OF THE TREE AND
USING THE ESSENTIAL OIL AS AN ACTIVE COMPONENT.
CONSTITUTION:THE OBJECTIVE VERMIN-REPELLENT HAVING THE FORM OF LOTION, AEROSOL,
CREAM, ETC., CAN BE PRODUCED BY USING 1-20WT.% OF ESSENTIAL OIL OF JAPANESE
CYPRESS, ADDING AN ADDITIVE SUCH AS EMULSIFIER, HUMECTANT, PRESERVATIVE AND
PROPELLANT TO THE OIL AS NECESSARY AND COMPOUNDING THE MIXTURE TO A CARRIER
SUCH AS WATER, ALCOHOL AND ALIPHATIC HYDROCARBON. IT CAN BE MICROENCAPSULATED AND USED IN THE FORM OF LOTION, AEROSOL, ETC. THE AMOUNT OF THE
VERMIN-REPELLENT IS 0.05-0.5MG OF THE ESSENTIAL OIL OF JAPANESE CYPRESS PER
1CM<2> OF THE SKIN TO BE TREATED.
599/1651
132. JP4132797 - 07.05.1992
ESSENTIAL OIL OF JAPANESE CEDAR AND JAPANESE CYPRESS AND PRODUCTION THEREOF
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP4132797
Inventor(s):
others: 01 (--); CHIKA TAKUMI (--)
Applicant(s):
BII ANDO AI SHINKOU KIYOUDOUKUMIAI (--)
IP Class 4 Digits: C11B; B27L
IP Class:
C11B9/02; B27L11/08
Application Number:
JP19900253660 (19900921)
Family: JP4132797
Abstract:
PURPOSE:TO CARRY OUT DETOXIFYING TREATMENT AND SIMULTANEOUSLY OBTAIN AN
ANTIMICROBIAL ESSENTIAL OIL BY SUBJECTING CHOPPED SUBSTANCES OF JAPANESE
CEDAR AND JAPANESE CYPRESS TO BLASTING TREATMENT UNDER SPECIFIC CONDITIONS
AND SEPARATING THE ESSENTIAL OIL FROM THE GENERATED GASES AND PRODUCED OILS.
CONSTITUTION:TREE BARK, WOODY PARTS, LEAF PARTS, ETC., OF JAPANESE CEDAR AND
JAPANESE CYPRESS ALONE OR MIXTURES THEREOF ARE CHOPPED TO A PRESCRIBED SIZE,
PLACED IN A HERMETICALLY SEALED CONTAINER AND SUBJECTED TO BLASTING TREATMENT
AT A HIGH TEMPERATURE UNDER A HIGH PRESSURE OF SATURATED STEAM. GENERATED
GASES IN THE BLASTING ARE COOLED WITH A CONDENSER TO RECOVER A LIQUID, WHICH IS
THEN SUBJECTED TO STEAM DISTILLATION TO SEPARATE AN ESSENTIAL OIL COMPONENT.
LIQUIDS PRODUCED IN THE BLASTING ARE SUBJECTED TO THE STEAM DISTILLATION TO
SEPARATE THE OBJECTIVE ESSENTIAL OIL INGREDIENT.
600/1651
133. JP4202211 - 23.07.1992
PRODUCTION OF ESSENTIAL OIL-CONTAINING DOUBLE-STRUCTURE EMULSION AND ITS
APPLIED PRODUCT
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP4202211
Inventor(s):
KOBAYASHI TATEO (--)
Applicant(s):
JIYUMOKU CHIYUUSHIYUTSU SEIBUN RIYOU GIJIYUTSU KENKIYUU KUMIAI (--)
IP Class 4 Digits: A61L; C08F
IP Class:
A61L9/00; C08F299/00; C08F2/22
Application Number:
JP19900331898 (19901129)
Family: JP4202211
Abstract:
PURPOSE:TO OBTAIN AN ESSENTIAL OIL-CONTAINING DOUBLE-STRUCTURE EMULSION
USEFUL FOR THE PREPARATION OF A WATER-BASED ADHESIVE OR A WATER-BASED COATING
MATERIAL WHICH SUSTAINEDLY RELEASES AN ESSENTIAL OIL BY POLYMERIZING ANOTHER
DOUBLE BOND- CONTAINING MONOMER ON THE SURFACE OF AN OIL-CONTAINING RESIN
PARTICLE OBTAINED BY IMPREGNATING A SYNTHETIC RESIN EMULSION PARTICLE WITH AN
ESSENTIAL OIL UNDER SPECIFIED CONDITIONS.
CONSTITUTION:AT LEAST ONE POLYMERIZABLE DOUBLE BOND-CONTAINING MONOMER
COMPRISING A MONOMER HAVING A FUNCTIONAL GROUP REACTIVE WITH THE FUNCTIONAL
GROUP OF A TERPENE AND HAVING A POLYMERIZABLE DOUBLE BOND ON THE SURFACE OF
AN OIL-CONTAINING RESIN PARTICLE PREPARED BY EMULSION-POLYMERIZING BY A USUAL
METHOD A MIXTURE OF AN ESSENTIAL OIL CONTAINING A TERPENE HAVING A
POLYMERIZABLE DOUBLE BOND AND/OR A FUNCTIONAL GROUP WITH A MONOMER FREE
FROM A FUNCTIONAL GROUP AND HAVING A POLYMERIZABLE DOUBLE BOND.
601/1651
134. JP4212804 - 04.08.1992
FANCY VENEER-CLAD WOODY FLOOR MATERIAL GRADUALLY EMITTING ESSENTIAL OIL FOR
PROLONGED TERM AND CONTROL METHOD OF GRADUAL EMITTING OF ESSENTIAL OIL
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP4212804
Inventor(s):
SUEHIRO KOICHI (--)
Applicant(s):
SANYO KOKUSAKU PULP CO LTD (--)
IP Class 4 Digits: B27K; B27D; E04F
IP Class:
B27K3/02; B27D5/00; B27K3/12; B27K3/34; E04F15/04
Application Number:
JP19900406327 (19901205)
Family: JP4212804
Equivalent:
JP2941435
Abstract:
PURPOSE:TO PROVIDE A FANCY VENEER-CLAD WOODY FLOOR MATERIAL CAPABLE OF
GRADUALLY EMITTING ESSENTIAL OIL FOR A PROLONGED TERM AND A METHOD FITTED TO
GRADUALLY EMIT ESSENTIAL OIL FROM THE WOODY FLOOR MATERIAL FOR A PROLONGED
TERM.
CONSTITUTION:IN A WOODY FLOOR MATERIAL, IN WHICH FANCY VENEERS ARE LAMINATED
AND BONDED ON A BASEPLATE FLITCH WHILE TOP-COATING IS EXECUTED, ESSENTIAL OIL IS
CONTAINED IN THE INTERNAL LAYER OF SAID WOODY FLOOR MATERIAL AT THE RATE OF
2G/M<2> OR 10G/M<2> SO THAT SAID ESSENTIAL OIL IS VOLATILIZED SLOWLY AT THE RATE
OF 0.0005G/M<2>-0.005G/M<2> PER A DAY FROM THE SURFACE OF THE FLOOR MATERIAL
AND ESSENTIAL OIL IS EMITTED FOR A PROLONG TERM. THE ANTIFUNGAL PROPERTIES,
VERMIN- PROOFNESS AND MOTH-PROOFNESS OF A RESIDENTIAL SPACE CAN BE MAINTAINED
FOR A PROLONGED TERM.
602/1651
135. JP4217910 - 19.06.1991
COSMETIC COMPOSITIONS FOR TOPICAL APPLICATION COMPRISING ESSENTIAL OILS.
URL EPO = http://v3.espacenet.com/textdoc?F=3&CY=ep&LG=en&IDX=JP4217910
Inventor(s):
RICHOUX ISABELLE (FR)
Applicant(s):
OREAL (FR)
IP Class 4 Digits: A61K
IP Class:
A61K7/48; A61K7/00; A61K7/06; A61K9/127
E Class: A61K8/92C; A01N65/00+M; A61K8/14; A61K9/127B2; A61Q15/00; A61Q17/02
Application Number:
EP19900403450 (19901205)
Priority Number: FR19890016479 (19891213)
Family: JP4217910
Equivalent:
CA2032105; DE69005801; ES2062462; FR2655542
Cited Document(s):
EP0347306; FR2490504; FR2485921
Abstract:
COSMETIC COMPOSITION FOR TOPICAL APPLICATION, CONTAINING ESSENTIAL OILS
COMPRISING, IN A CONTINUOUS AQUEOUS PHASE FOR DISPERSION, IONIC OR NONIONIC
AMPHIPHILIC LIPID VESICLES STABILISING A DISPERSION OF DROPLETS OF ESSENTIAL OILS.
IN THE COMPOSITION THE ESSENTIAL OIL IS PRESENT IN A PROPORTION OF 0.1 TO 16% BY
WEIGHT RELATIVE TO THE TOTAL WEIGHT OF THE COMPOSITION, AND THE WEIGHT RATIO OF
THE LIPID PHASE TO THE ESSENTIAL OIL IS BETWEEN 0.2 AND 4. THE ESSENTIAL OILS
EMPLOYED IN PARTICULAR HAVE AN ANTIBACTERIAL AND/OR ANTIFUNGAL ACTIVITY, IN
603/1651
PARTICULAR AN ACTIVITY AGAINST THE GRAM-POSITIVE BACTERIA FOR THE PREPARATION OF
DEODORANT OR AN INSECT-REPELLENT ACTIVITY.Description:
COMPOSITION COSMETIQUE POUR APPLICATION TOPIQUE CONTENANT DES HUILES