History of CO2 Gas Analysis of Air by Chemical Methods
Dipl. Biol. Ernst-Georg Beck StD, 31 Rue du Giessen, F-68600 Biesheim,
egbeck@biokurs.de, 3/2007
Content
Part 1
1. Summary of actual knowledge on CO2 gas analysis in air (2006)
p. 3
Part 2
2. Methods of CO2 gas analysis in air
2.1
2.2
2.3
2.4
p. 15
Relative IR spectroscopic determination of the background level of carbon dioxide since 1958
Direct chemical determination of local effective CO2 concentration prior to 1958
Methods of historical CO2 gas analysis in air by chemical means
Sources of errors and summary
p. 15
p. 16
p. 23
p. 33
Part 3
3. Results of chemical CO2 gas analysis in air 1800 –1961
p. 34
3.1 Data of historical CO2 gas analysis in air by chemical means
3.2 Correlation of CO2-concentration with surface temperature
3.3 increase of CO2 between 1880 and 1927
Müntz p. 52, Heine p. 54, Spring p.54, Uffelmann p. 56, Petermann p. 57, Heimann/v.Frey p. 57,
Letts&Blake p. 60, Brown&Escombe p. 61, Benedict p. 62, Lundegardh p. 63, summary, p. 66,
Montsouris p. 67
p. 34
p. 49
p. 52
3.4 Verification of the CO2 maximum 1942
p. 68
Kreutz p. 68, Duerst p. 70, Buch p. 72, Lockhart p. 72, Misra p. 73, Hock/Scholander p. 74, Scandinavian
Network p. 75, Steinhauser p. 76, summary p. 77
Part 4
3.5 Verification of further CO2-maximas 1857 and 1876
p. 78
v. Gilm p. 79, Schulze p. 79, Haesselbarth p. 81, Farsky p. 83, Reiset p. 84,
summary p. 87
3.6 Evaluation of the CO2 characteristics before 1857
p. 88
de Saussure p. 89
3.7 Monthly cycling of carbon dioxide content according to lunar phases
p. 91
4. Discussion
p. 93
5. Conclusions
P. 100
6. References
P. 102
Continuing with PART 4
2
,
3.5 Verification of further CO2-maximas 1857 and 1876
78
Part 4
3.5
Verification of further CO 2-maximas 1857 and 1876
Twentynine yearly averages, chemically determined are used to contruct CO 2 concentration between
1857 and 1880, two are interpolated and nine resulted on measuring series lasting several month and
years: v. Gilm, Schulze (2x), Smith, Reiset (2x), Farsky, Haesselbarth und Montsouris.
Predomination measuring procedure was the Pettenkofer method partly modified. Duration of analysis of
one sample was up to 24 hours conducted by Reiset. Measurements from different authors differ in
regularity of sampling (irregular days a month or time a day) which resulted in distorted diurnal and
seasonal variation and comparison between scientists is difficult. Sampling of Schulze, Farsky, and
Haesselbarth was mostly daily at the same time and conducted by a tube through the window of
analysing laboratory of the agrocultural station so possible errors of contamination are excluded.
Smith used the Petterkofer method ( oxalic acid for titration) and sampled a comprehensive amount of
data throughout England and Scotland in cities and rural areas. The data sampled in rural Scotland are of
special interest [206].
Fig. 76 shows uncorrected CO2 concentration since 1857 up to 1880 determined chemically.
Since 1857 used methods were calibrated against each other resulting in maximally average accuracy <=
3% (since v. Gilm 1857). Reconstructed curve fell down since 1857 from approx. 400 ppm to a low of
approx. 300ppm around 1870 and rises again up to 1876forming a new little maximum. Despite beeing in
error range of 3% this little maximum correlates with the IPCC temperature maximum and the 1857 CO 2
maximum fits to the GHCN temperature peak in 1857 (see fig. 33).
Fig. 76 Envelope of reconstructed CO2 concentration from 29 yearly averages chemically determined in
Europe 1857 – 1880 uncorrected showing maximum around 1857 und 1876.
CO2 maxima around 1857 and 1876 are essentially based on the analyses conducted by v. Gilm
(Innsbruck, 1856/57, corrected average: 383 ppm), Schulze (Rostock, 1863/64, corrected average: 351
respectively 361 ppm), Smith ( Perth, Scotland 1866, 336 ppm), Henneberg (Weende, 1872, 320 ppm),
Farsky (Tabor, 1874, 346 ppm) and Haesselbarth, Dahme 1874, 330/340 ppm). With the exception of
Smith there are comparing tests researchable of all other authors. Data from Tissandier 1875 (one day in
march), Claesson 1876 (31 values in 1 month) and Montsouris 1877 (1 year with remarkable low values)
are not included in Fig. 76.
Measuring series at Montsouris (Paris) are not reviewed here referring to Stanhill [112].
3.5 Verification of further CO2-maximas 1857 and 1876
79
Fig. 77 CO2 gas analysis of air in the garden of his institute of university of Innsbruck (Austria) conducted
by H. v. Gilm from november 1856 to march 1857( 19 samples). Full moon: 12-11-1856, 11-12-1856, 101-1857, 9-2-1857 [191].
The chemist Hugo v. Gilm worked under the famous austrian chemist Hlasiwetz and used one of the
accuratest methods at that time [104]). V. Gilm was the first researchable scientist, who tested his
analysing procedure against air with known CO2 content achieving an accuracy of +-2,8%. Thereby he
checked amount of CO2 absorption in Baryta Water. Pettenkofer himself, who experimentated in parallel
compared accuracy of his titration method to v.Gilm´s procedure ( [58] and [138], p. 178). A test in winter
1858 (?) in Munich results in 452 ppm. Comparing measurements to the method of v. Gilm result in a
deviation of 3,5%.
The measuring series (6 month, 19 samples) in winter 1856/57 in Innsbruck displayed clearly the
seasonal winter maximum in december 1856 with approx. 435 ppm. In march of the following year only
390 ppm was measured. Combining a guessed Innsbruck summer average 1857 of 350 ppm with a
winter average of 416 ppm we can calculate a yearly average of 383 ppm (see table 4 ). Despite the few
samples analysed by v. Gilm quality of sampling and analysing procedure is comfirmed by displaying
monthly cycling with 3 corresponding CO2 maxima at full moon.
Daily sampling of air by the chemist Prof. Franz Schulze in the Agricultural Experimental Station in
periphery of Rostock, Baltic Sea, Germany 1863/64 [139] show accurate seasonal variation [140].
3.5 Verification of further CO2-maximas 1857 and 1876
80
Fig. 78 CO2 gas analysis of air in Rostock, Baltic sea by Franz Schulze 1863-64. Full moon [191]: 11-251863, 1-23-1864, 4-22-1864, 5-21-1864, 8-17-1864, 9-15-1864, 10-15-1864, 11-13-1864, 12-13-1864.
Fig. 79 Location of Agricultural Station Rostock (Baltic Sea) outside the city (above photo of the city of
Rostock 2006 [139]).
Above right corner: Franz Schulze, Prof. in chemistry and pharmacology 1850 –73 University of Rostock
[139]
The late autumn in 1863 at Rostock was warmer compared to 1864 (140). Regularly sampling in 13
month show a rise in CO2 concentration which corresponds to the contour of temperature (IPCC and
other sources). Furtheron again monthly cycling is evident and the correlation to lunar phases is striking.
3.5 Verification of further CO2-maximas 1857 and 1876
81
Average of all samples is 359,7 ppm. Schulze was in doubt of the precision of his measurements
because of high level of values and hesitated in publishing his findings. At the same time R.A. Smith
measured in several rural areas of Scotland similar values and a summer (august, september) average
level in 1865 of 336 ppm using Pettenkofer method [206].
Schulze examined was in doubt of his procedures leading to a new measuring series in 1868 to 1871.
([140], vol. 14, 1871, p. 366)
These analyses using a modified Pettenkofer process and conducted in university of Rostock by sampling
air through a tube in the window of laboratory 6-7 m above ground ( see position of university within
historical city (exact location: Bluecherplatz [140]) in fig. 79 display also seasonal variation however with a
level of approx. 50 ppm lower. Accuracy since 1870 was especially high. Three years average was 291,3
ppm. Again rising contour fits to rising temperature and monthly variation to lunar phase.
Fig. 80 CO2 measurement of air in Rostock (Baltic Sea) by Franz Schulze 1868-71 [140] compared to
IPCC temperature showing monthly cycling. Full moon : 10-1-68, 4-26-69, 6-24, 8-22, 11-12, 1-17-70, 317, 7-12, 10-9, 12-8, 5-7-71, 5-5.
Schulze discussed in detail influence of weather and wind eg. from the baltic sea containing less CO 2.
Between 1874 and 76 P. Haesselbarth and J. Fittbogen [141] conducted daily CO2 measurements in the
Agricultural Experimental Station at Dahme (Prussia, near Berlin). Franz Farsky had visited Haesselbarth
and analysed air Tabor [142] (Bohemia) at the same time. Both used Pettenkofer method by Schulze
Rostock.
3.5 Verification of further CO2-maximas 1857 and 1876
82
Fig. 81 Location and 1940 view of Agricultural Experimental Station at Dahme (Prussia near Berlin, [143])
founded in 1857 by Hermann Hellriegel.
Hellriegel, director of Station at Dahme had discovered root-fixation of N2 by bacteria in 1886.
Procedures and equipment wer nearly identical used by Haesselbarth and Farsky sampling air by a tube
through laboratory window.
Haesselbarth did air sampling every morning between 8.30 am and 11.30 am in 2,85 m height from
courtyard of Agricultural Station in periphery of the small rural town of Dahme (Prussia), which was in
former times a center of agricultural research.
Abb. 82 Diurnal CO2 variation measured on 24th /25th of july 1876 at Dame (Prussia) by Haesselbarth
Additionally careful protocolling of several meteorological data by Haesselbarth can be researched. Since
1875 Fig. 83 display a typical seasonal contour. Because of starting his measurements in july a precise
judgement of the year 1874 is difficult. Accuracy of work can be seen in several analyses of diurnal
variation of CO2 (fig. 82) and minimal amplitude varaitions (fig. 83).
Care, reliable Pettenkofer method and regularly measurements of 347 samples in rural location do no
doubt quality of data despite distorted seasonal variation showing an average of 334 ppm.
3.5 Verification of further CO2-maximas 1857 and 1876
83
Fig. 83 CO2 analysis of air near Dahme (Prussia) by Haesselbarth and Fittbogen 1874/75. Full moon: 1015-1874, 12-23, 8-17-1875, 10-14.
F. Farsky conducted 295 measurements during same years as Haesselbarth 1874/75 in periphery of little
bohemian town Tabor ( today Czechia) [142] at the Agricultural Station.
He started his analysis of nearly daily samples according the schedule of Schulze and Fittbogen and
several tests in october 1874. Samples are collected in rural location in spring and summer in the morning
and autumn and winter in the afternoon by a tube through the window of a building facing a rural street in
free surround at aheight of 4,5 m in eastern direction.
Fig. 84 CO2 analysis of air near Tabor ( today Czechia) by F. Farsky 1874/75 [142]. Full moon: 10-251874, 11-24,12-23, 2-20-1875, 3-21, 4-20, 5-20, 7-18
3.5 Verification of further CO2-maximas 1857 and 1876
84
Fig. 85 Old agricultural school outside Tabor (Cz) [169, 142], location of measurements by Franz Farsky
1874/75
Out of almost daily measurements a 10-days-average (decade) was calculated and plotted. Fig. 84
displays seasonal variation and full moon maxima as the accuracy of the Pettenkofer method with a
yearly average of 346 ppm.
1872/73/75 and 1879 French chemist Jules Reiset conducted CO2 measurements near Dieppe
(Normandy, North Sea, France) and Paris. 1872/73 analyses of 92 samples are conducted in his field
station 8 km southern to Dieppe, at a height of 96 m above ocean level, resulting in an average of 290
ppm. 27 measurements in a deciduous forest resulted in an average of 292 ppm; in the field with
blooming red clover he measured in june the average of 289,8 ppm and in 30 cm above ground in a field
of barley in july 281,9 ppm. In Paris Reiset measured in 1873, 1875 and 1879 in the street of Vigny in
may: 302,7 ppm. ( all values averages) Please notice unusual low values in the fields with high soil
respiration.
In [66] 1879 he described the very high carbon dioxide levels measured the past and documented in
literature as 400 – 600 ppm and a strong fluctuating concentration in air.)
He constructed sophisticated portable analysers using the Pettenkofer procedure with a huge volume of
aspiration of 600 l (Reiset´s tower) for absorbing air in Barium Hydroxide titrating resulting carbonate by
sulfuric acid. In contrast to german and other scientists air was dried by flowing through a U-tube with
sulfuric acid ( see fig. 86). Reiset did not realize that this results in too low values because of CO 2
absorption in H2SO4 ([181] p. 83; Bunsen absorption coefficient H2SO4 at 25°C = 0,96; H2O at
25°C=0,759; [198]) These systematic errors were known since 1848, Hlasiwetz [103] 1856 and Spring
[181] 1885 determined these absorption losses to 7-10% or about 20 ppm.
I cite here the refering sentence out of reference [144], p. 165:
Fig. 86 Scan of reference [144] showing proof of drying air by sulfuric acid in Reisets equipment
3.5 Verification of further CO2-maximas 1857 and 1876
85
Fig. 87 Location of field station in Dieppe (France) of J. Reiset 1872-80 and first part of analysing
equipment (144)
In Reisets mobile analyser samples are drawn at aheight of 4 above ground, whole anlysis procedure
lasts beetween 7 and 24 hours, average 9 hours.
Abb. 88 Mobile CO2 gas analyser of J. Reiset used near Dieppe (F) 1872-80 including tower like
aspirator (2 m) with a volume 600 L (144)
In (144, 1882) he precisly described his apparture and careful procedure. Unfortunatedly he did not
measur at regularly times sometimes during daytime then at night and not daily. The result is seen in
fig.89 showing a distorted image of seasonal variation and no diurnal fluctuation is researchable.
Reiset knows diurnal and seasonal variation from de Saussure and Boussingault nevertheless he
critisized de Saussure for his high level values as Marie-Davy of Montsouris observatory Paris for his
strongly fluctuating values within 4 years 1877 to 1880 and Schulze for his contradicting results
measured in 1868-71 accusing him using a erroneous method. This though Schulze´s average in 18681871 of 291 ppm was almost identical to Reiset´s 294 ppm für 1872/73 war.
He claimed Schulze´s values in 1863/64 as wrong furtheron he tried to contradict Schulze´s postulate that
wind direction and absorption capacity of the ocean influence carbon dioxide concentration if air.
In total Reiset´s comments show the concurrence of French and German scientists at war times in
1870/71 to get scientific honours.
Because of procedural and systematic errors only some data of Reiset are presented here.
86
3.5 Verification of further CO2-maximas 1857 and 1876
Fig. 89 Analysis of 92 air samples near Dieppe (Normandy, France) by J. Reiset in 1872/72. Full moon:
7-20-72, 2-12-73, 3-14, 4-12, 5-12, 6-10, 7-10.
Reisets data sampled 8 km near North Sea have to display a seaonal variation of at least approx. 25
ppm. Fig 89 shows an untypical fluctuation with lows in winter and highs in summer. Nevertheless the
graph with 10 days averages show some lunar phase correlation, irregular measurement intervals
prevent displying precise monthly cycling. Perhaps Reisets impressive equipment with huge aspirated air
volume was rather than for demonstrating accuracy to French Academy of Science. The equipment of
Krogh, Lundegardh, Schuftan and Scholander demonstrate that accurate and fast measurements are
possible without such large air volumes.
According to Martin et al. [106], Kauko [63] and Kleiber [111] absorption efficiency of CO 2 is dependend
on concentration of absorption solution, speed of gas flow and design of absorption equipment. Errors
risewith large volumina [111]. Incontinous sampling was mentioned above.
Reiset led Pettenkofers fast and simple method ad adsurdum beeing not able to analyse diurnal variation.
The erronous too low values of Reiset can be seen analysing his data sampled in 4 m to 30 cm above
ground in forest and cultivated field.
Other authors e.g.Wollny [161] and Lundegardh [52] had found different values:
free air
red clover
Reiset
290 ppm
289,9 ppm (-0,04%)
Wollny
2m (- 6%)
Lundegardh
317 ppm
Rommell*
Meinecke*
Gut*
De Selm (164) 320 ppm (summer)
from Duerst ([67], p. 308)
barley and other
281,9 (–2,8%)
forest
292 (+ 0,7%)
oat (up to –40%)
2m ,( up to +70%)
treetop ( up to +70%
> + 100%
~ + 72%
1, 2 m ( +68%)
Table 7 Comparison of measurements in free air and area with vegetation
Nervertheless Reiset´s work was mentioned as exemplary and especially accurate throughout
contemporary literature e.g. Letts& Blake [53]), Brown&Escombe [145,146], Lundegardh, [52] Callendar
[113,119], Keeling [147]. Brown and Escombe actually used Reiset´s absorption apparatus in 1898
modified from 600 l to approx. 200 – 300 liter air. Callendar praised Reiset´s measurements as the most
reliable accuracy of which was not achievedlater on despite citing Lundegardh who conducted
measurements in southern Sweden using a Pettenkover variant displying lowest error range of +-1% in
1920-1926. Keeling [147] did a detailed discussion of Reiset´s data and denoted them without errors too
and certified measurements precision of modern age (1986). This is remarkable because accuracy of
Reiset´s Pettenkofer variant was approx. +-3%, that means 9 ppm compared to carbon dioxide
3.5 Verification of further CO2-maximas 1857 and 1876
87
concentration in air at that times of approx. 300 ppm. A diurnal variation of 5 ppm at night is therefore not
possible to measure because of long analysing time as Keeling postulated in [147, p. 96].
Fig. 90 CO2 -analysis of air by . Reiset 1872/72 cited by From& Keeling (1986) compared to Reiset´s data
out of original paper [144]
Fig 90 displays Reiset´s data averaged per month found in [147, p. 96, Fig. 3] (left part) sampled in
1872/73 [144]. Comparison of data extracted out of Reiset´s peper [144] to the data cited by From and
Keeling results in poor correlation with lacking july/august 1873 data. From&Keeling´s graph show a
seasonal variation which cannot be extracted out of the original Reiset paper.
Summary:
Data sampled and analysed by v. Gilm 1856/57, Schulze 1863/64, Haesselbarth 1874/75, Farsky 1874/75 and Reiset
1872-1879 were summarized. Despite of a less amount of values prior to 1880 CO 2 data fit well to temperature
maxima (IPCC) around 1857 and around 1876. All inspected measurements reflect a monthly cycling
corresponding to lunar phase change by displying CO 2 maxima during full moon. With exception of
Reiset´s data showing procedural and systematic errors ( in the order of 20 ppm too low) not considered
by modern scientists (e.g. Callendar, Keeling) and all consecutive institutions in 20 th century( WMO,
IPCC) great majotity of available data show higher CO 2 values as reconstructed out of ice core data.
3.5 Verification of further CO2-maximas 1857 and 1876
3.6
88
Evaluation of the CO2 characteristics before 1857
Evaluation of CO2 measurements prior to 1857 ( see table 4) is difficult because of few data, lacking
calibration, comparative measurements and some prooven systematic and procedural errors ( e.g.
Thenard, Brunner, Regnault) e.g. using highly absorptive sulfuric acid for drying air. Using of gravimetric (
Thenard, Brunner, Boussingault) and volumetric (Regnault) analysing procedures as open systems
including eudiometers which allowed determination of CO2 as a difference of O2 and N2 results in partly
inaccurate data.
( see discussion of methods)
Additionally no continous sampling was conducted so preventing of accurate tracking diurnal and
seasonal variation.
Previous review of historic data reveals in contrast to modern published conclusions that carbon dioxide
content of air follows temperature and so climate in agreement with known laws of thermodynamics and
dissolution. Indication is drawn out of inspection of extended temperture measurements available down to
1740 in northern hemisphere and reliable since approx. 1820 [51]. Modern temperature graphs published
by IPCC, Hansen or others present data only since approx. 1880.
Here I present the result using approx 17 averages since 1812 (see table 4)showing an error range not
beeing able to quantify accurately:
Fig. 91 Envelope of CO2 –analysis in air by chemical methods prior to 1857 (see table 4) compared to ice
core analysis, showing Tambora volcanic event in 1815, de Saussures measuring series and 3% error
range since 1856 (v. Gilm).See linear falling trend up to the late 19 th century.
Total 19th century average using 81 yearly averages since 1812 –1900 (data 1880 –1900 not included in
Fig. 91) result in 322 ppm in contrast to 285 ppm published by modern climate scientists showing a
difference of + 11,5%. Dispite of unknown accuracy prior to 1857 outstanding carefull analysed data by
de Saussure (1811-1830) indicate higher level of air content in the beginning if the 19 th century compared
to the late decades with lowest levels around 1890 corresponding to low levels in temperature. High
temperatures can also be seen in extended temperature measurements compiled by Angell et al.1885
showing a peak around 1825 see fig. 94.
Out of 17 reviewed papers dating back to first half of 19th century I will present extracts of the work of two
scientists to show characteristics of data analysed prior to 1857.
3.5 Verification of further CO2-maximas 1857 and 1876
89
Fig. 92 Chemical analysis of CO2 in air of Paris by Boussingault 1829-1841.
J.B. Boussingault, famous French chemist at university Lyon and Paris conducted several series of
measurements of CO2 in air in France between 1833 and 1853 [53, 200]. In early years he determined
CO2 content in air at Lyon to 600 –800 ppm [201]. Later on he calculated the amount of carbon dioxide
produced in Paris within 24 hours to 2,9 x 106 m3. Between january 1840 and july 1841 he conducted 142
almost daily measurements in Paris using the Brunner apparatus (gravimetric, drying air by sulfuric acid)
resulting in an average of 400 ppm ( see fig. 92). He also sampled and analysed air in other localities
inclusive rural areas in France not presented here resulting in winter-spring 1839/40 in 365 ppm, his 48
measurements at night in Paris resulted in an average of 420 ppm in comparison to sampling at daytime
of 390 ppm which confirmed diurnal variation [199]. In total daily values sampled in his Paris series show
strong fluctuations within a 200 –700 ppm range showing local influence of the city, and systematic errors
due to weighing and absorption in sulfuric acid and others. Winter maxima of CO 2 content can be seen in
Fig. 92.
In contrast to the analyses done with Brunner and Regnault equipment since 1832 T. de Saussure used a
modified gravimetric procedure since 1800 also Thenard used 1812 for his gas analysis. He tested
several variants and had optimized his analyses until 1826 conducting several 100 measurements at
Chambeisy (Lake of Geneva) up to 1830 [50].
The latest analyses are most accurate conducted on a well ventilated grassland area, 250 m wide, soil of
clay , 16 m above sea level of Lake Geneva at Chambeisy lying 388 m above ocean level. 35 -45 l air
was sucked by an air pump through a solution of Baryta Water and the resulting carbonate precipitated by
sulfuric acid and then dried and weighed. Absorption was several hours, the absorbing vessel was
washed using HCl and combined with absorbing Baryta Water.
Data prior to 1826 by de Saussure are not presented here. Out of his measuring series between 1826 to
1830 ( approx 200 data) 66 values were selected concerning the same measuring conditions in time and
weather without rain or fog. Precise measuring cinditions are presented in chapter 2.3 [1], methods. He
tested in detail influence of humidity (rain, fog, snow and ice also of ice covered ground).
Plotted data using 66 selected values is presented in fig. 93.
3.5 Verification of further CO2-maximas 1857 and 1876
90
Fig. 93 Chemical CO2 gas analysis of air by Th. de Saussure 1826-1830 (see table 4) compared to
temperature reconstructed by Angell et al. 1985 including volcanic events and monthly cycling. Full moon:
5-11-1827, 6-9, 7-26-1828, 9-26, 10-23, 2-20-1829, 4-19, 6-17, 7-16, 8-14, 10-12, 12-10.
Strikingly is the sharp falling graph down to 1830. Some seasonal can variation also be seen. Because of
ffew data within measuring period, no calibration against other methods or later measurements a
quantifying of errors is difficult. But monthly cycling corresponding to lunar phases and relative low
variation since 1828 indicates high quality of data for that times. Yearly average in 1827 was 481 ppm,
1828: 431 ppm, 1829: 385 ppm.
Accepting aconstant systematic and procedural error through 3 years of measurements we are able to
quantify a decrease of 140 ppm which clearly correspond to the falling temperature at that times
according to the northern hemisphere reconstruction by Angell et al [165]. A comparison with Angells
temeperaturereconstruction during the whole time of chemical analysis is also interesting because all
evaluated CO2 measurements show correlation to temperature and Angells reconstruction date back to
1800.
3.5 Verification of further CO2-maximas 1857 and 1876
91
Fig. 93 Chemical analysis of CO2 of air 1812 to 1861in northern hemisphere (NH) compared to
temperature in NH (Angell et al. [165]) since 1800 including volcanic events
Angell et al. [165] used data by Jones et al. 1982 and Grovemann and Landsberg 1979 back to 1740. Th
temperature graph shows a maximum around 1827 similat than that in 1942. Correlation in contour is
relatively good. The eruption of Tambora has produced a guessed emission of 150 km3 matter compared
to Pinatubo 1991 15 times more [202]. Sulfate emission is guessed to 200 Million tons compared to
Pintubo 30 Million to. This event led to the “year without summer “ in 1816 as one of the coldest years in
200 years [203].
This analysis show that Reiset or Müntz in the late 19th century wrongly critizised de Saussure for his
high level data above 400 ppm which fell down dramaticlly later on.
3.7 Monthly cycling of carbon dioxide content according lunar phases
Included in most evaluated historic data are the correlation of a quasi monthly cycling of CO 2 in air at a
wavelenght of about 28-30 days. Full moon events correlate with a maximum in CO2 in the order of 10-20
ppm in historic papers with high seasonal variation and some ppm with low variation. Modern NDIR
measurements also displays this signal in the order of 1 ppm.
3.5 Verification of further CO2-maximas 1857 and 1876
92
Fig. 93 a Monthly CO2 cycling in modern Mauna Loa measurements 2004 according lunar phases. Full
moon at maximum.
Often there is a disconnection in summer reinstalled in autumn to winter. Causes seem to be the same as
explaining tidal forces; Occurrence, amplitude variation spreading over latitudes had to be further
investigated. Because of beeing able to find well fitted variations in nearly all historic data it seems to be s
strong test for the validity of old data. Especially the pre-1857 era concerning the de Saussure
measurement series up to 1830 gets more validity beside seasonal variation and correlation with
temperature maximum. So high CO2 levels around 1825 seems to have really existed.
5. Schlussfolgerungen:
93
4. Discussion
Data concerning historical gas analysis in air used in this study are researchable in several
comprehensive libraries and papers.
Year
Authors
1900 Letts and Blake [53]
1912 Benedict [51]
1940 Callendar [113]
1951 Effenberger [54]
1952 Stepanova [118]
1956 Slocum [128]
1958 Callendar [119]
1958 Bray [129]
1986 Fraser [149]
1986 Keeling [147 ]
2006 Beck [this study]
1 see references
Cited authors and papers
with data
Total
19 th c.
20thc.
252
252
137
137
13
7
6
56
32
24
229
130
99
33
22
11
30
18
12
49
20
19
6
6
18
18
156
82
74
Notes
only 19th century (+)
+; focus on O2-determination
cited Letts&Blake and Benedict
cited Duerst1, Misra1 and Kreutz1
citation as Effenberger
cited Duerst and Kreutz
no citing of Duerst, Kreutz and Misra
cited most important through the centuries
+, same as Callendar
+, same as Callendar;
only chemical determination until 1961
Table 8 Bibliographies and citation of papers
Inspecting more than 250 data sets available in literature I selected 156 measurement series since 1812
to 1961 reducing to 138 yearly averages ( approx. 90 000 single measurements) spread over the northern
hemisphere to reconstruct the variation of the CO2 content in air during period of chemical determination.
In contrast to modern climate science I used 74 analysed in 20th century beside 82 data sets from 19th
century too. Analytical chemistry had evolved and optimized since early 1800 up to the 30s of the 20th
century so accurate procedures and test equipment were available in form of the titrimetric Pettenkofer or
the volumetric Pettersen/Sonden/Haldane or Schuftan gas analysers.
Consequently 26 most important data, locations, methods and scientists are evaluated with the help of
test criteria to accept or reject quality of data.
Comparison with modern NDIR procedure is only possible by inspecting measurements around 1960
(Steinhauser). Results fit perfectly within the error range (3%) of chemical methods. Steinhauser got a
yearly average of 325 ppm +-3% (= +-10 ppm) in the city of Vienna in 1957/58 by using chemical
Pettenkofer procedure. At the same time Keeling conducted measurements at Mauna Loa volcano in
approx. 3000 m height in marine area resulting in a yearly average of 315 ppm +-1-4% [112]. Difference
of 10 ppm can also explained by measuring wet air in Vienna and dry air in Mauna Loa and absorbing
about 10 ppm in the oceans around Hawai and measuring in 3000m with a little lower CO 2 level.
Further criteria are the reproduction of the seasonal and diurnal variation, calibration and intercalibration
of different methods and correlation with lunar or solar influences.
For selected measurements since 1857 v.Gilm/Pettenkofer an intercalibration was researchable with
systematic errors within 3%. Solar and lunar influences were imaged by most of reviewed data sets in
contrast to published literature especially by Callendar and Keeling.
Between 1800 and 1961, more than 380 technical papers that were published on air gas analysis
contained data on atmospheric CO2 concentrations. Callendar [113, 117, 119] Keeling and the IPCC did
not provide a thorough evaluation of these papers and the standard chemical methods that they
deployed. Rather, they discredited these techniques and data, and rejected most as faulty or highly
inaccurate [119, 141,147, 149, 150, 154].
Though they acknowledge the concept of an ‘unpolluted background level’ for CO 2, these authors only
examined about 10% of the available literature, asserting from that that only 1% of all previous data could
be viewed as accurate (Müntz [71, 152, 153], Reiset [144], Buch [78].
During the 100 years of using the historic equipment and methods most basics of modern knowledge in
medicine, biology and physiology had been established taught today in every texbooks of this diciplines.
5. Schlussfolgerungen:
94
The most important are
The photosynthetic balance
The cell respiration balance
Blood gas metabolism
Basic Metabilic Rate (BMR) of man and animals
and so on.
6 CO2+ 6 H20  C6H12O6 + 6 O2
C6H12O6 +6 O2 -> 6 CO6 + 6 H2O
Several Nobel prices had been awarded to involved scientists (Krogh 1923, Warburg 1933), Benedict
was aNobel nominee in 1923 and other awards will be assigned to outstanding scieentific work bearing
the name of many of the authors mentioned in this study as for example the Schuftan Memorial Prize in
Process Design in Chemical Engineering (UK)- and the Pettenkofer-Preis (medicine, D).
Other scientists as Lundegardh made revolutionary contributions to the insight of ecology and olant
physiology e.g. by the invention of the flame photometer 1929, or the discovery of the cytochromes in
1950, [100]. And without the accurate determination of blood gas levels by the analyser of van Slyke 100
000s of patients were died during last 70 years.
Modern greenhouse hypothesis is based on the work of G.S.Callendar and C.D. Keeling, following S.
Arrhenius, as latterly popularized by the IPCC . Review of available literature raise the question if these
authors have systematically discarded a large number of valid technical papers and older atmospheric
CO2 determinations because they did not fit their hypothesis? Obviously they use only a few carefully
selected values from the older literature (<1%), invariably choosing results that are consistent with the
hypothesis of an induced rise of CO2 in air caused by the burning of fossil fuel. Evidence for lacking
evaluation of methods results from the finding that as accurate selected results show systematic errors in
the order of at least 20 ppm. Most authors and sources have summarised the historical CO2
determinations by chemical methods incorrectly and promulgated the unjustifiable view that historical
methods of analysis were unreliable and produced poor quality results.
Starting point of the modern greenhouse hypothesis were the publications of G.S: Callendar who defined
the criteria for an accurate CO2 content of air. Acceptable values should not vary more than „10% from
the general average of time and region“. Measurements for biological purpose were inacceptable. [113].
Fig. 94 G. Callendars definition of acceptable CO2 values in 1958 [113]
Therefore Callendar rejected all data prior to 1870 because of 50-100% differences betweenthe averages
of past authors. So natural variation was excluded as a possible cause.
The only accepted 19th century authors were Reiset (a), Müntz (b), Letts&Blake (c) and Brown&Escombe
(d, see fig 95) certifying the average of these 4 sources of 290 ppm an accuracy of 1%. The only criteria
were size of value and weather, no quantitative evaluation of methods, locations, seasonal or diurnal
variation and other which had revealed the systematic errors of procedures used by Reiset and Müntz of
at least 10%.
5. Schlussfolgerungen:
95
Fig. 95 Callendars “fuel line” [113] containing selected data according to his 10% variation criteria
ignoring data by Duerst, Kreutz, Misra, Lockhart and Scholander measuring the 1942 peak.
Fig. 95 shows callendars selction of data with a, b, c (19th century) and 1-12 (20th century).
He did not correct the 3 month Lets&Blake series in spring 1897 for seasonal variation and mostly rainy
days. Brown&Escombe used the erroneous Reiset method and had incontinous data.
Used 20th centuries data ar given in fig.96.
Fig. 96 Callendars 20th century data [113] containing selected data according to his 10% variation criteria.
Callendars citing of Benedict, Lundegardh, Buch, Haldane was erroneous and selectively too low ( see
chapter 3.3), e.g. Lundegardh measured from 1920-1926. Carpenter was not able to detect seasonal
variation within a year. Recalculating the averages of Buch´s values show higher ppm and must be
5. Schlussfolgerungen:
96
corrected because of lacking data and sea absorption ( see chapter 3.3). The Haldane value of 324 ppm
was an average of 153 samples only in august showing low summer levels. Combining with 386 ppm at
night it would be 355 ppm and still too low because of lacking winter data. He ignored data measured by
Haldane at the coast in august and september with an average of 370 ppm.
In the end Callendar did not realize the procedural errors of the analysis conducted by the scandinavian
network between 1950 and 60.
Because of his attempt to proove his “fuel line” a verification or falsification of a huge amount of available
other data (see Stepanova [118]) especially Duerst, Haldane, Kreutz, Misra, Scholander was not
undertaken.
In total Keeling joined this view of literature and also presumed overall contamination, faulty methods or
local industrial influence [147].
Fig. 97 Keelings reproduction of Callendars „fuel line“ with the Reiset CO2 average of 292 ppm fitting in
ice core reconstruction of CO2 by Neftel et al.(1985) [147]) fig. 10, p. 102. Actual value without absorption
error supplemented as *.
292,4 ppm as the average of Reiset is praised by Keeling as the accuratest at the end of the 19th
century, concerning the five mesuring series Callendar had choosed. In other papers Keeling denoted the
Pettenkofer method as extremly inaccurate, Reiset´s variant is judged by him as very accurate within 1-2
ppm meaning an accuracy of 0,3 – 0,7% compared to the average of Reiset. According to Stanhill
(Climate change, 1984, 6, 409) Keeling himself achieved up to 1976 an accuracy of +-4 ppm with NDIR
method because of errors.
Lundegardh 1920 measured within 1%, or +- 3 ppm using an optimized automatic apparature. Kauko
analysed Pettenkofer method thoroughly in 1932 [63] resulting in a theoretical accuracy of simple
Pettenkofer method of +-0,0006 Vol%. d.h. 2% so Keelings indication of 1-2 ppm accuracy for Reiset´s
equipment can be contradicted.
Nevertheless Keeling postulated that Reiset was the first scientist that presented correct seasonal
variation. This honor is due to Th. de Sausure 1830 and later Schultze 1864.
The accuracy of Callendars and Keeling evaluation of Reisets work is underlined by the fact that Keeling
named Reiset 1993 a Belgian and Dieppe, the location Reiset analysed would be placed at Belgian coast
[47]. Callendar confused the surname of Reiset instead of Jules he cited him as Jean Reiset. [113].
Callendar and Keeling also praised the data analysed by Müntz especially because of low CO2 levels
down to 0,02% during French expedition to Antarctica 1908-1910. In reviewed literature of Callendar and
Keeling there is no precise evaluation of the open, volumetric gas analyser of Muentz researchable. (See
5. Schlussfolgerungen:
97
the above mentioned systematic absorption errors and no seasonal and diurnal variation visible in data by
Muentz).
Other authors as de Saussure 1826-1830 or Petermann 1884 were cited erroneously and data wer
selected to fit.
Review of more then 250 papers ( approx. 200 cited here) there is no evalution of teh work of the most
accurate measurement series done by W. Kreutz 1939-1941 at Giessen, Germany. Sampling an
analysing 120 daily data with an automatic, electrified registration system for weather data led to more
than 70 000 CO2 values analysed with similar accuracy Keeling had done 20 years later. [126] showing
precise seasonal variation.
Reserach on history of CO2 gas analysis revealed that the chemist Keling did probably no study of
literature in 1954 when he began his inverstigations. He also did not use the approved Scholander
Gasanalyser available at that times because Scholander was also a member of the same institute at that
times. Ignoring available knowledge he went to the field and conducted measurements using a self made
manometer needing several hours for one value resulting in the same CO 2 concentrations at all location
he measured. [47].
Keelings merits are the development of an extremely accurate gas analyser and proof of a rising CO2
content in air since 1958.
The merits of Callendar are minor to his selective and speculative postulation of rising CO 2 since 1880 to
1930 by about 20 ppm. His speculative cause with inacceptable criteria for excluding accurate values was
burning fossile fuels so he established modern greenhouse thesis.
This study prooves contradicting Callenadar that this rise can also be reconstructed by using available
data rejected by Callendar and Keeling.
Most authors cited in this study from, de Saussure 1826 to Scholander in 1947 had the only aim to
measure as accurate as possible local CO2 concentration in air. Review of available literature shows
however that the authors in the 19th century denoted the CO 2 content in air as constant as the O2
concentration.
In 20th century e.g. Lundegardh discussed in detail diurnal and seasonal variations in available literature
since de Saussure and the dependence on weather., vegetation soil respiration and ocean/sea
absorption [52]. Because of no indication for a significant enduring natural variation of atmospheric CO 2
concentration seen in his data between 1920 to 26 he did not deal with this issue beside the fact that he
knows of Arrhenius speculations on CO2 induced temperature rise.
As mentioned above Callendar 1938 and Keeling since 1958 categorical excluded possible enduring
natural CO2 variations, denoted it as errors or ignored those data as e.g. the CO 2 maximum in 1940.
Most interestingly Fonselius [80] displayed some data forming this 1942 maximum (Duerst, Kreutz and
Misra) but ignored quality also cited by Slocum in [128].
5. Schlussfolgerungen:
98
Fig. 98 Fonselius graph of available CO2 data 1800-1955 including data showing peak in 1942 [80]. Thick
grey line is overlayed graph of CO2 analysis by chemical means (this study) showing peak in 1942,
Fonselius correctly cited. Encircled are the data Callendar used.
Analysing of backgroundlevel in maritime areas to get the actual CO 2 concentration is not the only
concept of getting well mixed CO2 data of air. Lundegardh in 1920 still discussed in detail influence of
free air by several biotic and abiotic factors and absorption of CO 2 by sea resulting a lower CO2 level in
ocean air. So Callendar was not the inventor of free air concept.
In fact only desert air was uninfluenced by biota, soil and water absorption only winds may change local
concentrations.
CO2- reconstructions out of ice cores seem to be inaccurate because not resolving CO 2 peaks presented
in this study. In several papers Jaworowski claimed this indication [176, 205] because of producing
artefacts by decompressing cores cutting them in small fractions and so resulting in gas leakage by
transition of clathrates to bubbles. So further investigations have to be undertaken to elucidate accuracy
of ice core proxies.
Carefully analysing CO2 data sampled on continental areas also supply accurate values taken into
account the severals sources and sinks and measuring under selected conditions. Especially the CO 2windspeed-relation used by F. Massen in [204] enabled to calculate by asymptotic approximation nearbackground level average out of data. Following a testing of the Kreutz data analysed 1939-40 at Giessen
(Germany) by the Massen procedure:
5. Schlussfolgerungen:
99
Fig. 99 CO2-windspeed correlation in data by Kreutz september 1939 - january 1940 at Giessen [91]
calculating asymptotic background level of 434 ppm by F. Massen [204]; CO 2 and wind data measured in
height of 14 m.
The CO2-windspeed test by Massen et al. revealed a background level at Giessen 1939/40 of 434,1 ppm
in 14 m. Kreutz averages the data to 434 ppm which means 100% agreement. So this is a further
indication of reliability of historical data.
Analysing the data of Steinhauser 1957/58 by the CO2-windspeed-test revealed the same reliability:
Fig. 100 CO2-windspeed correlation in data by Steinhauser 1957 at weather station Hohe Warte Vienna
[175] calculating asymptotic background level of 324 ppm by F. Massen [204]; CO 2
5. Schlussfolgerungen:
100
The corresponding early Keeling measurements at Mauna Loa in 1958 show a yearly mean is about 313
ppm. With a latitude correction [204] of 1 ppm we get 314 ppm. Adding a similar correction to the
Steinhauser values we get 323 ppm and a difference of 9 ppm. This is well within 3% error range derived
for Pettenkofer procedures (Steinhauser used Krogh-Pettenkofer-variant, the same was used by
Fonselius and Bischof in Scandinavian network).
So we are able to show that historic Pettenkofer process and modern NDIR-procedures fit within
systematical error range and therfore old methods are valid.
5. Conclusions
Finally let´s summarize established knowledge by historical authors reviewed in this study.
During the late 20th century, the hypothesis that the ongoing rise of CO 2 concentration in the atmosphere
is a result of fossil fuel burning became the dominant paradigm. To establish this paradigm, and
increasingly since then, historical measurements indicating fluctuating CO 2 levels between 300 and more
than 400 ppmv have been neglected.
A re-evaluation has been undertaken of the historical literature on atmospheric CO2 levels since the
introduction of reliable chemical measuring techniques in the early to middle 19 th century. More than
90,000 individual determinations of CO2 levels are reported between 1812 and 1961. The great majority
of these determinations were made by skilled investigators using well established laboratory analytical
techniques. Data from 138 sources and locations have been combined to produce a yearly average
atmospheric CO2 curve for the northern hemisphere. This curve contradicts to a 19th century or
preindustrial CO2 level of 294 ppm. By valid chemical and direct measurements the 19th century CO2
level has to revised to 341 ppm, using data since 1857 with 3% error range at least 310 ppm.
The historic data agree with the relative linearly rising CO 2 amount since 1880 to 1930 showing typical
difference of about 10-20 ppm more on northern hemisphere continental air compared to ice core
reconstructed concentrations.
The historical data that I have considered to be reliable can, of course, be challenged on the grounds that
they represent local measurements only, and are therefore not representative on a global scale. Strong
evidence that this is not the case, and that the composite historical CO 2 curve is globally meaningful,
comes from the correspondence between the curve and other global phenomena, including both sunspot
cycles and the moon phases, the latter presented here probably first time in literature and the average
global temperature statistic. Furthermore, that the historical data are reliable in themselves is supported
by the credible seasonal, monthly and daily variations that they display, the pattern of which corresponds
with modern measurements. By the CO2-windspeed-test it is possible to approximate background level
out of measurements on northern continental areas. Inspected historic measurements fit within analysed
error level. Further evidence of historic data come from comparing to oxygen level which displays
corresponding minima to CO2 maxima.
It is indeed surprising that the quality and accuracy of these historic CO 2 measurements has escaped the
attention of other researchers. Validity of historic data open discussion on actual ice core- and C-flux
models which do not fit to these observations. They have to be revised or rejected because of their basis
as a human induced climate change.
The reinvestigated historic data fill the gap IPCC has left beetween large scale time periods of hundred
thousands of years and short-time CO2 data (diurnal/seasonal). Carbon dioxide do also follow climate in
hundreds and decads of years and there are cyclic fluctuations through the centuries. Looking at CO 2
maxima around 1857, 1942 and 2001 shows a remarkable wavelenght as the Gleisberg-cycle of 70 to 80
years. This suggests a falling of CO2 and temperature in near future.
5. Schlussfolgerungen:
1. Trotz hohem fachwissenschaftlichem Stand der Chemietechnik und Bewährung in Medizin und
Biologie ignorierten Callendar und Keeling als die neben Arrhenius wichtigsten Begründer der
modernen Treibhaustheorie ( IPCC) einen großen Teil der verfügbaren Fachliteratur zu CO 2Messungen - besonders die des 20. Jahrhunderts -und selektierten nur wenige Daten, die Ihr
Forschungsziel einer durch Verbrennung fossile Kohlenstoffverbindungen erhöhten CO2Konzentration bestätigen sollten. Weiterhin beurteilten und reproduzierten sie die wenigen
historischen chemischen Messungen teilweise falsch und propagierten ein unzutreffendes Bild
über deren Qualität, ohne sich mit der Methodik auseinandergesetzt zu haben. Alle modernen
Autoren und Meetings ab ca. 1975 bis zum IPCC (UNO), die sich mit historischen Messungen
befassten übernahmen diese selektive, ignorante und unwissenschaftliche Vorgehensweise. Dies
ist die historisch nachweisbare Basis der moderenen Treibhaustheorie.
5. Schlussfolgerungen:
101
2. Durch sorgfältige Recherche historischer Fachliteratur der Chemie, Medizin, Ernährungslehre,
Physiologie und Agarmeteorologie konnte gezeigt werden, dass es vor 1958 extrem präzise
Messungen des CO2-Gehaltes der Luft mit unter 3% Genauigkeit gab, deren Ergebnisse im
Widerspruch zur veröffentlichten Meinung der Klimatologen stehen.
3. Der Vergleich des CO2-Verlaufs aus chemischer Messung mit dem Temperaturverlauf der
Nordhemisphäre zeigt, dass die CO2-Kurve präzise alle Temperatur-Schwankungen abbildet. Es
gibt also keine wie in der Literatur (IPCC) dargestellt seit dem industriellen Zeitalter exponentiell
gleichmäßig ansteigende CO2-Kurve sondern eine der Temperatur folgende Kurve.
4. Auch die vorindustrielle CO2-Konzentration der Nordhemisphäre im 19. Jh. war genau so
schwankend wie die des 20. Jahrhunderts mit einem großen Maximum um 1825 mit vermutlich
über 400 ppm, einem kleineren um 1857 von über 350 ppm. Ein konstanter, vorindustrieller CO 2Wert von 285 ppm existiert nicht und resultiert aus selektiver und fehlerhafter Betrachtung
weniger, ungeigneter historischer Daten ab 1880.
Diese Studie zeigt klar, dass die wissenschaftliche Basis der modernen anthropogenen Treibhaustheorie
des aktuellen Klimawandels nicht der Realität entspricht, weil sie durch selektive Wahrnehmung und
Ignoranz der Fakten zum Beweis einer spekulativen Theorie der beteiligten Wissenschaftler zustande
kam. Die allgemein akzeptierte vorindustrielle CO2-Konzentration von ca. 285 ppm entspricht zwar
ungefähr der tatsächlichen um ca. 1885, ist aber nur eine Momentaufnahme eines stark schwankenden,
dem Klima folgenden Verlaufs in 2 Jahrhunderten. Die moderne Temperaturkurve des IPCC (18), Abb. 32
die um 1860 beginnt suggeriert am unteren Rand eher abfallende Temperaturen, tatsächlich belegt der
historische Datensatz GHCN eine nach unten ansteigende Temperatur.
Die heute als Erkenntnisse propagierten Zusammenhänge über die Ursachen des modernen
Klimawandels sind letztendlich falsche und voreilige Schlussfolgerungen aus mangelhaften Analysen von
Callendar und Keeling wie auch Arrhenius. Callendar analysierte im Übrigen auch die spektralen
Absorptionseigenschaften von CO2 basierend auf den Arbeiten von Arrhenius, ohne bemerkt zu haben
dass dessen Analysen auf fehlerhaften spektralen Daten beruht. Die Mängel der Arrhenius-Analyse von
CO2 als Wärmeabsorber bzw,. –Emittent lässt sich wiederum durch Analyse der historischen Fachliteratur
leicht belegen (siehe Hans Erren: Arrhenius was wrong! (173)).
6. Referenzen
102
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Danksagung:
Für die freundliche Hilfe bei der Recherche historischer Literatur und Daten und Überlassung von
Materialien bedanke ich bei
Dr. L. Brake, Stadtarchiv Gießen
Jana Farová, Infocentrum Město Tábor, (Cz)
Ralph-Christian Mendelsohn, Deutscher Wetterdienst (DWD), Offenbach (D)
Dr. Franziska Rogger, Archiv der Universität Bern (CH)
Prof. Dr. Albrecht Vaupel, ehemals DWD (D)
Dr. W . Wranik, Institut für Biowissenschaften, Meeresbiologie Rostock (D)
New Sources:
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