INVESTIGATIONS OF ENVIRONMENTAL IMPACTS FROM THE DEPLOYMENT OF
DU-BASED MUNITIONS.
1.SUMMARY.
1.1. The abundance of uranium isotopes was determined in urine
specimens collected from the Gulf War I (GWI) veterans from four
countries, in 1998-9, by nuclear and mass spectrometric methods.
The abundance of the isotopes and the total uranium in 24-hour
urine specimens allowed the determination of the excretion rate of
depleted uranium (DU) from the body [1]. In this study the isotopic
abundance of U-235 has been determined by the delayed-neutrons
emitted by some fission products (for example, I-137 a fission
product that decays to Xe-136 with a half life of 24 seconds by
emitting electron {beta particle}, neutron and gamma rays [2]).
Such fission products are formed in the irradiation of fissile
material like uranium-235, the only naturally occurring isotope,
with thermal neutrons and thus permit the assay of U-235 only
without any interference from any other elements. The amount of U238, another naturally occurring isotope of uranium, has been
determined by the well-known instrumental neutron activation
analysis [3]. The capture of thermal neutron by U-238 leads to the
formation of U-239 by the reaction, U-238(n,gamma)U-239. U-239 is
assayed with the emission of its characteristic gamma rays (73-kev
energy) to Np-239 [2]. The ratio, R, of [U-235]/[U-238] permits the
evaluation of the fraction of DU and total DU in an aliquot of a
specimen [4]. This task was accomplished in 1998.
1.2. This work had a set back during the month of July 1999, when,
reasons unknown to us to date, the University of Waterloo denied
office and laboratory spaces to Professor Emeritus Hari D. Sharma
and confiscated urine specimens that were sorely needed for the
determination of the biological half life. We firmly believe that
uncontrolled release of radioactivity in the environment will
eventually have deleterious consequences. We decided to continue
the work against obstacles and with our meagre financial resources.
However, with timely help from many well-meaning persons we did
continue our work on this important problem. This study has reached
the stage that it provides definitive answers to questions that
have been lacking thus far, namely, suitability of deployment of
DU-munitions that release radioactivity in the environment and
whether it has long-range deleterious effects to the environment.
This led Dan Fahey to write two reports titled "Don't Look Don't
Find" and "Science or Science Fiction" [5,6]. We looked for DU in
urine specimens from exposed veterans and civilians and found it,
We confirmed our findings by determining DU in tissues from exposed
civilians, thus leaving no doubt that DU found its way into
civilians residing near the battlefield area through inhalation of
DU oxide contaminated air.
1.3. We invite comments and questions on our report from interested
heads of NATO countries and other organisations and individuals. We
are apolitical and therefore we request scientists and people at
large, to refrain from raising political questions. While some
damage to the environment in Iraq might have been done, we must
remember that we can still find answers to risk estimates from lowlevel exposure from internalised depleted uranium through
inhalation of DU oxides-aerosols [DUOA]. If I may be bold enough to
suggest that the protagonists should organise a very far-reaching
study before they plan to use DU munitions again that may lead to
dispersal of radioactivity. What follows now is an account of our
contribution to clarify some issues that were related to the
deployment of DU-munitions in the Gulf in 1991, in BosniaHerzegovina and in Kosovo.
1.4. A dedicated computer controlled facility at the McMaster
University Nuclear Reactor enables the irradiation of an aliquot of
urine dried in a polyethylene bag in a clean fume hood, for a preset time. After another pre-set delay time, the irradiated specimen
is assayed either for delayed neutrons with a dedicated neutron
detector or for assaying gamma rays with a high resolution
germanium detector and a pulse-height analyser for recording the
spectrum. The two methods were previously used successfully in
identifying work-related uranium in workers' tissues [Appendix I].
Eight standards were run for uranium analysis with each set of the
specimens (Appendix II).
1.5. The analytical data that are presented in this report, were on
the urine specimens that were collected during the 1998-9 period
from the GWI veterans who were allegedly exposed to DU during the
1990-91 Gulf conflict, and sent to us for the determination of DU
content. The clearance rate of DU from the veterans' bodies was
thus evaluated to be 1 to 5 micrograms of DU per day during the
1998-9 period. The excretion rate of DU in residents of Basra, who
resided there during the 1991-4 period, was found to be lower than
that from the exposed veterans. Five specimens taken in 1999 from
the residents of Baghdad during 1990 to 1994,revealed that only one
showed the presence of DU while the other four had mostly natural
uranium.
1.6. It is evident that the clearance rate must be associated with
a very slow rate of solubilization of depleted-uranium oxides
aerosols (DUOA) in body fluids or from some body compartment where
it is stored. The trans-location of DUOA may pass through many body
compartments but the rate of excretion may be controlled from at
least one component represented by a very long half life. It
appears that ingestion of DUOA must have occurred through
inhalation of the contaminated air; and that might have led to the
accumulation of the DUOA in the lungs. The clearance rate of DUOA
or at least one of the components of DUOA is associated with a very
long biological half life.
1.7. To test the accuracy and reliability of two methods (DNC and
INAA) for the determination of DU in the specimens, another method
using a surface ionisation mass spectrometer (SIMS) was followed
for the determination of abundance of the uranium isotopes in the
urine specimens [4,7]. The two sets of results agreed with each
other within the errors. The DNC and INAA methods do not require
dissolution of the specimens. However, the other method did require
complete dissolution of ceramic type of uranium dioxide in the
specimens. Results obtained from the use of ICP-MS did not agree
with the results by the use of SIMS or the DNC and INAA methods. It
was shown that only uranium (VI) compounds could be either
solubilized in the body fluids or in tissues when treated with
ultra pure nitric acid and hydrogen peroxide. It appears that
uranium compounds with the oxidation state of IV were not converted
to oxidation state of VI. Nearly five hundred analyses with ICP-MS
only showed the presence of NU in the specimens. Undissolved solids
from the digestion of tissues showed the presence of DU as
determined by the DNC and INAA methods.
1.8. Total ingestion of DU by an active GWI veteran during the Gulf
conflict, through inhalation of DUOA, has been estimated to be
about a few milligrams of DU-oxides. The ICRP model has been
followed for estimation of radiation dose from the DU [8].
1.9. Tissue specimens of deceased residents who had resided in
Basra from 1991 to 1994, were procured for testing the hypothesis
to the effect that air was contaminated with the ceramic DU oxides
aerosols for at least over a period of two years in the battlefield
area and its vicinity. Lateral dispersion of the DU aerosols would
lead to contamination of air in large urban areas near the
battlefield. Therefore, it is expected that residents of Basra
would have accumulated the aerosols through inhalation, in the
alveolar tissues in the lungs and perhaps other organs before they
were excreted from the body. The DU content in urine specimens
received from two different localities of Basra was determined with
SIMS. The results showed without any ambiguity the presence of DU
in one specimen. Air samples did not show the presence of DUOA in
air after the end of 1993.
1.10. It has been shown unambiguously that the deployment of DUbased munitions leads to contamination of air with aerosols of its
ceramic oxides. Inhalation of contaminated air then leads to
accumulation of highly insoluble particulate DU oxides in the lungs
in milligram quantities. Even such deposition of ‘mildly’
radioactive isotope does inflict harm to human health by its
attendant radiation insult under certain conditions. If the DUbased munitions have been deployed by the coalition forces during
the Gulf War II, a set of DU determinations have been suggested in
Chapter 8, to show conclusively that the DU munitions do not
violate the dictates of the Geneva conventions. It was unfortunate
no testing of environmental specimens was performed or no results
of such tests made public soon after the cessation of GWI. However,
it is now possible to conduct DU mapping in the entire country as
well as in parts of the country where extensive use of DU-based
munitions were deployed extensively during GWII.
1.11. A relatively simple and accurate methodology has been
suggested for the determination of DU in environmental specimens.
According to Goldstein et al. delayed neutron counting and energy
dispersive x-ray fluorescence (EDXRF) methods are direct solid
analytical techniques that are non-destructive, rapid and require
no dissolution step [13]. We have used the activation methods for
determining U-235 and U-238 contents. In the case of U-238, we
estimated U-239 as the indicator nuclei and high-resolution gamma
ray spectrometry. EDXRF analizes the total uranium which can be
regarded almost equal to U-238 if the specimen has DU or NU or the
mixture of DU and NU.
2. INTRODUCTION.
2.1. It is well known that over 20 per cent of the GW1 veterans
have been suffering from symptoms that are part of the Gulf War
syndrome [9]. During the conflict, the veterans were exposed to
several causative agents; and among them, DUOA from DU-tipped
missiles that were deployed for destroying battlefield tanks.
Metallic DU bullet on striking an armoured vehicle catches fire and
it burns to its oxide dust with release of large amount of heat
that aids in penetrating the armour. The ceramic oxide-dust of
micron or sub-micron size forms aerosols. Inhalation of DUOA would
lead to accumulation of the highly insoluble oxide in the lungs.
During the past five years we have endeavoured to determine the
pathways of such oxide dust in the veterans and among the civilians
for aiding in finding its toxicity in humans. Although it is well
known that the oxide dust with its isotopic ratio, R = [U-235]/[U238] as signature, enters the human body through inhalation, but
hardly any attempts have been made so far to look for its pathways
through body compartments with their respective biological half
lives [10]. No systematic epidemiological studies have been
conducted to show ‘cause and effect’ of DUOA inside the body or at
least in one of the body compartments. Lack of knowledge of its
pathways and respective parameters has prevented evaluation of
radiation insult from inhalation of DUOA or its chemical toxicity.
In this investigation, an attempt has been made to determine the
presence of DU in urine and tissue specimens by reliable methods
and therefore we suggest a likely scenario that might have resulted
in the accumulation of DUOA in the lungs and in the thoracic lymph
nodes.
2.2. Exposure to uranium is encountered by workers in mining,
milling and refining of the desired compounds needed as nuclear
fuel etc. There are three classes of compounds, namely, D, W and Y,
designated by the ICRP for assessing its radiological toxicity
[10]. The extent of human exposure to uranium is evaluated by
determining its daily rate of excretion of total uranium and the
isotopic ratio, R = [U-235]/[U-238] in 24-hour urine specimens. The
two parameters are the excretion rates of DU and NU and the ratio,
R, for evaluating DU fraction in urine that may also contain NU.
Metabolic data for uranium suggested by ICRP [10], indicates that
there is an intake of about 1.9 micrograms of uranium (mostly as
NU) in food and water. That results in transfer of about one to two
percent of the intake, from the gastrointestinal tract to the blood
stream; and that is finally excreted through urine. The daily
excretion rate among non-occupational subjects has been found to be
ranging from 3 to 310 nanograms of NU per day [11]. It is expected
that GWI veterans and civilians exposed to DU may have two
different excretion rates for the mixture of DU and NU. Exposure to
DUOA leads to accumulation of DU oxides in the lungs whereas NU
enters the gastrointestinal tract as soluble compounds of uranium.
The bio-kinetics of the two types is expected to be vastly
different. It is essential that reliable methodology for the
estimation of DU and NU must be followed for establishing the biokinetics of inhalational DU-oxide dust for assessing its toxicity.
3. METHODS FOR DETERMINING DU IN URINE SPECIMENS FROM GWI VETERANS
AND RESULTS
3.1. An aliquot of urine was drawn from a well-stirred 24-hour
urine specimen from a GWI veteran exposed to DU during the Gulf
conflict. The aliquot of a urine specimen was transferred to a
dedicated polyethylene bag and was allowed to evaporate to dryness
in a clean fumehood. The bag with the dried specimen was folded and
put in a polyethylene capsule for irradiation by using a computercontrolled facility that has been in operation for this purpose for
over thirty years at the McMaster University Nuclear Reactor. The
specimen can be irradiated several times and U-235 content assayed
each time for either delayed-neutron counting (DNC method) or U-238
by gamma-ray spectroscopy (INAA methodology[3]). Ms. Alice
Pidruczny, Manager, Analytical Services, carried out the
irradiation of the capsules and subsequent assay by the DNC method
or the INAA method. Her typical report is presented as Appendix II.
At no time did we indicate the content of the capsule to her. In
other words, the irradiation and subsequent assay was performed at
arm's length. The results are presented in Table 1.
3.2. Results from irradiations performed at the McMaster University
Nuclear Reactor for the determination of U-235 and U-238 by the DNC
and INAA methods respectively are expressed in microgram per liter.
U-235(NU) depicts all uranium evaluated by dividing U-235 content
with 0.00725, as determined in the specimen by the DNC method. It
must be noted that urine specimens are likely to have both kinds of
uranium, i.e., NU with R = 0.00725 and depleted uranium with R =
0.002015. It has been shown that 79 to 97 per cent of specimens of
environmental concerns contain NU and no DU [15]. In other words,
uranium from laboratory wares and from chemicals in the specimens
is likely to be NU and not DU or EU. Special care was, however,
taken to minimise the possibility of uranium entering from
environmental sources.
The specimens were handled in a clean
fumehood and in treated laboratory wares (Appendix III).
TABLE 1.
U-235 and U-238 content in urine specimens
from the UK veterans
Ser.
No.
Volume
mL
U-235(NU) by the
DNC# method
microgram
U-238 by the
INAA method,^
microgram
1.
74
80
0.04
0.07
0.03
0.12
0.2
<0.2
2.
76
<0.02
0.02
0.3
0.2
<0.2
0.17
Uranium
content/L*
NU#
DU#
0.47
1.19
0.2
2.7
<2.5
0.3
3.
87
77
<0.02
0.04
0.02
0.07
0.3
<0.2
<0.2
<0.2
0.17
0.71
2.3
2.1
4.
73
<0.2
0.05
0.2
<0.2
0.42
2.1
5.
86
0.02
0.03
0.6
0.2
0.29
4.6
6.
79
<0.02
<0.02
<0.2
<0.2
7.
76
76
<0.020
0.10
<0.02
0.09
<0.2
0.4
<0.2
0.5
8.
75
<0.02
<0.02
<0.2
<0.2
9.
88
77
0.03
<0.02
0.04
0.05
0.2
<0.2
0.2
<0.2
0.4
10.
75
81
<0.02
0.14
<0.02
0.07
0.2
0.2
<0.2
<0.2
IND
1.3
1.9
11.
84
75
<0.02
0.04
<0.02
0.02
<0.2
0.2
<0.2
0.3
0.4
IND
3.3
12.
81
<0.02
0.08
0.2
<0.2
0.5
1.8
13.
78
0.04
<0.02
0.2
0.5
0.3
4.3
14.
71
78
<0.02
0.11
<0.02
0.06
<0.2
<0.2
<0.2
<0.2
IND
IND
15.
78
75
<0.02
0.05
0.02
0.05
<0.2
<0.2
<0.2
<0.2
IND
IND
16.
82
0.07
<0.02
0.2
<0.2
17.
81
0.06
0.11
<0.2
<0.2
Mix
18.
75
<0.02
<0.02
<0.2
<0.2
IND
19.
78
0.10
0.10
<0.2
<0.2
IND
20.
68
<0.02
0.07
<0.2
<0.2
IND-Mix
21
80
0.05
0.08
<0.2
<0.2
22.
79
0.07
0.11
<0.2
<0.2
IND-Mix
1.1
2.5
23.
75
<0.02
0.17
<0.2
<0.2
IND
24.
77
0.03
0.03
<0.2
<0.2
IND
25.
79
0.11
0.08
<0.2
<0.2
Mix
IND
IND
1.25
5.9
IND
0.5
2.27
IND
1.83
26.
80
<0.02
0.06
<0.2
<0.2
27.
80
0.13
0.16
0.2
<0.2
28.
78
<0.02
0.12
<0.2
<0.2
29.
78
<0.02
0.12
<0.2
IND
1.8
3.1
IND
DU --depleted uranium found in the specimen. [U-235]NU -- total
natural uranium evaluated by dividing [U-235] found in a specimen
with 0.00725 = [U-235]/[U-238]. In column 3 and 4,[U-235]/0.00725
is reported where brackets [ ] indicate the quantity (in this case
U-235) in microgram. IND:- not possible to determine because either
[U-235] or [U-238] is below the detection limit and hence R for
uranium in the specimen could not be determined with the required
precision. Mix:- predicts a mixture of DU and NU. * NU stands for
natural uranium ([U235]/0.00725]) per litre and DU stands for
depleted uranium content in one litre of specimen, derived from the
R = [U-235]/[U-238] for the specimen. Both in NU and DU, the
abundance of U-238 ranges between 99.245 to 99.8 per cent. It can
be assumed that total uranium is almost equal to [U-238]. < sign
denotes less than. Concentration of uranium isotope is depicted by
[U-238] as microgram(s) of uranium in a specified volume.
-----------------------------------------------------------------
TABLE II.
DU AND/OR NU CONTENT PER LITER FOUND IN URINE
SPECIMENS FROM GULF WAR VETERANS.
Ser
No.
Remarks
[U-235]
nanograms
Errors
ng
[U-238] or
U microgram
Errors
microg
1.
Most of uranium
is DU & NU neg.
3.4
8.6
1.4
1.3
2.703
<2.500
1.912
1.769
2.
Mostly DU -~90%
1.4
1.3
3.289
1.97
3.
1. Mostly DU
2. U-238 not
accurate
1.23
5.12
1.2
1.3
2.299
IND <2.597
1.626
1.838
4.
Mostly DU, NU-N
3.0
1.4
2.055
1.959
5.
Mostly DU, NU-N
2.1
1.2
4.65
1.645
6.
IND
<1.83
1.3
<2.53
1.79
7.
1st. IND, 2nd.
DU
1.9
6.9
1.3
1.3
<2.63
5.921
1.86
1.86
8.
IND
1.9
1.2
<2.67
1.89
9.
1. DU 2.U-238
not k.a.
2.9
2.8
1.2
1.3
2.273
<2.597
1.61
1.83
10.
1. Needs better
measurements
1.9
9.4
1.4
1.3
2.000
1.852
1.89
1.75
11.
1. IND
2. DU
1.7
2.9
1.2
1.4
<2.38
3.333
12.
1. DU
4.0
1.3
1.852
13.
1. DU
2.3
1.3
4.321
Ser
No.
Remarks
14
1. IND
2. IND
Pr. DU+
[U-235]
nanograms
Errors
+/-ng
2.0
7.9
1.68
1.889
1.75
[U-238]
micrograms
Errors
+/-mig
1.4
1.3
<2.82
<2.564
1.993
1.814
15
IND Needs U-238
content with b.a
1.4
4.8
1.3
1.4
<2.56
<2.667
1.81
1.89
16
DU
3.3
1.3
1.829
1.73
17
DU+
7.6
1.3
<2.469
1.75
18
DU
1.9
1.4
2.667
19
M.L. DU Needs Ut
9.3
1.3
<2.564
1.81
20
M.L. DU Needs Ut
4.0
1.5
<2.941
2.081
21
DU+ Needs Ut
5.9
1.3
<2.500
1.77
22
DU + NU R=0.0033
8.3
1.3
2.532
1.79
23
NU+DU R=~0.004
8.7
1.4
<2.667
1.889
24
DU+ Needs Ut
2.8
1.3
<2.597
1.84
25
NU likely
8.7
1.3
<2.532
1.79
26
DU+NU Needs Ut
3.2
1.3
<2.500
1.77
27
DU+NU R=0042
13.2
1.3
3.125
1.77
28
DU+ Needs Ut
2.7
1.3
<2.439
1.726
29
DU+NU Needs Ut
6.0
1.3
<2.564
1.814
1.887
< = less than; DU in this study stands for depleted uranium with
R=0.002015; NU = natural uranium with R=0.00725. Ut=total uranium
or almost = U-238. M.L.= most likely. R=[U-235]/[U-238], b.a. =
better accuracy desired, k.a = known accurately. The abundance of
U-235 in depleted uranium = DU*0.002 microgram or 2*DU nanograms
where the amount of DU is in micrograms. If U-235 is greater than
2.015*DU nano gram, it represents a mixture of DU and NU. Fraction
of DU ~ (0.00725 - R)/(0.00725 - 0.2015).
----------------------------------------------------------------3.3. The concentration of U-235 given in Table II can be evaluated
from the amount given in Table 1, in microgram in a certain volume,
V, of urine specimen in litre = U-235(N)/(137.8*V), where U(N) is
expressed as if U-235 content is present in natural uranium. Our
report was sent to Mr. Shaun Rusling, Chairman, The National Gulf
War Veterans and Families Association, 4 Maspin Close, Kingswood,
Hull, HU7 3EF, U.K. We were advised that the report was forwarded
to the U.K. Ministry of Defence.
3.4. The isotopic abundance in atom percent for uranium isotopes in
DU that was deployed in the Gulf War I and in NU are given below
(14,15):U-234
U-235
U-236
U-238
Depleted Uranium
0.0008
0.2015
0.0030
99.7947
Natural Uranium
0.0055
0.720
0.00
99.2745
Commercially
0.00083
0.2219
0.0000102 99.635
available Uranium*- 0.00224
0.3468
0.02148
99.788
*Ref.[15]. Range of abundance in commercially available compounds.
Based on the above data one can deduce the fraction of DU in a
mixture of DU and NU in a specimen by determining R = [U-235]/[U238]. DU is a generic term. It has no fixed isotopic abundance. The
isotopic abundance of U-235 has to be less than 0.725. It is
essential to have the abundance data of DU deployed.
3.5. Let fraction of uranium be X, in total uranium, T, that is DU,
then
X/T = (n5 - n8R)/[(d8 - n8)R + n5 - d5],
where n5 and n8 = 0.0072 and 0.992745 are the respective abundance
of U-235 and U-238 in natural uranium,(see above),
d5 and d8 are the respective abundance of U-235 and U-238 in the DU
fraction, and R = the ratio of U-235/U-238 in the mixture of DU and
NU present in a specimen. With the assumption n8 and d8 are almost
equal to 1, the expression for the DU fraction, X/T = (0.00725 R)/(0.00725 - 0.002015).
TABLE III.
DU and NU Fractions for R values in specimens
R = [U-235]/[U-238]
DU Fraction, X/T
0.002015
100 per cent
NU Fraction = 1-X/T
0.0 per cent
0.003
81.18
18.82
0.004
62.08
37.92
0.005
42.98
57.02
0.006
23.88
76.12
0.007
4.3
95.7
0.00725
0.0
0.0
3.6. According to Dang et al., the average daily excretion rate in
the general population may vary from 3 to 300 nanograms of NU per
day [11]. This is a small amount compared to the daily excretion
rate of 1 to 5 micrograms of DU per day by the GWI veterans. It is
expected that ingestion of DU through intake of DU compounds from
the environment would result in the presence of both DU and NU with
R of the mixture between 0.00725 and R (<0.00725) of the DU
compounds.
3.7. It should also be noted from table II that the uranium content
in some specimens was found to be below the detection limits and
therefore it has not been possible to evaluate the depleted uranium
fraction in such specimens. However, the DNC and INAA methods can
provide results with lower limits of detection and better accuracy
by either increasing the volume of urine specimen for irradiation
and/or by carrying out repeated irradiation of each specimen at
weekly intervals. Dang et al., [11] have suggested that the
detection limit of U-238 by the INAA method can be reduced to 20
parts per billion (ppb) by introducing pre-irradiation and post
irradiation steps. Uranium can be removed from a urine sample with
calcium phosphate and then irradiated with neutron flux of 10^[13]
per second for one day. Np-239, thus produced from the irradiation
of U-238, can be separated from irradiated calcium phosphate by an
anion exchange resin. Np-239 can then be assayed by gamma-ray
spectrometry, using a high-resolution germanium detector.
3.8. A more sensitive method was desired for evaluating depleted
uranium content from total uranium determined by the analytical
methods. We decided to determine the [U-235]/[U-238] ratio by using
surface or thermal ionisation mass spectrometry. We are indebted to
Dr. Patricia Horan, who was at the Memorial University in the year
1999, in St.John's, Newfoundland for undertaking the determination
of isotopic abundance of U-234, U-235, U-236 and U-238 in 25 urine
specimens from the Gulf War veterans. The first batch of the
specimens sent to her, were found to contain too much of organics.
An aliquot of one of the specimens apparently exploded on a rhenium
filament inside the mass spectrometer. A second batch of 25
specimens was then prepared using the same glassware that had been
treated with nitric acid and hydrogen peroxide. Prior to this,
uranium was leached from the glassware with 1-M phosphoric acid
according to a procedure suggested by Medley et al [12]. It can be
seen from Table III that Dr. Horan determined the ratios [U235]/[U-238] and [U-236]/[U-238] among other ratios for uranium
isotopes in 18 specimens. She also determined total uranium in 11
specimens.
3.9. Dr. P.Horan's Report “Uranium Analysis, Urine Samples from
Gulf War Veterans”, is available with us for any one to peruse. Of
course specimens with codes were sent to her for analysis and no
names were given. In her e-mail to me she stated that she did not
wish to take any responsibility for the results quoted in her
report. Even the volume of urine or the nationality of the veterans
was not known to her. According to us she was within her rights to
do so. The specimens were treated with nitric acid and hydrogen
peroxide by us in our laboratories. I believe that the experimental
measurements associated with the determination of isotopic
abundance were performed in a professional way. I have also since
re-tested both reagents and water as blanks, for uranium content by
using an inductively-coupled plasma mass spectrometer (ICP-MS).
Mrs. Pamela Collins at the McMaster University conducted
experimental work associated with ICP-MS at arm's length with
little knowledge where the specimens originated from. Mrs. Collins
determined isotopic abundance, following a procedure suggested by
Ejnik et al.,(16) in more than 300 synthetic urine and human urine
specimens by using an ICP-MS Elan 6100. Dr. G. Spier also tried to
measure the abundance of uranium isotopes by using an ICP-MS with
little success. He also utilized specific anion exchange resin for
separating uranium from the specimens that were treated with conc.
nitric acid and hydrogen peroxide; and then followed by elution of
uranium from the resin. Unfortunately, we could not attain
reproducibility or the desired accuracy. We, therefore, after
analysing a large number of specimens, abandoned the use of ICP-MS
for determining R in urine specimens.
3.10. There is only one complete result from the UK veterans'
specimens and another one from Canadian veterans among eleven
complete results reported by Dr. Horan. The abundance of uranium
isotopes were determined in eighteen specimens and total uranium
content was determined by her in eleven specimens. Other results
pertain to veterans from other countries and Iraqi civilians.
3.11. We endeavoured to measure the DU content by four
methodologies but we have only two results where we can compare
them. It can, however, be seen that DU is present in microgram
quantities in urine specimens from the GWI veterans who were in the
battlefield area.
3.12. It is interesting to note that we were not aware of the
presence of U-236 in DU in 1999 when most of the urine specimens
were received. However, L. Dietz, now a retired senior scientist
from the Knoll Laboratory in Schenectady, NY, USA and who worked
for many years there with DU, provided the isotopic analysis of DU
that was deployed in Gulf War I (14).
3.13. Uranium hexafluoride also had a mixture of uranium from spent
fuel that had the man-made isotope of uranium, U-236 and NU
depleted in U-235. In an operating nuclear reactor, U-236 is formed
by the U-235(n,gamma)U-236 reaction apart from the U-235(n,fission)
reaction.
Uranium, separated and purified by removing fission
products and trans-uranic elements from the spent fuel elements
that had unreacted U-235, was converted to uranium hexafluoride for
enrichment in U-235. In the diffusion plants, most likely, U-236
hexafluoride would be expected in both streams, i.e., EU stream and
the DU one. However, the presence of U-236 PROVIDES US A KEY RESULT
FOR IDENTIFYING THE SOURCE of DU and another method for determining
DU in a specimen. The ratio, [U-236]/[U-238], was found to be
within the range expected from a mixture of DU and NU. Presence of
MASS PEAK AT 236 DOES CONFIRM THE PRESENCE OF DU IN THE URINE
SPECIMENS. CARE MUST BE EXERCISED THAT PEAK AT MASS NUMBER 236 IS
FROM ONE OF THE ISOTOPES OF URANIUM AND NOT FROM ANY OTHER
CONTAMINANTS. The half life of U-236 is 2.34E[07] years and it
decays with the emission of alpha particles of about 4.57 MeV.
Consequently, its radiological toxicity can be compared with that
of U-234 present in NU and to some extent in DU in terms of the
alpha-particle energies and the half life. U-236 is less toxic by
two orders of magnitude when compared to U-234 found in NU.
3.14. Pure NU has no U-236 in it but both EU and DU streams have U236. The abundance of U-236 is found to be as much as 30 parts per
million (0.000030) in DU-munitions [14]. Measurement of U-236 in a
mixture of NU and DU can be very helpful in determining the
fraction of DU in a mixture of NU and DU. However, one needs a
dedicated mass spectrometer for the determination of isotopic
abundance of uranium in the specimens.
3.15. The DU content can also be determined by alpha-particle
spectroscopy. We are, at present looking into the feasibility of
using a low-background liquid scintillation spectrometer. Monoenergetic alpha particles of 4.19 MeV energy from U-238 and of 4.78
MeV energy from U-234 can be identified in the spectrum. The peaks
of the two groups of alpha particles from NU have equal heights
whereas peak from the 4.19 MeV alpha particles is seven times
higher than that from U-234 in DU deployed in GWI.
3.16. Results on the determination of DU fraction by TIMS or SIMS
and by the DNC and INAA methods agree within the error limits. It
is apparent that the exposed population whether it be veterans or
civilians were found to be excreting DU through urine in
microgram(micg) quantities as shown in table IV.
TABLE IV
ISOTOPIC RATIOS OF URANIUM ISOTOPES IN URINE SPECIMENS (SIMS).
Ser. No.
& (code)
[U-235]/
[U-238]
[U-236]
/[U-238]
DU
fraction
DU(micg/L)
content
Remarks
1.(IraqV)^
0.005327
0.000149
0.366
1.3418
Exp.
NA.
2.(IraqV)^
0.007022
0.000093
0.0434
Low 0.081
Ditto
3.(Ir.CBr)@
0.006421
0.000043
0.158
0.1468
Ditto
4.(Ir.CBr)@
0.007781
0.000067
None
None
same as
5.(Ir.CBr)@
0.006750
0.000030
0.0952
0.4155
6.(B.V.)#
0.004323
0.000063
0.5575
0.7348
7.(C.V.)$
0.004366
0.000058
0.5493
N.A.
8.(C.V.)$
0.004981
0.000123
0.4322
0.5941
9.(Ir.CD)*
0.006204
0.000042
0.1992
10.(Ir.CD)*
0.007586
0.000028
ML NU
11.(Ir.CD)*
0.007171
0.000021
NU
12.(Ir.CD)*
0.003889
0.000022
0.6402
13.(Ir.CD)
0.007106
0.000026
NU
Negl.
14.(US)
0.006453
0.000081
0.1518
0.2517
15.(US)
0.004351
0.000130
0.5522
0.9244
16.(US)
0.005222
0.000092
0.3863
0.8441
17.(US)
0.002837
0.000042
0.8406
18.(US)
0.004136
0.000072
0.5931
See
para
code:- (Ir.V)^Iraqi GWI veteran., (Ir.CD)* civilian from Baghdad.,
(Ir.CBr)@
Civilian from Basra., (B.V.) British veteran.,(US)
Veteran from the USA. Exposure data not available for Iraqi
veterans and civilians.
------------------------------------------------------------------
3.17. It can be seen that the U-235 content can be determined by
the DNC method by irradiation with neutrons at the McMaster
University Swimming pool Reactor, with the help of the computercontrolled facilities, repeatedly to attain better accuracy. The
detection limit for U-235 is 145 picograms. Total uranium that is
almost equal to the U-238 content, can also be determined by
fluorometry as well. These two methods can provide sufficient
information for the evaluation of DU in human specimens as well as
in environmental specimens like soil, water and air. It will be
shown that DU oxide could accumulate in the lungs of civilians.
Presence of DU has been confirmed in the civilian population that
resided in Basra during the 1991-4 period. IT SHOULD BE NOTED THAT
THE MILITARY PERSONNEL FROM ALL COUNTRIES THAT TOOK PART IN GULF
WAR II AND THE IRAQI CIVILIANS SHOULD NOT HAVE BEEN HARMED BY THE
DEPLOYMENT OF DU-MUNITIONS DURING AND AFTER THE CESSATION OF THE
HOSTILITIES. IT IS; THEREFORE, INCUMBENT ON THE INVADING FORCES TO
DEMONSTRATE THAT THE DICTATES OF THE GENEVA CONVENTIONS HAVE NOT
BEEN VIOLATED.
4. PARAMETERS FOR THE EVALUATION OF RADIATION DOSE FROM INGESTED
DU.
4.1. In the Royal Society Report, "The Health Hazards of Depleted
uranium Munitions Part 1", the radiation dose has been estimated
based on different scenarios applicable to deployment of DUmunitions during the GWI [17]. It has not been possible to answer
in the negative, under all scenarios, that the radiological hazard
to the veterans and to the civilians after the cessation of
hostilities is minimal. It is concluded in the report that based on
'their' estimates of intakes of DU, except in extreme circumstances
any extra risk of developing fatal cancers as a result of radiation
from internal exposure to DU arising from battlefield conditions
are likely to be small compared to general risk of dying from
cancer over a normal life. Overall conclusions that are drawn in
the report, amount to very low hazard from ingestion of DU to
veterans exposed to DU-oxides dust in the battlefield area. The
greatest exposures will apply to a small fraction of soldiers
during the conflict, for example, those who survive in vehicles
struck by a DU penetrator. The life time risk of death from lung
cancer is unlikely to exceed twice that in general population. This
statement appears to be in contradiction to the test data compiled
by the US Department of Defense (DoD) [18]. Under the above
conditions, it is stated that DU will present radiological hazard
from DU-oxides inhaled within fifteen minutes. Our own report, we
believe, by very conservative risk estimates derived from
analytical data of urine specimens from GWI veterans, give much
higher fraction of soldiers exposed to DUOA-contaminated air, and
will be or are suffering from radiation related illnesses.
4.2. Many reports evaluate risk factors from dispersal scenarios of
DU rather than from quantification of exposure from causative
agents. Thus, it is not possible to examine the "cause and effect"
by properly designed epidemiological studies. The Royal Society
report does recommend better quantification of DU and its oxides as
aerosols. Some of the recommended studies may never be performed
such as long-term in vivo studies of the dissolution of DU oxides.
There is an urgent need to gather test data to determine the
concentration of DUOA in air and soil after the end of the recent
conflict.
4.3. There is a general agreement that DU on impact with an armour
plate catches fire to form its oxides. As long as there is
sufficient oxygen to support combustion, it keeps burning with the
evolution of enormous amount of heat. The bullet pierces the armour
and keeps producing finely divided DU-oxide dust. The dust
disperses as aerosols in air. The particle size of the dust is in
the micron and sub-micron ranges. Inhalation of the aerosols leads
to deposition of the oxides in the lungs. It is appropriate to test
whether indeed a veteran present in the battle field area would
have been exposed to DU deployed in Gulf War I during the 1990-1
period.
4.4. The Rand report is a compilation of work that relates to the
health effects in uranium miners [19]. It is now important to find
better ways of estimating uranium in workers. Estimating the extent
of contamination of workers by urine analysis and having a very
high level for investigational purposes are only good for D class
of uranium compounds. Conclusions based on the past experiences
with miners, appear to be that the radiation hazard to soldiers who
took part in GWI was minimal. The soldiers were also exposed to
highly insoluble uranium compound, namely, uranium-dioxide dust.
4.5. Our literature survey indicated that there were three other
papers that were not included in the above reports. The findings in
those papers provided data in support for our proposed scenario
wherein the DU bullet strike a hard surface and catches fire and
burns into fine oxide dust. More than 50 per cent of the dust forms
aerosols. DU oxides appear to be present in air for a period of
almost three years [20]. Soil samples were taken from 12 sites for
determining the isotopic compositions and total uranium. Three
sites were located in Kuwait city and Jahra, three on the beach and
the rest were from the desert including four sites chosen in the
Gulf war battlefield. We summarise the result of analysis of
samples collected in each location in Table 5. An Interim summary
on the state of the environment summarises total uranium and
isotope uranium results in 22 soil samples in Kuwait for operation
southern watch 1998 [21]. 21 samples showed the presence of NU in
the range of 0.26 to 1.34 microgram per gram of soil and one sample
showed 33 microgram of almost pure DU with R= 0.00216.
Table 5.
Uranium content in soil samples (ref.20 and Appendix IV)*
----------------------------------------------------------------Collection Sample Nos.
Uranium Conc. U-235/U-238 DU content
Location
in
refers to Average
Table 1
micrograms/g
Ratio, R
Remarks
of the paper
of soil
---------------------------------------------------------Kuwait City
5, 7 & 8
0.54^+/-0.15
0.007
Most likely
and Jahra
all NU
Beach area
Battlefield
area
1 & 3
0.48^+/-0.08
0.006(2)
4
1.55 +/-0.29
0.007(1)
0.35^+/-0.12
0.006
9,10 & 12
0.38 +/-0.12*
11
1.85 +/-0.68
* weighted average. ^ Arithmetic average.
DU fraction
0.24
Most likely
NU
DU fraction
0.24
0.006
0.006
4.6.
According to our scenario, any one, either a veteran or a civilian,
who happened to be present in the battlefield area or in its
vicinity during the 1991 to 1993 period, would have ingested DUoxide aerosols (DUOA) through inhalation. The DU aerosols are known
to travel long distances in air. Dietz (private communication)
found the presence of DU some 40 kilometers away from the
laboratory [14]. This is a very important point that has been
ignored. Contamination of air with DUOA can spread over a much
wider area depending on meteorological conditions during the
period. Recently, UNEP found DU in air in two areas in the Balkans
(Pijackovica and Cape Arza), where DU munitions were presumably
used. Air sampling at the two sites, conducted more than two years
later, revealed the presence of DU [22]. However, other sites only
showed the presence of NU. This shows that under some conditions DU
contamination can be present for a long period.
4.7. The Battelle Northwest Pacific Laboratories report DE8500978,
PNL-5415,"Potential Behaviour of Depleted Uranium Penetrators under
Shipping and Bulk Storage Conditions" compiled by J.Nissima, M.A.
Parkhurst, R.I. Sherpelz and D.E. Hadlock, March 1985 compiled for
DoD, stated that the DU-based munitions upon ignition, burn almost
to one hundred per cent ceramic form of oxides[23]. The
solubilization rate data of the ceramic oxides, in simulated lung
fluid given in the Bettelle report, was replotted by L. Dietz. He
found that the rate of solubilization can be represented by the
solubilization half life of 3.852+/-0.075 years or 1407+/-27 days.
This is a very significant result in the sense that it permits the
evaluation of the radiological toxicity of DU. This will be
apparent later.
4.8. A Canadian report IAEA-SM-276/5, entitled "Canadian Uranium
Fuel (Uranium dioxide) Fabrication Study:I Intake, Retention and
Excretion Monitoring Results, II Comparison of Results with
Metabolic Models", by M.R. Avadhanula et al., from the Atomic
Energy Control Board, the Atomic Energy of Canada Ltd., and the
Radiation Protection Division of Health and Welfare of Canada [23],
indicated that the clearance rate of uranium dioxide can be
represented by two short components (half lives 3 and 280 days) and
two long components (half lives 800 and 3500 days) [24]. Since the
excretion rate was monitored 8-11 years after the alleged exposure
to the DU-oxides aerosol (DUOA), the aerosols with short biological
half lives (3 or 280 or 800 days) must have been excreted from the
body by now. We adopt the biological half life for the DU-oxide
dust component present in the body eight years after the exposure,
as low as the solubilization half life (3.852 years) or the longest
as (3500 days). We present the evaluation of the radiation dose
using the above two long components only.
5. INGESTION OF DU AS DUOA THROUGH INHALATION DURING GULF WAR I AND
ITS SUBSEQUENT EXCRETION FROM THE BODY.
5.1. We have considered the ingestion of DUOA through inhalation
only during GWI. It is now well known that a total of 320 metric
tons of DU was deployed during GWI. Twenty six per cent of the DUmunitions (0.26*320 = 83.2 tons) found their targets and probably
seventy four per cent are probably lying in the desert sand as DU
metal attached to un-exploded munitions. It has been reported that
DU upon hitting its hard target burns to its oxides releasing
enormous amount of heat; thereby forming at least 50 per cent of DU
oxides in the inhalational particle size range (micron or sub
micron size). The finely divided DU-oxide dust attaches itself to
aerosols or forms aerosols which we refer to as depleted uranium
oxides aerosols (DUOA). We assume that DUOA was present in air in
the battlefield area over a period of two to three years. BouRaabi's results [see table IV in the paper [15] on air monitoring
indicate that air was contaminated with 0.34 nanogram/m3 (/m3=per
cubic meter of air) with R = 0.005, during the months of July and
in August 1993,R increased to 0.006. The DU fraction during July
1993 was evaluated as 0.43 and the NU = 0.57. During the months of
December 1993 and January 1994, the R was 0.007 with DU fraction as
less than 0.05. It is assumed that the concentration of the DU
contaminant in air, decreased slowly with time (from 146 nanograms
per cubic meter during the month of February 1991 to ~7 nanograms
per
cubic
meter,
in
January
1994).
5.2. It is appropriate to evaluate DU content in soil in the battle
field area of about 2400 square kilometres from data reported by
Bou-Raabi [20]. Four samples of top soil were taken for analysis
over the area, each of 100 square centimetre (cm2) and three cm.
depth. The density of sand is assumed to be 1.43 grams/cm3. Sample
No. 9, 10 and 12 conform to the above specifications but sample No.
11 differs. The weighted average of the amount of uranium content
was found to be 0.38 microgram per gram of sand. R value was
constant in all the four samples as 0.006. The DU fraction is 0.24
in the samples. The total amount of DU in the 300 cubic cm. is
found to be 0.38*300*1.43*0.24 = 39 micrograms. It can be seen that
the total fall-out over 2400sq.km =
2400*1000meters/km*1000meter/km*100cm/meter*100cm/meter = 2.4E[13].
The total amount of DU in the battle field area = 2.4 E[13]*39E[6]/100sq.cm = 9,360,000 grams or 9.36 metric tons. The uniformity
of the concentration of DU in soil makes us believe that the fallout of DU occurred as DUOA from air to soil took place slowly. In
other words, the concentration of DUOA during the 1990-1 period was
the highest and with gradual fall-out it reduced to a negligible
value in the winter of 1993-4. There may have been lateral
dispersion and some DU contaminated soil may be there below 3
centimetre depth. The initial amount of DU in air as DUOA was
considerably higher than the calculated value of 9.36 tons perhaps
two or three or four times this value. Re-suspension of DUOA from
soil with R=0.006 cannot lead to contamination of air with DUOA
with R = 0.006.
5.3. From the Depleted Uranium Case Narrative reports [18], about
41 mtons of DU oxides (ceramic type) might have formed and about 20
mtons formed DUOA that mixed with air over the battlefield area of
2400 sq.km. uniformly over 500 meter from the ground level, leading
to contamination of air with DUOA over the entire volume of air.
From anecdotal accounts, we understood that soot from oil fires
formed a blanket over the battlefield area. With these assumptions
we can evaluate the concentration of DU in air =
20mtons*1E[12]micrograms/mton/(2400sq.km.*1000m/km*1000m/km*500m) =
17 micrograms/cubic meter.
5.4. A person on active duty inhales 33 cubic meters of air per
day. It can be seen a person can accumulate 0.5 milligrams of DUOA
per day in his/her lungs. It can also be seen that over 90-day
period IT IS FEASIBLE FOR A PERSON TO ACCUMULATE OVER 20 MILLIGRAMS
OF DUOA IN THE ALVEOLAR TISSUES IN THE LUNGS. IF THE ABOVE
ASSUMPTIONS NEED TO BE VERIFIED, ONE CAN DESIGN A TEST PROTOCOL TO
JUSTIFY IT BASED ON ANALYTICAL DATA WHETHER DU-BASED MUNITIONS MEET
THE GENEVA CONVENTIONS OR NOT TO DEPLOY IT. TUNGSTEN HAS BEEN
SUGGESTED AS A GOOD SUBSTITUTE. THERE IS STRONG CASE FOR CONDUCTING
IN-DEPTH INVESTIGATIONS AT THE PRESENT TIME. IT IS OUR VIEW THAT IF
THE COALITION (US AND UK) INVADING FORCES DID DEPLOY ONE OR TWO
THOUSAND TONS OF DU DURING GWII, THERE ARE GOING TO BE A VERY LARGE
NUMBER OF DELAYED CASUALTIES. THE HEADS OF NATO COUNTRIES WERE
WARNED BY US VIDE MY LETTER DATED JULY ??, 1999 (SEE APPENDIX V)
AND WE INCLUDE A REPLY RECEIVED FROM MR. MARK NEWMAN OF UK MINISTRY
OF DEFENSE. WE HAVE VERIFIED OUR RESULTS ON DU CONTENT IN URINE
SPECIMENS FROM GWI VETERANS FROM FOUR COUNTRIES BY FOLLOWING TWO
METHODOLOGIES. DU IN URINE WITH ITS SIGNATURE MUST ORIGINATE FROM
VETERANS' BODY. 97 PER CENT OF ENVIRONMENTAL SPECIMENS CONTAIN
NATURAL URANIUM AS REPORTED BY GOLDSTEIN, RODRIGUEZ AND LUZAN [7].
WE HAVE LOOKED FOR SOURCES OF DU CONTAMINATIONS BUT WE HAVE FAILED
TO FIND ITS ENTRY INTO THE SPECIMENS DURING WET COMBUSTION OR
OXIDATION BY NITRIC ACID AND HYDROGEN PEROXIDE (SEE APPENDIX III).
BLANKS OF ALL MATERIALS THAT HAVE BEEN USED FOR CONVERTING
SPECIMENS INTO SOLUTION FOR ANALYSES DID NOT SHOW THE PRESENCE OF
DU. IT IS EVIDENT THAT THE CIVILIAN POPULATION IN IRAQ AND THE
VETERANS ARE AWAITING AN EPIDEMIC OF CANCERS. THE PRESENCE OF DU IN
LYMPH NODES WITH ABOUT TEN TIMES THE CONCENTRATION PRESENT IN LUNGS
DOES AFFECT THE IMMUNE SYSTEM. THAT MAY TURN OUT TO BE A BIGGER
CATASTROPHE. FOR THE SAKE OF THE ENTIRE POPULATION OF IRAQ AND THE
MEMBERS OF THE INVADING FORCES, IT IS OUR SINCERE HOPE THAT THE
ABOVE IS NOT TRUE. WE DREAD THE AFTER EFFECTS OF THE WAR. WE SHOULD
DEVOTE ALL EFFORTS TO MITIGATE THE EFFECTS OF THE PRESENCE OF DUOXIDE DUST.
5.5. Our analytical data on urine specimens from GWI veterans
indicated that the clearance rate of DU was between one to five
micrograms per day. More precise analytical data on DU content in
urine specimens can be obtained by applying a little more care and
pre-concentration and post-irradiation radiochemical separation
steps. We now attempt to calculate the radiation dose based on this
proposed scenario. Following the ICRP model and assuming the
biological half life for the contaminant is the same as the
solubilization half life of 1407 days, we shall evaluate the amount
of DU inhaled by a veteran during his active duty during the 1990-1
period, in the next chapter.
6. EVALUATION OF RADIATION DOSE FROM INHALATIONAL DUOA.
6.1. The clearance rate, R, of DU in microgram through urine, per
day is determined as a function of time over a few years. A is the
total amount of inhalational DU and k = 0.693/biological half life
or = 0.693/1407days = 0.000492 day-1 or equal to 0.63/solubilizing
half life. A plot to logR vs. time can be resolved in terms of
components i, as Ai with each Ri with its respective biological half
life [8,25].
or R = R1 + R2 + -- + Ri = k1A1 + k2A2
--The clearance rate of DU per day was determined by estimating DU
content in 24-hour urine specimens received from some DU-exposed
veterans during the 1998-9 period or about 8 years after exposure
to DU-oxide dust. There was cessation of work for a year or two
till alternate facilities were organised. We had hoped to confirm
our earlier analytical data as well as augment with other data on
fresh urine specimens collected from the exposed veterans on an
annual basis. These additional measurements would have provided a
fairly good estimate of the biological half life or lives for one
or many components. If it is assumed that DUOA can only be removed
from the lungs by solubilization, the excretion rate is then
inversely proportional to the amount of DUOA in the lungs. The
initial excretion rate at t=0 (at the time of exposure) is given by
Ro = Rexp[kt]
where Ro = the clearance rate at the time of exposure to DU during
the 1990-1 period for the component that had a biological half life
as the solubilization half life of ceramic DU oxides in simulated
lung fluid,
t = time elapsed between the exposure and measurement of R.
For example, at t = 8.5 years (during the 1998-9 period)
Ro = 4.614 micrograms and
Ao = 1.4*1407days*4.614 micrograms
= 9.1 milligrams for R = 1 microgram per day determined
during the 1998-9 period.
6.2. It can now be seen that the value of excretion rate of 1 to 5
microgram per day in 1998-9 period is compatible with the amount of
formation of DUOA and its concentration as a contaminant in air
over the battle field area during the Gulf conflict that lasted
about 90 days. Two sets of data namely the excretion rate through
urine and the amount of inhalational DUOA gave almost the same
value despite many reasonable approximations that include the
biological half life same as solubilization half life as deduced
from the data presented in the Bettelle report[23]. Some of the
approximation can now be confirmed by determining the DU content in
the environment in the aftermath of the present conflict in Iraq.
6.3. According to ICRP model, the radiation dose in Gray (Gy) can
be quantified by the total energy in joule deposited by a radiation
source in one kilogram of tissues in an organ [26]. Weighting
factors for the type of radiation and for tissues lead to the
evaluation of radiation dose in Sievert (Sv). The rate of emission
of alpha particles of 4.19-MeV energy from U-238 plus the rate of
emission of alpha particles of 4.78-MeV energy from U-234 can be
evaluated by the following equation[2]:dN/dt = Number of alpha particles emitted per minute =
Number of U-238 nuclei*0.693/half life in minutes of U-238 = weight
of U-238 in grams*Avogadro's number/atomic weight of U-238
(6.02E[23])*0.693/4.46E[09]years*5.2596E[05]min./yr.
If 10 milligrams of U-238 are present in the lungs (total weight of
the lungs = 1 kg), the rate of deposition of radiation energy in
the lungs from 10 mg of DU = (7472*4.19 + 1200*4.78)*1.602E[13]J/Mev = 5.935E[-09] joule/min or = 0.0044 J/yr.
Total amount of dose deposited over a period of 50 years =
1.4*1407days/365.25days/yr*0.0044 J/kg = 0.0238 Gy.
Quality factor of alpha particles = 20
Radiation dose deposited = 0.476 Sv . or 47.6 REMS over the entire
life. This is the organ dose and it should be multiplied with
tissue weighting factor of 0.12.
6.4. There are other factors that have not been taken into
considerations for evaluating radiation dose and attending
predicted risk factors in terms of probability of dying from fatal
cancer. The progeny (daughter and the grand daughter), Th-234 and
Pa-234, of U-238 are present in secular equilibrium with the parent
U-238. We have not included the energy dissipated by beta
(electron) particles from the progeny of U-238 in the lungs. It is
suggested that particulate matter, highly insoluble radioisotope
such as uranium dioxide may be localized in a tissue rather than
the entire lungs. According to UNSCEAR report (1972)[25], the
tissue dose may result in oncogenesis near the imbedded particulate
radioisotope. Following the ICRP model one can evaluate the
radiation dose from a picocurie of (2.22 alpha particles per
minute) alpha particles from 2.6 micrograms of DU as shown below.
The range of 4.19-MeV and 4.78-MeV alpha particles does not exceed
1 gram of tissues.
Radiation dose per year = 2.22*5.2596E[05]min./year*4.308MeV*
1.602E[-6]erg/MeV/100ergs/RAD = 8.058 RADS/year or = 161 REMS/year
(Quality Factor = 20 for alpha particles). It is our view that the
biological half life can range from 4 to 10 years for a highly
insoluble compound of uranium. This, of course, is the worst-case
scenario if we take the biological half life of 10 years.
Integration of dose over fifty years, the tissue dose can range
from 900 REMS to 2100 REMS. For lungs, the weighting factor is
adopted as 0.12. Radiation biology is in its infancy. Care must be
exercised so that exposure to radiation does not harm the general
population. Lastly, there are suggestions that the ICRP model is
not adequate to evaluate risk estimates for low-level chronic
exposure to ingested radioisotopes like DUOA [27]. Inhalation of
DUOA in the lungs represents a low-level source of radiation source
for which ECRR [28] has suggested modification of the ICRP model.
According to ECRR, the risk estimates are enhanced in the region of
0.01 Sv. to 0.1 Sv over the risk estimates predicted by the linear
or the threshold hypothesis.
6.5. Expectant mothers contaminated with DUOA also provide a source
of DUOA to the unborn child at the fetal stage. There is evidence
to indicate that fetus is harmed by exposure to very low level of
radiation. In this regard one can quote the evidence presented by
Alice Stewart [29.30]. Children born to expectant mothers that had
diagnostic x-ray exposures during pregnancy,were more likely to
suffer from childhood leukaemia than those who did not. Her work
led to revision of exposure levels to radiation in the work place
for expectant mothers. It has been shown that trans-uranic
radioisotopes can be transferred to fetus through the placenta
[31]. There have been many reports in the media that there has been
enhancement of birth defects among children born to mothers
residing in Basra. No direct evidence has been sought so far for
transfer of DU to the fetus and thus causing damage to the fetus.
6.6. A scenario that DU on impact with hard target burns briskly
with the evolution of finely divided dust that forms aerosols
(DUOA) that results in DU becoming a contaminant in air, has been
proposed. Inhalation of DUOA results in the accumulation of DUOA in
the alveolar tissues in the lungs. The long biological half life
explains the inhalation of DU oxides as DUOA, can lead to
deposition of sufficient radiation insult in the body.
6.7. Thus, it can be seen that the risk factors can be as low as
0.5 per cent or as high as 80 per cent because DUOA is particulate
matter that can be imbedded in tissue for a long period. Tissue
dose reaches the level that can result in oncogenesis. One needs to
keep a careful watch of morbidity data particularly of residents of
Basra and now Baghdad and other inhabited areas near the battle
field zone.
6.8. For testing the validity of our calculations, we decided to
get tissues of various organs from deceased persons who resided in
Basra from 1990 to 1994. We received tissues taken from 40 deceased
persons. Their age ranged from 12 to 45 years, through some medical
practitioners in Basra. The tissues, preserved in formalin, were
received through a courier service. The results are summarized in
brief, below. The tissues were received by us in five packages
containing numerous types of tissues from the deceased persons
although we requested to have tissues from lymph nodes, lungs,
kidneys and liver etc. We had considerable difficulty in
identifying each one of them.
Table No. VI
Specimen
DNC method
INAA
ICP-MS
Fraction
Average of four
Ave of 4
Ave
DU* DU^
U = U-235/0.00725
U-238 U-235 R from
_________________
_________
_____
_____
DNC &
parts per million
% abundances INAA
______________________
____________ __________
IIA
0.02
0.04
99.26 0.72
0.68 0.72
IVA
<0.02
0.03
99.25 0.71 >0.46 0.71
VIIIA
<0.05
0.11
99.24 0.72 >0.75 0.83
XA
0.05
0.07
99.26 0.71
0.39 0.75
XIIA
<0.02
0.04
99.21 0.74 >0.68 0.88
XIV
<0.02
0.05
99.24 0.71 >0.83 0.85
XVI
0.02
0.03
99.24 0.75
0.46 0.88
XIX
<0.02
0.05
99.24 0.73 >0.83 0.73
XXII
0.02
0.06
99.25 0.76
0.92 0.81
_________________________________________________________________
*Fraction of DU = (0.00725 - R)/(0.00725 - 0.00205).
^Total uranium determined by the INAA method - U-238 from NU as
determined in the dissolved uranium from tissues by the ICP-MS =
Amount of DU in the tissues. DU fraction = Amount of DU in the
tissue/the total uranium. This method was improved upon by taking a
larger sample of tissues. It can be seen that the U-235 and the U238 contents in the tissues by the DNC and the INAA methods yielded
as ~90 per cent DU and 10 per cent NU in the tissues and only
natural uranium was found in the tissues by using the ICP-MS. This
is somewhat remarkable that total uranium can be determined by any
other method and NU can be estimated by the use of ICP-MS. We can
deduce from our data on uranium content in tissues from deceased
residents of Basra that there is at least 8 times the amount of
uranium in their body compared to the amount reported in the ICRP
Standard Man. Moreover, we believe the biological half life is much
longer than 500 days (ICRP suggested value for highly insoluble
uranium compounds (10).
Specimen
[U-235]
DNC(ppb)
<DL
<0.087
Table VII
[U-238]
INAA(ppb)
<DL
35+/-16*
Natural uranium(ICP-MS)
U-238
[U-235]/[U-238]
<DL
ND
4.9+/-0.03# 0.0079
A (Blank)
B (Tissue)
(kidney)
C (Tissue)
<12
<19
5.07+/-0.06 0.0069
(liver)
*Represents total uranium and R = 0.0025. # Represents NU with R =
0.0079 +/-0.0006.
6.9. Uranium content was determined by us in the early eighties in
three deceased uranium workers. Two of them worked in diffusion
plants -- one on the DU stream and the other on the EU stream. The
third person was a health physicist in a plant where enriched
uranium was handled. They all died from cancer. Their medical
records and cause of death along with uranium content in various
tissues are summarized in Table VIII. The tissues were sent by
respective Coroners from hospital settings with chain of custody,
at the behest of the respective lawyers.
Worker
Table VIII
Medical and Work history of
three uranium workers
X
Y
Year of Birth
1921
Death
1980
Cause of
Metastatic adeno
Death
carcinoma
Nature of
work
Worked as a control
operator in buildings
C310 & C315 meant for
product and tailing
withdrawl.
1927?
1984
Cancer
Z
Not Avaible
1981
Carcinoma of
the tongue
In uranium
Employed at
Enrichment
Feed Material
plant(building) Center in
1410 in the K25 Fernald, OH
facility at Oak
Ridge, TN.
End Product DU & EU
94% EU
Handling of EU
Employment
1952 - 1971
1947-1961.
1952-1981
Medical
Stomach ulcer (1954) Surgeries for
Sore tongue in
History
Gestretomy (1961)
stomach ulcers July 1980.Sore
Unusual skin compl(1968)& (1975), related to
aints.Overgrowth of
lung tumor(74) malignancy &
cartilegous tissues
bladder tumor( )subsequent
and several attacks
lung tumor (79) growth on the
of pneumonia.
neck.
Exposure to Uranium hexafluoride UF6
EU & DU
Table
VIII
Uranium Isotopic Content in Tissue Specimens
Worker X
Worker Y
Uranium IsotoU-235*
U-238
U-235* U-238
U-238+
pic content in
DNC
DNC
INAA(U-239) INAA(Np-239)
tissues
----------------------------------------------U in microgram/g or parts per million (ppm)
____________________________________
Bones I-I
Bones II-II
I-I
II-II
0.3
<0.01#
<0.02#
<0.02#
0.8
0.1
0.2
0.2
Lungs I
Lungs II
Kidneys I
kidneys II
Liver
Lymph nodes
Type of uranium:-DU,with R=0.0027
nearly the same
R as found in DU
deployed in GWI
0.036+/-0.004,
0.040+/-0.004.
<0.3
<0.2
0.027+/-0.013, <0.16; <0.22^
0.13 +/-0.018, <0.13; <0.039
0.020+/-0.006, <0.4;
0.036+/-0.005, <0.2;
0.025+/-0.006, <0.25;
0.24 +/-0.04 , <0.2 ; <0.06
EU with U in the lymph nodes
with R= 0.035. Lymph nodes
have higher U content about 2
to 10 times higher than in the
tissues and with tissues from
kidneys and liver also having
higher amounts (Table 8).
Table VIII (contd.)
Uranium Content in Tissue Specimens from Worker Z.
_________________________________________________
Specimen
Uranium content microgram/gram
Alpha activity
mBq/kg
________________
__________
_________
DNC methoda
INAA (U-238
through NU
thru. U-239
b
Bone(Sternum) 0.027+/-0.01
0.33 (0.05)#
b
Bone(neck)
0.022+/-0.01
0.27 (0.05)#
c
Kidney(wet-Ox) 0.024+/-0.01
0.29 (0.005)#
c
Kidney(F-D)
0.034+/-0.004
Blank
0.001
nil
c
Lungs(wet-Ox) 1.105+/-0.02
0.98+/-0.5
13.4 (0.015)#
Enriched
Lungs(F-D)
0.870+/-0.004c
1.09+/-0.1
Slightly
Depleted
_____________________________________________________________
aTotal uranium = U-235/0.00725.,b
c
#(alpha
activity in Standard man [31].
6.10. It can be seen from the table that worker X, whose case was
designated by the Department of Energy as the first martyr of the
atomic age. He was exposed to uranyl fluoride UO2F2 and hydrofluoric
acid produced by the hydrolysis of UF6 in presence of water, during
his duties in the diffusion plant. He had excessive amount of
uranium (0.8 microgram of DU per gram of bone) in soft bone tissues
and much lower amount in hard bone tissues (0.02 microgram per gram
of bone tissues). Nevertheless, uranium content in the skeletal
mass was nearly 3 to 100 times more than what has been reported in
the literature (Table 8). We did not receive any other body tissues
from worker x. It is unlikely that the skeletal mass contained a
maximum of 4 milligrams of depleted uranium. During the last nine
years before he died, he was not exposed to uranium compounds from
his work environment. The clearance rate of uranium in soft bones
must have a component with a very long biological halflife. There
is a great deal of inhomogeniety in the distribution of uranium in
skeletal mass. Tissue dose in soft bone may indeed be very high in
relation to total skeletal dose. This results in very high
radiation insult to some tissues and much lower insult to others.
It is difficult to assess risk estimates without complete data on
internalised uranium in various body compartments.
6.11. Worker Y worked in the product withdrawl section of the plant
where enriched uranium hexafluoride with enrichment up to 94% in U235 was collected. It appears that exposure to total uranium
hexafluoride was from a mixture of depleted and enriched uranium
hexafluorides. In his case bone tissues contained about a maximum
of four times higher amount of U-235 than in a standard man (R
could not be determined). However, total uranium in the skeletal
mass could be less than 300 microgram. Kidney tissues of the worker
had about the same uranium content (25 nanogram per gram of
tissues). Uranium with U-235 as > 3 per cent was not uniformly
distributed in the lungs. Two tissue-specimens from the lungs
showed a very wide variation (0.027 to 0.13 microgram per gram of
tissues. The lymph nodes contained the highest amount among the
tissues that were analysed. It is certain that some particulate
insoluble compounds of enriched uranium must have entered his lymph
nodes through inhalation. We estimate the total amount of uranium
to be less than a milligram of enriched uranium.
6.12. Worker Z, according to our information worked as a Health
Physicist in the plant. He had a supervisory role to ensure that no
worker handled radioactivity in a way so that the prescribed
maximum permissible limits were not exceeded. It was a puzzle to us
how worker Z could have ingested uranium in his body. Highest
concentration of uranium was found in the lungs. Measurements of
alpha activity in the tissues also indicated that there was at
least some EU inside his lungs. We believe that he must have been
engaged in duties connected with accidents associated with burning
of all types of uranium. EU, NU and DU were indeed handled in the
plant. Some comments about the analytical data are in order.
Uranium content in bone tissues and tissues from the kidneys were
slightly higher than the normal amount found in the "ICRP" standard
man. However, his lungs had about one milligram of uranium with r =
0.0072. He left the plant one year before he died from cancer
(tongue and neck). Intake of soluble type of uranium compounds
should have been flushed out during one year. Ingestion of
insoluble type of compounds through gastro-intestinal track (GIT)
should not lead to accumulation of uranium in the lungs. It appears
that particulate radioactive uranium compound might have imbedded
in his tongue for a long period. The lung tissues did show alpha
activity much higher than expected from the same amount of NU.
Additional alpha activity might have been from U-234 in EU. What
follows below is a copy of a report of examination of the alveolar
tissues in the lungs from his body exhumed nine years after his
burial."The lung tissues were sectioned and several slides of the
sections of the tissues were examined under a microscope. Three
slides were randomly selected for a detailed microscopic
examination. The slides revealed clumps (clusters) of particles of
7 to 12 micrometers (microns) in walls of tissues of the air ways
leading to alveoli lines. The size of particles in the clumps
ranged from 0.5 to 1.25 microns. In a field of view of 0.4
millimeter (mm) or 400 microns diameter, the number of clumps
ranged from 2 to 14 with an average of six clumps in field of view.
It can be surmised that there is a great deal of heterogeneity with
respect to location of clumps in the tissues of the air ways." The
particulate matter appeared to us as ceramic uranium dioxide. It is
hard to believe that any other uranium compound will fit this
description.”
6.13. It is believed that the uranium content in thoracic lymph
nodes is approximately ten times higher than it is in the lungs.
The radiation insult in the lymph nodes will be consequently ten
times the dose evaluated for the lungs. This has serious
consequences with respect to the immune system. Radiological
toxicity and indeed the entire area of assessment of risk estimates
from low-level chronic exposure from internalised radioisotopes
needs re-visiting.
6.14. The above narrative has been presented here because we feel
very apprehensive that inhalation of the highly insoluble uranium
dioxide will enhance morbidity and mortality when and where ever DU
munitions are used in conflicts. If indeed they are shown to be as
lethal as we believe they are, it is incumbent on the only super
power to show that they do not leave such a huge radiation insult
to the environment in Iraq that will linger on for years to come.
We suggest that the Super power should conduct a program similar to
the one set in motion at the end of World War II in Hiroshima and
Nagasaki in Japan. The A-bomb survivor data provided results that
are considered the back bone of safety standards for safe handling
of radioactivity for the last fifty years. The knowledge gained
after 1945 through national and international committees for
setting standards has helped in reducing morbidity and mortality of
workers in the area of ionising radiation. Having spent our meagre
resources, and lacking data concerning the deployment of DU
munitions in GWII, we can only suggest that epidemiological studies
should be conducted in a transparent manner. The detailed reports
for the three workers are given in Appendix I to illustrate the
difficulties in assessing the toxicity. We also recommend that no
radioactive munitions be deployed in conflicts.
Metabolic Data (ICRP) [Ref.10]
Standard Man
micrograms
Total Uranium (75 kg)
90
Skeletal tissues (7kg)
59
Kidneys (300 grams)
7
Average Daily Intake
1.9
See
Ref.
32
for
organ
7.
ppm*
0.0012
0.008
0.023
mass.
PROPOSED INVESTIGATIONS.
7.1. It can be concluded from the analytical data gained by the
well-tested methods, the DNC and INAA methods for the determination
of U-235 and U-238 respectively, that there was DU present in 24hour specimens of urine taken from the veterans from four
countries. Uranium oxides were found in deceased civilians who
resided in Basra during the 1990-94 period. The concentration of DU
was much higher in specimens from veterans than that taken from
civilians.
7.2. In my letter to the Heads of NATO countries, our concerns
about the deployment of DU-munitions were communicated to the
effect that the DU aerosols in large quantities may bring about a
very large number of delayed casualties to the civilian population
(see Appendix V). Indeed, DU in many ways need to be identified as
weapon of mass destruction as mentioned in one of the replies to my
letter from an Officer of the Ministry of Defence. It is indeed
surprising to find that there has been no mention of any study
concerning the determination of the biological halflife for
inhalational ceramic DU-oxides dust.
7.3. Now Gulf War II is over. It is essential to start as soon as
possible, without further delay to determine the concentration of
DU in air and in soil in areas (including cities in Iraq) where
ever DU has been deployed. It is alleged that as much as 1000 to
2000 mtons of DU might have been deployed during the GWII. In fact,
we feel that there are conjectures about the amount of DU deployed
during the second Gulf conflict that range from 25 mtons to 2000
mtons. If the Coalition forces did use 2000 mtons of DU during the
second conflict, a major catastrophe is in store for the Iraqi
people.
7.4. For the sake of humanity and for determining the suitability
of deployment of DU in future conflicts, a concerted effort must be
made to assess the radiological and chemical toxicities from using
such huge amounts of DU. We present in the last table, equivalences
in terms of total alpha activity from 2000 mtons of DU and energy
of alpha particles deposited in the unit mass of tissues, for wellknown radioisotopes like Radium-226, Plutonium-239. It can be seen
that presence of DU-oxides aerosols certainly does not meet even
the spirit of the Geneva conventions. If 500 mtons of DU-aerosols
survive for over two years in air as contaminants as they did in
Kuwait, the use of DU-munitions must be classified as weapon of
mass destruction. Is this proof enough that your own invading
soldiers are suffering from mysterious illnesses?
Has anyone
considered the fate of Iraqi population if 2000 mtons of DU in the
DU-munitions have been deployed? This work must be commenced at
the earliest after it has been ascertained the amount of DU used
and the success rate in hitting its targets. A rough material
balance must show that the amount deposited through fall-out on the
soil plus the amount present in air is roughly equal to the amount
of DU-based munitions that found their targets. If no DU is found
in air and if there is no deposition of DU through fall-out on the
soil, it may not be necessary to conduct any further analyses. 24hour urine specimens must be collected from a study group
consisting of DU-exposed veterans and civilians for analysis. For
simplicity, creatinine levels might provide the normalizing factor.
If one adopts this procedure, it is not necessary to have 24-hour
urine specimens from the veterans and the civilians. All effort
must be made to determine the biological half life of DUOA from the
lungs. In short, all the analytical data should be collected for
the evaluation of the risk factors for the veterans and the
civilians. The exposed veterans should endeavour to provide,
whenever and where ever possible, the availability of tissue
specimens for compiling analytical data. It will help in
determining pathways of highly insoluble fine dust through the body
before it is excreted from the body. A wide-ranging epidemiological
study should be launched after carefully drawing an acceptable
protocol. This study will help in determining the causative
agent(s) for the symptoms of Gulf war syndrome. A tested
methodology for the determination of DU oxides of ceramic type in
environmental specimens should be followed. Dang et al. have
suggested that the INAA method can be improved by at least a factor
of 10 by chemical separation of Np-239 with calcium phosphate [11].
The two methods (DNC and INAA) can be rapid and cost effective for
the determination of U-235 and U-238 in environmental specimens
that include urine, soil specimens, filters for air-monitoring.
Table 9
Equivalent mass of some radioisotopes in terms of alpha activity
from 2000 mtons of DU.
Radioisotope
Activity/gram
Total mass of
the isotope
(grams)
Total alpha
activity
U-238
14,900/sec
2,000,000,000
2.98E[13]
Pu-239
2.3E[09]/sec
10.32 kilograms
2.37E[13]
Ra-226
3.7E[10]/sec
800 grams
2.7E[13]*
*Alpha activity from progeny
not included.
8. Conclusions.
8.1. After exploring various methodologies for determining the
amount of depleted uranium in environmental specimens, we recommend
U-235 content can be estimated by the DNC method and U-238 content
by the INAA method using Np-239 as the indicator isotope. These two
measurements permit us to determine DU and NU fractions and the DU
content in the specimens. This will also permit evaluation of
radiation insult to the environment in Iraq. If the radiation
insult is found to be excessive, Mitigation methodologies may be
explored to reduce the insult as soon as possible.
8.2. The suggested measurements of DU content in air, in soil
should be made wherever DU munitions have been deployed in Iraq.
8.3. The GWII veterans may be tested periodically by measuring the
DU content in their respective urine sample.
8.4. Children are more susceptible to radiation and therefore
special consideration may be given to shield them from ingesting
particulate matter containing DU. Our analysis of the situation as
it exist today, we have little knowledge as to the amount of DU
that has been dispersed in the form of oxide dust. In case
excessive amount of DU has been deployed during this year, it is
incumbant on the countries to clean the entire country.
9. Acknowledgements.
We are grateful to the veterans who willingly provided 24-hour
urine specimens and to the University authorities for providing
space for conducting this work up to July 1999. Their attitude
toward this study changed suddenly and forced us to stop all work
by confiscating specimens etc. for no valid reasons. We are
extremely grateful to Dr. Beatrice Boctor for arranging to get the
desired specimens for this study and for providing moral support.
Mrs. Pamela Collins unselfishly devoted her time in finding
appropriate methodology for isotopic analysis of uranium isotopes
in environmental specimens. Without her help, this work presented
in this report would not have been performed. Ms. Alice Pidruczny
initially provided help in the eighties in identifying the type of
uranium in body tissues and thus helped in establishing the DNC
method for the determination of U-235 and the INAA method for the
determination of U-238. She provided valuable information for the
determination of abundance of U-235 and U-238. Lastly, we managed
to re-start the study after eviction from the University without
any outside financial support but with our strong belief that
dispersal of radioactivity in the environment will eventually
results in harming bio-life including human beings. Consequently,
such dispersal must be avoided at all cost. Our sincere gratitude
to Dr. G. Spier for providing his expertise in analytical chemistry
willingly without any renumeration.
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