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Investigations of Environmental Impacts from the Deployment of Depleted Uranium MunitionsDr. Hari Sharma
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 U-238, 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 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 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
pre-set 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 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 1.10. It has been shown unambiguously that the
deployment of DU-based 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
DU-based 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 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]/[U-238] 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 bio-kinetics 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 computer-controlled 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 Ser.
No. Volume
mL U-235(NU) by the DNC# method microgram U-238 by the INAA method,^ microgram Uranium content/L* NU# DU# 1.
74 80
0.04 0.07 0.03
0.12
0.2 <0.2 0.2
<0.2 0.47
2.7 1.19 <2.5 2.
76 <0.02 0.02 0.3 0.17 0.2
0.3 3.
87 77 <0.02
0.04 0.02
0.07
0.3 <0.2 <0.2
<0.2 0.17
2.3 0.71 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
2.27 10.
75 81 <0.02
0.14 <0.02
0.07
0.2 0.2 <0.2
<0.2 11.
84 75 <0.02
0.04 <0.02
0.02 <0.2 0.2 <0.2
0.3 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 15.
78 75 <0.02
0.05 0.02
0.05 <0.2
<0.2 <0.2
<0.2 16. 82 0.07 <0.02 0.2 <0.2 0.5
1.83 17. 81 0.06 0.11 <0.2 <0.2 Mix 18. 75 <0.02 <0.02 <0.2 <0.2 19. 78 0.10 0.10 <0.2 <0.2 20. 68 <0.02 0.07 <0.2 <0.2 IND-Mix 21 80 0.05 0.08 <0.2 <0.2 IND-Mix 22.
79
0.07 0.11 <0.2 <0.2 1.1
2.5 23. 75 <0.02 0.17 <0.2 <0.2 24. 77 0.03 0.03 <0.2 <0.2 25. 79 0.11 0.08 <0.2 <0.2 Mix 26. 80 <0.02 0.06 <0.2 <0.2 27. 80 0.13 0.16 0.2 <0.2 1.8
3.1 28. 78 <0.02 0.12 <0.2 <0.2 29. 78 <0.02 0.12 <0.2 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. ----------------------------------------------------------------- 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 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. <1.83 1.3
<2.53 1.79 7. 1st. 1.9 6.9 1.3 1.3
<2.63 5.921 1.86 1.86 8. 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. 2. DU 1.7
2.9 1.2
1.4
<2.38 3.333 1.68
1.889 12. 1. DU 4.0
1.3
1.852 1.75 13. 1. DU 2.3 1.3
4.321 Ser No. Remarks [U-235]
nanograms Errors
+/-ng [U-238]
micrograms Errors+/-mig 14 1. 2.0
7.9 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 1.887 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 < = 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, 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]/[U-238]. 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 NU Fraction = 1-X/T 0.002015 100 per cent 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 [U-235]/[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 3.10. There is only one complete result from
the 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 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 3.14. Pure NU has no U-236 in it but both EU
and DU streams have U-236. 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. Mono-energetic 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 See para 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 code:- (Ir.V)^Iraqi GWI
veteran., (Ir.CD)* civilian from (Ir.CBr)@ Civilian from
Basra., (B.V.) British veteran.,(US) Veteran from the ------------------------------------------------------------------ 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 computer-controlled
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 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
DU-munitions 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 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 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
1 & 3
0.48^+/-0.08 0.006(2) DU fraction
0.24
4 1.55 +/-0.29 0.007(1) Most likely
NU Battlefield
9,10 & 12 0.35^+/-0.12 0.006
DU fraction area 0.24 0.38 +/-0.12* 0.006 11 1.85 +/-0.68 0.006 * weighted average. ^ Arithmetic average.
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 DU-oxide 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 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
DU-munitions (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. Bou-Raabi'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 fall-out 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 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 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 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 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 6.8. For testing the validity of our
calculations, we decided to get tissues of various organs from deceased persons
who resided in 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 U-238 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 Table VII Specimen [U-235]
[U-238] Natural uranium(ICP-MS)
DNC(ppb) INAA(ppb) U-238
[U-235]/[U-238] A (Blank)
<DL <DL <DL ND B (Tissue)
<0.087 35+/-16* 4.9+/-0.03# 0.0079 (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. Table VIII
Medical and Work history of
three uranium workers Worker X Y Z Year of Birth 1921 1927? Not Avaible
Death 1980 1984 1981 Cause of
Metastatic adeno Cancer Carcinoma of Death
carcinoma the tongue Nature of
Worked as a control In uranium
Employed at work operator in buildings Enrichment Feed Material
C310 & C315 meant for plant(building) Center in
product and tailing 1410
in the K25
withdrawl. 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 Isoto- U-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
0.3 0.8 0.036+/-0.004, <0.3 Bones II-II <0.01# 0.1
0.040+/-0.004. <0.2
I-I <0.02# 0.2
II-II <0.02# 0.2 Lungs I
0.027+/-0.013, <0.16; <0.22^ Lungs II 0.13 +/-0.018, <0.13; <0.039 Kidneys I 0.020+/-0.006, <0.4; kidneys II 0.036+/-0.005, <0.2; Liver 0.025+/-0.006, <0.25; Lymph nodes 0.24 +/-0.04 , <0.2 ; <0.06 Type of uranium:-DU,with R=0.0027
EU with U in the lymph nodes nearly
the same with R= 0.035. Lymph
nodes R as found in
DU have higher U content about 2 deployed in GWI 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 Bone(Sternum)
0.027+/-0.01b 0.33 (0.05)# Bone(neck)
0.022+/-0.01b 0.27 (0.05)# Kidney(wet-Ox) 0.024+/-0.01c 0.29 (0.005)# Kidney(F-D) 0.034+/-0.004c Blank
0.001
nil Lungs(wet-Ox) 1.105+/-0.02c 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 U-235 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 Metabolic Data (ICRP)
[Ref.10] Standard Man micrograms ppm* Total Uranium (75 kg) 90 0.0012 Skeletal tissues (7kg) 59
0.008 Kidneys (300 grams) 7 0.023 Average Daily Intake 1.9 See Ref. 32 for organ
mass. 7.
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
24-hour specimens of urine taken from the veterans from four countries. Uranium
oxides were found in deceased civilians who resided in 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 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 well-known 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 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 kilo-grams 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 8.2. The suggested measurements of DU content
in air, in soil should be made wherever DU munitions have been deployed in 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. 10. References. (1) Shleien, B., L.A.
Slaback and B.K. Birky,
Handbook of Health Physics and Radiological Health, Publishers, Williams and
Wilkins, Baltimore, MD, U.S.A., Working Safely with Uranium, pp 720 – 726. (2) N.E. Holden, Table of the Isotopes,
Handbook of Chemistry and Physics, 78th Edition, 11-41 to 11-146 (1997-98). (3) Gerhart
Friedlander, Joseph W. Kennedy, Edward. S.Macias and
Julian M. Miller, Nuclear and Radiochemistry, John Wiley & Sons, (4) Diets, L., Isotopic Measurements of
Depleted Uranium by Mass Spectrometry. Private Communication
1999. (5) Fahey, D., The
Military Toxic Project, Don’t Look Don’t Find, Gulf War Veterans, the (6) Fahey, D., Science or Science Fiction? Facts, Myths and Propaganda, In the Debate over Depleted Uranium
Weapons. An Essay. (7) Diets, L., and H.C. Hendrickson,in
Selected Measurement methods for Plutonium and Uranium in the Nuclear Fuel
Cycle, Compiled and edited by R.A. Jones, Method 2.502, Mass Spectrometric
Isotopic Analysis of Uranium and Plutonium using the V type Surface-Ionization
Filament. (8) International Commission on Radiological
Protection (ICRP). 1994. Human Respiratory Tract Model for Radiological
Protection. ICRP Publication No. 66. Anals of the ICRP 24(1-3) (9) (10) International Commission on Radiological
Protection (ICRP). 1975. Report of the Task Group on (11) Dang, H.S., V.R. Pullat,
K.C. Pillay, Determining the Normal Concentration of
Uranium in Urine and Application of the Data to Its Biokinetics,
Health Physics, 62, 1992, pp 562-556. (12) Madley, D.W., R.L.Kathren, and A.G. Miller, Diurnal Urinary Volume and
Uranium Output in Uranium Workers and Unexposed Controls. Health
Physics, 1994. 67, pp 122-130. (13) Goldstein, S.J., J.M. Rodriguez, and N. Luzan, Measurement and Application of Uranium Isotopes for
Human and Environmental Monitoring, Health Physics, 72, 1997, pp 10-18. (14) Diets, L., Isotopic Measurements of
Depleted Uranium by Mass Spectrometry, Private Communication, 1999-2002. (15) Richter, S., A. Alonso, R. Wellum, and P.D.P. Taylor, The
Isotopic Composition of Commercially Available Uranium Chemical Reagent, J.
Anal. At. Spectrom., 14, 1999, pp 889-891. (16) Ejnik, J.W.,
A.J. Carmichael, M.M. Hamilton, M. McMiarmid, K.
Squibb, P.Boyd and W. Tardiff,
Determination of the Isotopic Composition of Uranium in Urine by Inductively
Coupled Plasma Mass Spectrometry, Health Physics, 2000, 78, pp 143-146. (17) The Royal Society, The Health Hazards of
Depleted Uranium Munitions, Part 1, Policy Document 6/01, May 2001. (18) Fahey, D., Case Narrative, Depleted
Uranium (DU) Exposures, Military Toxic Group, The National Gulf War
Resource Center Inc., Report 23 quoted on pp 15,
Summation of ARDEC Test Data Pertaining to the Oxidation of DU During
Battlefield Conditions, US Army Armament Research, Development and Engineering Center (ARDEC); March 8, 1991;p 2. (19) Harley, N., E.C. Foulkes,
L.H. Hilborne, A. Hudson, and C.R. Anthony, A Review of the Scientific Literature as Pertains to the
Gulf War Illnesses, Volume 7, Depleted Uranium, Rand Corporation National
Defence Institute, (20) Bou-Rabee, F.,
Estimating the Concentration of Uranium in Some Environmental samples after the
1991 Gulf War, Appl. Radiat.
Isot., 46, 1995, pp217-220. (21) Operation Southern Watch, Interim Soil
Report, Total Uranium and Isotope Uranium Results, CHPPMProject
No. 47-EM-8111-98. (22) United Nations Environmental Programme, Depleted Uranium in (23) Nishima, J.,
M.A. Parkhurst, R.I. Shelpelz,
and D.E. Hadlock, Potential Behaviour of Depleted
Uranium Penetrators under Shipping and Bulk Storage
Condition, Bettelle Northwest Pacific Laboratories,
Report DE8500978 PNL-5415, March 1985. (24) Avadhanula,
M.R., R.M. Chatterji, P.J. Horvath, M.P. Measures and
H. Stoker, Atomic Energy Control Board, C. Pomroy,
Radiation Protection Bureau, Dept. of National Health and Welfare, J.R. Johnson
and D.W. Dunford, Chalk River Nuclear Laboratories,
Chalk river. Canadian Uranium Fuel
(uranium dioxide) Fabrcation Study:I. Intake, Retention and Excretion Monitoring
Results II Comparison of Results with Metabolic Models, The International
Atomic Energy Agency (IAEA)-SM-276/5. (25) UNSCEAR 1972 (United Nations Scientific
Committee on the effects of Atomic Radiation) Ionizing Radiation
: Levels and Effects. Volume I, pp 50-95. (26) UNSCEAR 1982 (United Nations Scientific
Committee on the Effects of Atomic Radiation) Ionizing Radiation: Sources and Biological
Effects. Pp 10 and 13-16. (27) 2003 Recommendations of the ECRR, The
Health Effects of Ionising Radiation Exposure at Low Doses for Radiation
Protection Purposes, Edited by Chris Busby, Published on behalf of the European
Committee on Radiation Risk, Green Audit, 2003. (28) Stewart, A.M., Radiogenic Cancers of
Childhood, Radiation Biology of the Fetal and
Juvenile Mammal, Proceedings of the Ninth Annual Hanford Biology Symposium at
Richland, WA, pp 681-691. (29) Sternglass,
E.J., Evidence for Low-level Radiation Effects on the Human Embryo and Fetus. Ibid., pp 691-717. (30) Moskalev, J.L.,
L.A. Buldakov, A.M. Lyaginskaya,
E.P. Ovacharenko and T.M. Egorova,
ibid., Experimental Study of Racionuclide Transfer
Through the Placenta and their Biological Action on the Fetus,
pp 153-160. (31) UNSCEAR 1988 (United Nations Scientific
Committee on the Effects of the Atomic Radiation). Sources, Effects and Risks
of Ionizing Radiation (32) Cember, H., Inroduction to Health Physics, 2nd. Edition,
Appendix III, The Standard Man: Mass and Effective radius of organs of the
Adult Human Body. This
page: http://www.stopnato.org.uk/du-watch/sharma/du-report.htm
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