Uranium isotope ‘forensic’ testing in relation to Gulf War Illness
Submitting Institution
University of LeicesterUnit of Assessment
Earth Systems and Environmental SciencesSummary Impact Type
TechnologicalResearch Subject Area(s)
Chemical Sciences: Analytical Chemistry, Other Chemical Sciences
Earth Sciences: Geochemistry
Summary of the impact
Professor Parrish at Leicester developed a unique high sensitivity urine,
soil and particle isotope assay for detection of DU pollution and applied
this to Gulf War veterans to quantify exposure to DU munitions. None of
the Gulf War veterans tested in a UK MoD study had detectable DU; this
allowed the UK government to conclude that DU exposure was limited, and
that the harm to veterans was small, although residual environmental
issues of chronic exposure have yet to be quantified. The test was also
applied to munitions' factory workers and nearby residents, and allowed
the exposure to DU to be quantified in individuals and environmental
materials. This latter study gave rise to a $0.5M exposure and health
study near by the New York State Dept. of Health to better assess the
health impacts of DU aerosol exposure.
Underpinning research
Underpinning research: Geochemical research in the Department of
Geology by Parrish, Brewer and PhD student Lloyd from 2004-2009 used
isotope geochronology and geochemistry methods in collaboration with the
NERC Isotope Geosciences Laboratory (NIGL) that Parrish leads on
secondment from Leicester, to advance uranium isotope measurement
innovation (5, 7). These uranium isotope method
advancements, with their origins in earth science and geochronology, were
adapted and applied to environmental contamination (1, 2, 4)
and environmental health topics in order to address important problems.
Urine and other matrices (soils, organic material, micron sized particles)
are often difficult to work with, but medically and environmentally
important; mass spectrometry methods were adapted in 2004-2008 for these
matrices and are ongoing. For urine, the work consisted of
co-precipitating, concentrating, and purifying tiny amounts (as small as
100 picograms) of uranium from the other undesired elements and compounds
contained in urines, and measuring the precise isotope composition of
uranium to attempt to detect and quantify anthropogenic uranium. This was
demanding since the expectation of the MoD was that samples of urine from
`DU-contaminated' soldiers might only have 1-5% of the uranium in the
samples consisting of DU, this being the expected result if a significant
contamination arose up to 15 years prior to taking a urine sample. A 1-2%
deviation of isotope ratio of 238U/235U was
required for total quantity of uranium of as little as 1 nanogram; in
addition the anthropogenic isotope 236U was required to be
measured at <50 femptogram level of abundance. This had never been
achieved before in either medical or geochemical research. This R&D
was validated by blind externally-administered proficiency tests,
administered by the EU IRMM to stand up to scrutiny (5). In
parallel a method of solid particle (<1003bcm in size) isotope
determination using laser ablation sampling was developed (3),
allowing forensic tracing of particles back to their source, a procedure
used by the IAEA to monitor uranium enrichment worldwide using different
and more costly methods. All of these method innovations have been linked
by the programme of environmental, technical, and health research
undertaken by the Leicester team.
The Leicester team consists of: Professor Randall Parrish
(1996-present, partly seconded to lead NIGL); Dr Tim Brewer (Senior
Lecturer 1994-2007; deceased 2007); Dr Nick Lloyd, PhD student 2006-2009;
Prof S Hainsworth (Engineering).
References to the research
1. Lloyd, N. S., Chenery, S. R. & Parrish, R. R. (2009). "The
distribution of depleted uranium contamination in Colonie, NY, USA."
Science of the Total Environment 408(2): 397-407.
2. Lloyd, N. S., Mosselmans, J. F. W., Parrish, R. R., Chenery, S. R.,
Hainsworth, S. V. & Kemp, S. J. 2009a. The morphologies and
compositions of depleted uranium particles from an environmental
case-study. Min. Magazine, 73 (3), 493-508.
4. Parrish, R. R., Horstwood, MSA, Arneson, J, Chenery, S., Brewer, T.,
Lloyd, N., Carpenter, D. 2008. Depleted uranium contamination by
inhalation exposure and its detection after ~20 years: implications for
human health assessment. Science of the Total Environment v. 390, 58-68;
doi:10.1016/j.scitotenv.2007.09.044.
5. Parrish, RR, Thirlwall, M, Pickford, C, Horstwood, MSA, Gerdes, A.,
Anderson, J., and Coggan, D., 2006, Determination of 238U/235U, 236U/238U
and uranium concentration in urine using SF-ICP-MS and MC-ICP-MS: An
inter-laboratory comparison. Health Physics v.90 (2), p. 127-138.
6. Parrish, RR, Impacts of Depleted Uranium to the natural environment: A
report commissioned by the Natural Environment Research Council for the UK
Ministry of Defence, submitted to NERC and MoD 2010.
Details of the impact
Background to Impact. Two major wars in the Persian Gulf area in
1991 and 2003-2008 involved more than 1M allied military personnel and the
use of DU munitions; subsequent to the 1991 conflict, ~250,000 UK, US, and
Canadian veterans developed Gulf War Illness, the cause of which remains
elusive. Possible culprits are the nerve gas Sarin, DU, excessive
pesticide use during the conflict, and post-traumatic stress. During the
period 1997-2008 there was considerable concern that exposure of military
personnel (and collateral exposure of civilians) to DU munitions might
contribute to illness of veterans (Gulf War Illness, cancer, birth
defects, etc) and have other deleterious environmental effects. These
concerns were documented by the Royal Society and the United Nations in
2001-2002. In 2005 the UK Government appointed the Depleted Uranium
Oversight Board (DUOB) to commission a study to both develop a high
sensitivity assay and to apply this to veterans to find out if DU exposure
was widespread (7); the MoD also commissioned a joint NERC research
programme on the environmental impacts (6). No such test was
available worldwide at that time. At the same time, sites of DU pollution
from manufacturing munitions were poorly studied and understood in terms
of their environmental footprint. A common thread in all of this science
is that a sensitive, reliable test to quantify DU exposure that took place
many years earlier had been lacking, unavailable to the environmental
health community. No DU-exposed human cohort had ever been studied in
terms of aerosol DU particle exposure, and this question was also
addressed by the Leicester group.
Beneficiaries: Beneficiaries of this work are primarily the UK,
Canadian and US governments who have learned that the DU exposure
sustained by Gulf War veterans is more limited than thought. Other
benefits are directly to those ~250,000 US, UK, and Canadian veterans with
Gulf War Illness who can achieve more clarity about whether DU played a
role in their illness. Other beneficiaries are New York Department of
Health who have adopted the Leicester test and are conducting a more
comprehensive exposure and health study on the DU munitions factory site
studied by Leicester personnel. As a follow up to this work, the Atomic
Weapons Establishment (AWE Aldermaston) sought collaboration with the team
and NIGL colleagues to develop a laser ablation ICP-MS method to analyse
uranium isotopes in tiny (~1 03bcm) particles to reduce the cost of
nuclear forensic testing in uranium enrichment establishments for the IAEA
and the UK government.
Direct Impacts. The urine-testing research showed that no tested
veteran had detectable DU (none out of 466 tested, documented in final
report of the DUOB (7 section 4), allowing the UK government to
conclude the study without costly subsequent follow up and be satisfied
that significant exposure to veterans by DU could not be substantiated in
terms of a large group of veterans. This allowed the UK MoD to largely
draw a line under this particular issue, and reduce future expenditure
related to DU-related issues. This is substantiated by a letter from the
lead author on the 2001-2002 Royal Society Report on DU, stating "The
Depleted Uranium Oversight Board were particularly impressed by the high
performance of NIGL in testing for uranium isotopes ....which has
resulted in a much clearer view of the levels of exposure to DU on the
battlefield (which subsequently have been supported by uranium isotope
measurements by Harwell on urine from veterans of the 2001 Gulf War) and
have very largely eliminated further consideration of DU exposure as a
contributor to Gulf War diseases" (C).
The environmental study in New York (1-3) documented the long term
environmental legacy of DU pollution, uptake by plants and animals, slow
migration in soil, and very slow corrosion of highly oxidized DU aerosol
particles. None of these conclusions were known until this work was done,
yet policy decisions need to rely on such evidence. The research proved as
entirely incorrect the conclusions of the US Agency of Toxic
Substances and Disease Registry (ATSDR)which stated that the DU
contamination legacy surrounding the New York manufacturing plant could
not be quantified and that detection in humans after 20 years would be
impossible. The method was applied to exposed individuals to show that DU
particulate exposure is still detectable after 20 years (4).
Arising from this work, the US Congress Committee on Science and
Technology sought testimony from Parrish on 12 March 2009 (A,B)
concerning the research in order to learn lessons about how to quantify
exposure and improve the performance of its own agency responsible for
health concerns in such sites (i.e. ATSDR).
The long term health and environment effects of chronic DU-inhalation or
ingestion exposure are as yet un-quantified, because no health study has
been conducted on putatively-exposed humans, even though numerous animal
studies show mutagenic and teratogenic effects. The Leicester study
directly prompted the New York State Department of Health to conduct in
2011-13 a larger (~$0.5M; cohort of 300) targeted DU exposure and health
study to address the continuing health concerns of that locality, and
Parrish is advising this group with parallel analyses to assess Quality
Control, advice on how best to conduct chemical separations, and in
critical evaluation of method publication. He will likely be involved in
interpretation of exposure once data is acquired by that laboratory on a
cohort in New York.
Although the whole of the 1991 Gulf War veteran cohort is unlikely to
have had significant DU-exposure, it can only be eliminated as a cause of
Gulf War Illness in a proper study of veterans suffering from the illness.
A direct impact of the research is that testing for DU is taking place
during 2011-13 by Parrish on 160 intensively studied Gulf War Illness
sufferers whose medical conditions were the subject of a 10-year, $20M
study at the Southwestern Medical Centre, University of Texas. This DU
exposure study will define the role, if any, of DU in this illness and
conclude in 2013, of considerable medical significance.
Finally, the AWE (Atomic Weapons Establishment Aldermaston) has consulted
Leicester and NIGL personnel in order to conduct collaborative development
and knowledge exchange to develop a more rapid and cost-effective
LA-ICP-MS method to analyse ~103bcm uranium particles in nuclear forensic
safeguard testing at AWE, who have a strategic regulatory national role in
this area. This capability of using LA-ICP-MS for U particle isotope
composition is a priority topic of the IAEA (Vienna) and the nuclear
forensic safeguards community because of the very high cost and time-
consuming nature of doing this work by the alternative FT-TIMS or SIMS
methods, which are the only methods currently accredited by the IAEA;
LA-ICP-MS offers similar sensitivity, faster turnaround and more rapid
analysis including the minor uranium isotopes.
A further specific impact is that the Leicester PhD student who
participated in this work was then quickly employed by a major mass
spectrometry manufacturer as a key applications scientist. He is now
involved in developing and marketing the type of instruments used in the
study to other scientific establishments worldwide including IAEA and AWE;
this is a tangible impact of the high-level training delivered as part of
the on-going research.
Sources to corroborate the impact
Media, and letters
(A) Testimony to US Congress Subcommittee on Investigations and Oversight,
Science and Technology, 12 March 2009 by R Parrish, transcript available
from US Congress Archives http://www.gpo.gov/fdsys/pkg/CHRG-111hhrg47718/html/CHRG-111hhrg47718.htm
(B) Chair of US Congress Subcommittee on Investigations and Oversight.
(C) Chair of Royal Society Working Group on Depleted Uranium, and member
of the Depleted Uranium Oversight Board.
Press
Release
March 12, 2009 Investigations and Oversight Subcommittee Examines
the Failures of the Agency for Toxic Substances and Disease Registry, US
Congress Committee on Science and Technology Hearings; http://archives.democrats.science.house.gov/press/PRArticle.aspx?NewsID=2390
[there have been many other related press releases related to the DU work
but are not itemised].