Beneficial antioxidant status of piglets from sows fed selenomethionine compared with piglets from sows fed sodium selenite.

BACKGROUND: Studies in mammals proved dietary organic selenium (Se) being superior to inorganic Se regarding effects on growth performance, antioxidative status, immune response, and Se homeostasis. However, the picture of possible effects of different Se sources and - levels can be expanded. The present field study evaluated the effects on weight gain, hematological and selected biochemical variables as well as plasma concentrations of vitamin E (vitE), total Se and selenobiomolecules in piglets throughout the suckling period. METHODS: Piglets were monitored from birth to 38 days of age (d). The mother sows' diets were enriched with l-selenomethionine (SeMet-0.26 and -0.43 mg Se/kg feed) or sodium selenite (NaSe-0.40 and -0.60 mg Se/kg feed) from 1 month prior to farrowing until the end of lactation period. Piglets received pelleted feed supplemented with Se similarly to the sows' diets from one week of age. Selenite at 0.40 mg Se/kg (NaSe-0.40) represents a common Se source and -level in pig feed and served as control diet. RESULTS: From 24d, piglets in SeMet-groups had higher mean body weight (BW) compared with piglets from sows fed NaSe-0.40. Furthermore, from five-d and above, piglets from sows fed NaSe-0.60 had significantly higher BW than offspring from sows fed NaSe-0.40. Neonatal piglets in group SeMet-0.43 had significantly lower red blood cell counts (RBC), hemoglobin (Hgb) and hematocrit (Hct) concentrations compared with piglets from sows fed with NaSe-0.40. Neonatal and 5d-old piglets in group SeMet-0.26 showed higher gamma-glutamyl transferase activity than piglets in group NaSe-0.40. From five d and above, group NaSe-0.60 excelled with increased specific hematological variables culminating at age 38d with increased Hct, mean corpuscular volume (MCV), and MC hemoglobin (MCH) as well as increased activities of aspartate transaminase and lactate dehydrogenase compared with the other groups. Generally, offspring in the SeMet groups had higher total Se-concentrations in plasma than those from sows fed selenite, and showed a dose-response effect on plasma Se-concentrations. Furthermore, SeMet-fed piglets had higher plasma levels of the selenoproteins (Sel) glutathione peroxidase 3 (GPx3) and SelP as well as selenoalbumin. Plasma vitE levels were significantly negatively correlated with RBC throughout trial period. CONCLUSIONS: Maternal supplementation with SeMet during gestation influenced hematology and clinical biochemistry in neonatal piglets in a different way than in offspring from sows receiving selenite enriched diets. Growth performance was positively influenced by both dietary Se source and Se level. Higher plasma levels of GPx3 observed in piglets receiving SeMet probably improved the protection against birth or growth related oxidative stress. These might prime the piglets for demanding situations as indicated by higher weight gain in offspring from sows fed with SeMet-supplemented diets. Our results on some enzyme activities might indicate that piglets fed NaSe-0.60 had to cope with increased levels of oxidative stress compared with those originating from sows fed SeMet or lower dietary levels of selenite. We assume that combining inorganic and organic Se sources in complete feed for breeding sows might be beneficial fro reproduction and the offspring's performance.

Turnover of Se in adequately fed chickens using Se-75 as a tracer.

Inorganic selenium (Se) in the form of selenite is applied to livestock to avoid Se deficiency. Selenite is, however, an artificial Se source in diets of unsupplemented chickens. It is therefore hypothesized that organic Se sources, such as Se-enriched yeast and wheat, could be a more suitable Se supply in animal nutrition, although information on the transition of Se from organic Se sources in fast-growing chickens is scarce. In this work, chickens were fed a low Se diet (0.27 ± 0.01 mg Se/kg, Se-enriched yeast) until 20 days of age, after which the Se concentration was increased to maximum concentration allowed by the poultry industry in Europe (0.5 p.p.m. Se). At the same time, a daily contribution of carrier-free (75)Se tracer from labelled wheat was administered from day 20 to 27. The chickens showed S and Se homeostasis, as the concentration of S and Se in liver, blood or kidney remained about constant, and steady state of S and Se in the other organs was reached 1 day after the diet shift. The uptake of (75)Se was readily seen in all organs. After 1 week, the depuration of the (75)Se tracer was followed, and biological half-lives and retention in individual organs were determined. The shortest biological half-lives were observed in major metabolic organs, the liver, kidney and pancreas with half-lives close to 4 days. There was a significant (p < 0.05) uptake in lung, brain and muscle that reached steady state when the administration of (75)Se was terminated. The half-life of (75)Se in heart was 9 days and 7 days in blood. The longest half-lives were observed in muscle (12 days), brain and lungs (13 days). All half-lives were shorter than in Se deplete animals.

Assessment of the radiological impact of gamma and radon dose rates at former U mining sites in Tajikistan.

An assessment of the radiological situation due to exposure to gamma radiation, radon ((222)Rn) and thoron ((220)Rn) was carried out at former uranium (U) mining and processing sites in Taboshar and at Digmai in Tajikistan. Gamma dose rate measurements were made using various field instruments. (222)Rn/(220)Rn measurements were carried out with field instruments for instantaneous measurements and then discriminative (222)Rn/(220)Rn solid state nuclear track detectors (SSNTD) were used for longer representative measurements. The detectors were exposed for an extended period of time in different outdoor and indoor public and residential environments at the selected U legacy sites. The results showed that gamma, (222)Rn and (220)Rn doses were in general low, which consequently implies a low to relatively low radiological risk. The radiation doses deriving from external radiation (gamma dose rate), indoor (222)Rn and (220)Rn with their short-lived progenies did not exceed national or international standards. At none of the sites investigated did the average individual annual effective doses exceed 10 mSv, the recommended threshold value for the general public. A radiation hazard could be associated with exceptional situations, such as elevated exposures to ionizing radiation at the Digmai tailings site and/or in industrial facilities, where gamma and (222)Rn/(220)Rn dose rates could reach values of several 10 mSv/a. Current doses of ionizing radiation do not represent a hazard to the health of the resident public, with the exception of some specific situations. These issues should be adequately addressed to further reduce needless exposure of the resident public to ionizing radiation.

Chronology of Pu isotopes and 236U in an Arctic ice core.

In the present work, state of the art isotopic fingerprinting techniques are applied to an Arctic ice core in order to quantify deposition of U and Pu, and to identify possible tropospheric transport of debris from former Soviet Union test sites Semipalatinsk (Central Asia) and Novaya Zemlya (Arctic Ocean). An ice core chronology of (236)U, (239)Pu, and (240)Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6m deep ice core from the Austfonna glacier at Nordaustlandet, Svalbard is presented. The ice core chronology corresponds to the period 1949 to 1999. The main sources of Pu and (236)U contamination in the Arctic were the atmospheric nuclear detonations in the period 1945 to 1980, as global fallout, and tropospheric fallout from the former Soviet Union test sites Novaya Zemlya and Semipalatinsk. Activity concentrations of (239+240)Pu ranged from 0.008 to 0.254 mBq cm(-2) and (236)U from 0.0039 to 0.053 µBq cm(-2). Concentrations varied in concordance with (137)Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and (236)U were found to be higher at depths corresponding to the pre-moratorium period (1949 to 1959) than to the post-moratorium period (1961 and 1962). The (240)Pu/(239)Pu ratio ranged from 0.15 to 0.19, and (236)U/(239)Pu ranged from 0.18 to 1.4. The Pu atom ratios ranged within the limits of global fallout in the most intensive period of nuclear atmospheric testing (1952 to 1962). To the best knowledge of the authors the present work is the first publication on biogeochemical cycles with respect to (236)U concentrations and (236)U/(239)Pu atom ratios in the Arctic and in ice cores.

Ecological risk assessment of Central Asian mining sites: application of the ERICA assessment tool.

Recent field expeditions to Central Asian mining sites have provided a wealth of data on radionuclide and metal concentrations in environmental media. In this paper the ERICA assessment tool was used to provide an assessment of the potential doses to non-human biota at the various sites. The aim was to identify the most exposed organism types and the radionuclides giving rise to the greatest doses. The measured media and biota activity concentrations were also used to compare site-specific Kds and CRs with default tool parameters. At all terrestrial sites, the maximum doses (up to ca. 600 µGy/h) were seen in lichens and bryophytes, with concentrations of radium in soils dominating the assessments. Internal alpha dose from (226)Ra was the biggest dose contributor, representing between 72 and 97% of the total dose, with U isotopes as the next most significant contributor. For aquatic organisms the highest calculated doses were obtained for aquatic plants (ca. 100 µGy/h), followed by molluscs, crustacean, zooplankton and insect larva, based on at site environmental media data. For aquatic plants, the internal alpha doses from uranium isotopes dominated the dose at most of the sites, hence the highest doses were seen at sites with the highest U concentrations. While the measured and modelled concentrations were usually in reasonable agreement, particularly for U and Ra in terrestrial plants, there were some differences, most notably for U and Po in the aquatic environment. Modelled concentrations of U in aquatic plants tended to be higher than those measured in site samples; while Po in fish was greater than modelled concentrations. Furthermore, not all the organisms listed in the ERICA tool had been sampled at the sites. Nevertheless, the assessment results should be of great benefit in identifying priority areas for future field studies.

Assessment of the radiological impact of gamma and radon dose rates at former U mining sites in Central Asia.

An assessment of the radiological situation due to exposure to gamma radiation, radon and thoron was carried out at selected former uranium mining and processing sites in the Central Asian countries of Kazakhstan, Kyrgyzstan, Uzbekistan and Tajikistan. Gamma dose rate measurements were made using various field instruments and radon/thoron measurements were carried out using discriminative radon ((222)Rn)/thoron ((220)Rn) solid state nuclear track detectors (SSNTD). The detectors were exposed for an extended period of time, including at least three seasonal periods in a year, in different outdoor and indoor public and residential environments at the selected uranium legacy sites. The results showed that gamma, Rn and Tn doses were in general low, which consequently implies a low/relatively low radiological risk. The major radiation hazard is represented by abandoned radioactive filtration material that was being used as insulation by some Minkush residents (Kyrgyzstan) for a longer period of time. Annual radiation doses of several hundred mSv could be received as a consequence of using this material domestically. In addition, the gamma and Rn/Tn dose rates at Digmai, Tajikistan, could reach values of several 10 mSv/a. The doses of ionizing radiation deriving from external radiation (gamma dose rate), indoor radon and thoron with their short-lived progenies in several cases exceeded the recommended annual effective dose threshold level of 10 mSv. At none of the sites investigated did the individual annual effective doses exceed 30 mSv, the internationally recommended value for considering intervention. Current doses of ionizing radiation do not represent a serious hazard to the health of the resident public, but this issue should be adequately addressed to further reduce needless exposure of the resident public to ionizing radiation.

Environmental impact assessment of radionuclide and metal contamination at the former U sites Taboshar and Digmai, Tajikistan.

Uranium (U) ore mining and processing were initiated in the former Soviet Republics of Tajikistan after the Second World War as part of the USSR nuclear weapon programme. The U mine in Taboshar was opened in 1936, and mining took place from 1945 to 1965, while the Digmai tailings dump was exploited during 1963-1993. The mining, milling and extraction activities have resulted in large amounts of waste rock deposits and U tailing materials placed in the vicinity of inhabited areas. To assess the environmental impact of radionuclides and trace metals in the Taboshar and Digmai mining and tailing sites in Tajikistan, field expeditions were performed in 2006 and 2008. In addition to in situ gamma and radon dose rate measurements, sampling of water, fish, sediments, soils and vegetation including in situ fractionation of water were performed. The U concentrations in water from Taboshar Pit Lake (2.0 mg U/L) were higher than in waters collected in the Digmai area. The Pit Lake and the stream water from the tailing mountain were also characterised by elevated concentrations of As, Mo, Mn and Fe, exceeding the WHO recommended values for drinking water. Uranium, As, Mo and Ni were present as low molecular mass species in the waters, and are therefore considered mobile and potentially bioavailable. The (238)U concentrations in sediments and soils varied between the sites; with peak concentrations (6 kBq/kg dw) in sediments from the Pit Lake, while the soil concentrations were significantly lower (296-590 Bq/kg dw). In contrast, high levels of the radium isotopes ((226)Ra and (228)Ra) were found in the Digmai soil (17-32 kBq/kg dw). Based on sequential extraction results, both U and Pb were found to be quite mobile at the Pit Lake site, showing that these elements were associated with the pH sensitive and redox sensitive amorphous fractions. In tailings, U was found to be quite mobile, but here Pb was rather inert. The transfer of radionuclides and metals from sediments to waters was in general low. In the Pit Lake, U was quite mobile (Kd = 90 L/kg), followed by Ni (1.5 × 10(3) L/kg) and As (6 × 10(3) L/kg), Cu and Cd (1.5 × 10(4) L/kg), while Pb (3 × 10(5) L/kg) was rather inert. The transfer from soil to plant, TFs (kg/kg dw), was in general low, while the bioconcentration factor for water living Poaceae and for fish from water was relatively high (Pb 1.8 × 10(5) and Cd 1 × 10(4)). These legacy sites, containing enhanced levels of natural radioactive material (TENORM) as well as heavy metals, may represent a hazard having a potential radiological and chemical impact on man and the environment, and measures should be taken to reduce the environmental risk to man and biota.

Uranium activity ratio in water and fish from pit lakes in Kurday, Kazakhstan and Taboshar, Tajikistan.

Kurday in Kazhakstan and Taboshar in Tajikistan were U mining sites operated during the 1950s and 1960s as part of the USSR nuclear weapon program. Today, they represent sources of potential U contamination of the environment. Within both mining sites, open pits from which U ore was extracted have been filled with water due to ground water inflow and precipitation. These artificial pit lakes contain fish consumed occasionally by the local people, and wild and domestic animals are using the water for drinking purposes. To assess the potential impact from U in these pit lakes, field work was performed in 2006 in Kurday and 2006 and 2008 in Taboshar. Results show that the U concentration in the lake waters were relatively high, about 1 mg/L in Kurday Pit Lake and about 3 mg/L in Taboshar Pit Lake. The influence of U-bearing materials on the lakes and downstream waters were investigated by measuring the U concentration and the (234)U/(238)U activity ratios. In both Kurday and Taboshar, the ratios increased distinctively from about 1 at the pit lakes to >1.5 far downstream the lakes. The concentrations of (238)U in gill, liver, muscle and bones in fish from the pit lakes were much higher than in the reference fish. Peak concentration of U was seen in bones (13 mg/kg w.w.), kidney (9.1 mg/kg w.w.) and gills (8.9 mg/kg w.w.) from Cyprinus auratus caught in the Taboshar Pit Lake. Bioconcentration factors (BCF) calculated for organs from fish caught in the Taboshar Pit Lake, with the same tendency seen in the Kurday Pit Lake, showed that U accumulates most in bone (BCF = 4.8 L/kg w.w.), gills (BCF = 3.6 L/kg w.w.), kidney (BCF = 3.6 L/kg w.w.), and liver (BCF = 2.5 L/kg w.w.), while least was accumulated in the muscle (BCF = 0.12 L/kg w.w.).

Micro-analytical characterisation of radioactive heterogeneities in samples from Central Asian TENORM sites.

The present work focuses on the use of micro-analytical techniques to demonstrate the heterogeneous distribution of radionuclides and metals in soils collected at Former Soviet Union mining sites in Central Asia. Based on digital autoradiography, radionuclides were heterogeneously distributed in soil samples collected at the abandoned uranium mining sites Kurday, Kazakhstan, Kadji Sai, Kyrgyzstan and Taboshar, Tajikistan. Using electron microscopy interfaced with X-ray microanalysis submicron - mm-sized radioactive particles and rock fragments with U, As, Se and toxic metals on the surfaces were identified in Kurday and Kadji Sai samples. Employing scanning and tomographic (3D) synchrotron radiation based micro-X-ray fluorescence (µ-SRXRF) and synchrotron radiation based micro-X-ray diffraction (µ-SRXRD) allowed us to observe the inner structure of the particles without physical sectioning. The distribution of elements in virtual crosssections demonstrated that U and a series of toxic elements were rather heterogeneously distributed also within individual radioactive TENORM particles. Compared to archived data, U in Kadji Sai particles was present as uraninite (U4O9+y or UO2+x) or Na-zippeite ((Na4(UO2)6[(OH)10(SO4)3]·4H2O), i.e. U minerals with very low solubility. The results suggested that TENORM particles can carry substantial amount of radioactivity, which can be subject to re-suspension, atmospheric transport and water transport. Thus, the potential radioecological and radioanalytical impact of radioactive particles at NORM and TENORM sites worldwide should be taken into account. The present work also demonstrates that radioecological studies should benefit from the use of advanced methods such as synchrotron radiation based techniques.

Po-210 and Pb-210 in water and fish from Taboshar uranium mining Pit Lake, Tajikistan.

Polonium-210 in water and (210)Pb and (210)Po in different fish organs from 3 different fish species in Taboshar Pit Lake (n = 13), located in the uranium mining area in Tajikistan, and in Kairakkum Reservoir (reference lake, n = 3), have been determined as part of a Joint project between Norway, Kazakhstan, Kyrgyzstan and Tajikistan. The average activity concentration of (210)Pb and (210)Po in liver, muscle and bone of Carassius auratus was higher than the concentration in similar tissues of C. carpio and Sander lucioperca from the reference site. The accumulation of (210)Po was higher than for (210)Pb, and the accumulation of (210)Po was highest in the liver of C. auratus (3673 ± 434 Bq kg(-1) ww). Although the average activity concentration of (210)Pb in liver and bones of C. auratus from Pit Lake were fairly similar, a huge variation in the liver activity concentrations (25-327 Bq kg(-1) ww) was found. The results confirm direct uptake of unsupported (210)Po into the liver, and that the distributions of (210)Po and (210)Pb in fish organs were different. The BCF (L/kg) for (210)Po in bone, liver and muscle clearly demonstrates high accumulation of (210)Po in C. auratus, especially in the liver. The average BCFs of liver, bone and muscle were >1.4 × 10(5), >2.5 × 10(4) and >1.4 × 10(4), respectively. All fish in the Pit Lake were found to be in the same trophic level, however, a linear correlation between log (210)Po in liver and δ(15)N could indicate biomagnification of (210)Po in liver of C. auratus. In regards to the recommended Annual Limit of Intake (ALI) for (210)Po, the concentration of (210)Po in muscle tissues of C. auratus is alarming, as there is a high probability for the local population at risk to exceed the recommended ALI through consumption of fish from Taboshar Pit Lake.

Environmental impact assessment of radionuclide and metal contamination at the former U site at Kadji Sai, Kyrgyzstan.

During 1949-1967, a U mine, a coal-fired thermal power plant and a processing plant for the extraction of U from the produced ash were operated at the Kadji Sai U mining site in Tonsk district, Issyk-Kul County, Kyrgyzstan. The Kadji Sai U legacy site represents a source of contamination of the local environment by naturally occurring radionuclides and associated trace elements. To assess the environmental impact of radionuclides and trace metals at the site, field expeditions were performed in 2007 and 2008 by the Joint collaboration between Norway, Kazakhstan, Kyrgyzstan, Tajikistan (JNKKT) project and the NATO SfP RESCA project. In addition to in situ gamma and Rn dose rate measurements, sampling included at site fractionation of water and sampling of water, fish, sediment, soils and vegetation. The concentrations of radionuclides and trace metals in water from Issyk-Kul Lake were in general low, but surprisingly high for As. Uptake of U and As was also observed in fish from the lake with maximum bioconcentration factors for liver of 1.6 and 75, respectively. The concentrations of U in water within the Kadji Sai area varied from 0.01 to 0.05 mg/L, except for downstream from the mining area where U reached a factor of 10 higher, 0.2 mg/L. Uranium concentrations in the drinking water of Kadji Sai village were about the level recommended by the WHO for drinking water. The (234)U/(238)U activity ratio reflected equilibrium conditions in the mining pond, but far from equilibrium outside this area (reaching 2.3 for an artesian well). Uranium, As and Ni were mainly present as low molecular mass (LMM, less than 10 kDa) species in all samples, indicating that these elemental species are mobile and potentially bioavailable. The soils from the mining sites were enriched in U, As and trace metals. Hot spots with elevated radioactivity levels were easily detected in Kadji Sai and radioactive particles were observed. The presence of particles carrying significant amount of radioactivity and toxic trace elements may represent a hazard during strong wind events (wind erosion). Based on sequential extractions, most of the elements were strongly associated with mineral matter, except for U and As having a relatively high remobilization potential. Low Kd was obtained for U (3.5 × 10(2) L/kg d.w.), intermediate Kds (~3 × 10(3) L/kg d.w.) were obtained for (226)Ra, As and Ni, while a high Kd (2.2 × 10(5) L/kg d.w.) were obtained for Pb. The accumulation of metals in fish gills reflected the LMM species in the Issyk-Kul water, and did not show any bioaccumulation. The muscle Hg concentrations in all fish species were low and did not represent any health risk even for groups at risk. Total gamma and Rn dose rate to man amounted to about 12 mSv/y, while the highest calculated dose rate for non-human species based on the ERICA Assessment Tool were obtained in terrestrial plants (164 µGy/h) due to the Ra exposure. The results obtained showed that radiation doses to resident public at all of the investigated sites in the Kadji Sai area were in general relatively low. Low radiological risk and no detrimental health impact on resident public can be expected at these sites. However, exposure to Rn and Tn in the living environment can be further reduced by implementing simple countermeasures such as ventilation of dwelling cellars. More focus in the Kadji Sai area should probably be put on trace elements, especially the As uptake in fish in Lake Issyk-Kul.

Environmental impact assessment of radionuclides and trace elements at the Kurday U mining site, Kazakhstan.

The Kurday uranium mining site in Kazakhstan operated from 1954 to 1965 as part of the USSR nuclear weapon programme. To assess the environmental impact of radionuclides and trace elements associated with the Kurday mining site, field expeditions were performed in 2006. In addition to in situ gamma and (220)Rn dose rate measurements, sampling included at site fractionation of water as well as sampling of water, fish, sediment, soils and vegetation. The concentrations of U and associated trace metals were enriched in the Pit Lake and in the artesian water (U exceeding the WHO guideline value for drinking water), and decreased downstream from the mining area. Uranium, As, Mo and Ni were predominantly present as mobile low molecular mass species in waters, while a significant proportion of Cr, Mn and Fe were associated with colloids and particles. Due to oxidation of divalent iron in the artesian ground water upon contact with air, Fe served as scavenger for other elements, and peak concentrations of U-, Ra-isotopes, As and Mn were seen. Most radionuclides and trace elements were contained in minerals in soils and sediments, and good correlations were obtained between U and As, Cd, Mo and (226)Ra. Based on sequential extractions, a significant fraction of U, Pb and Cd could be considered mobile. Radioactive particles carrying significant amount of trace metals may represent a hazard during strong wind events. The transfer of radionuclides and metals from soils or sediments to water was in general low. The Kd levels varied with the element in question, ranging from 0.5 to 3 × 10(2) L/kg d.w. for (238)U being relatively mobile, 10(3) for (226)Ra, As, Cd, Ni, to 10(4) L/kg d.w. for Cu, Cr and Pb being rather inert The transfer of radionuclides and metals from soils to vegetation (TF) was low, while higher if the transfer to vegetation, especially underwater mosses, occurred via water (e.g., BCF 37 L/kg w.w. for (238)U and 3 × 10(3) L/kg w.w. for (226)Ra). The transfer of Cd, Pb and As from water to fish liver (BCF) was rather high, showing BCFs in the range of 10(2)-10(3) L/kg w.w., and may, if eaten, represent a health risk. Furthermore, the high Hg level in fish filet reaching 0.3 mg/kg w.w. muscle and the tendency of biomagnification call for dietary restrictions. Total gamma and Rn dose rate to man amounted to about 6 mSv/y, while the highest calculated dose rate for non-human species based on the ERICA Assessment Tool were obtained in aquatic plants, with calculated mean doses of 700 µGy/hr, mostly due to the U exposure. Overall, it is concluded that measures such as restricted access to the Pit Lake as well as dietary restrictions with respect to drinking water and intake of fish should be taken to reduce the environmental risk to man and biota.

Solid state speciation and potential bioavailability of depleted uranium particles from Kosovo and Kuwait.

A combination of synchrotron radiation based X-ray microscopic techniques (mu-XRF, mu-XANES, mu-XRD) applied on single depleted uranium (DU) particles and semi-bulk leaching experiments has been employed to link the potential bioavailability of DU particles to site-specific particle characteristics. The oxidation states and crystallographic forms of U in DU particles have been determined for individual particles isolated from selected samples collected at different sites in Kosovo and Kuwait that were contaminated by DU ammunition during the 1999 Balkan conflict and the 1991 Gulf war. Furthermore, small soil or sand samples heavily contaminated with DU particles were subjected to simulated gastrointestinal fluid (0.16 M HCl) extractions. Characteristics of DU particles in Kosovo soils collected in 2000 and in Kuwait soils collected in 2002 varied significantly depending on the release scenario and to some extent on weathering conditions. Oxidized U (+6) was determined in large, fragile and bright yellow DU particles released during fire at a DU ammunition storage facility and crystalline phases such as schoepite (UO(3).2.25H(2)O), dehydrated schoepite (UO(3).0.75H(2)O) and metaschoepite (UO(3).2.0H(2)O) were identified. As expected, these DU particles were rapidly dissolved in 0.16 M HCl (84 +/- 3% extracted after 2 h) indicating a high degree of potential mobility and bioavailability. In contrast, the 2 h extraction of samples contaminated with DU particles originating either from corrosion of unspent DU penetrators or from impacted DU ammunition appeared to be much slower (20-30%) as uranium was less oxidized (+4 to +6). Crystalline phases such as UO(2), UC and metallic U or U-Ti alloy were determined in impacted DU particles from Kosovo and Kuwait, while the UO(2,34) phase, only determined in particles from Kosovo, could reflect a more corrosive environment. Although the results are based on a limited number of DU particles, they indicate that the structure and extractability of DU particles released from similar sources (metallic U penetrators) will depend on the release scenarios (fire, impact) and to some extent environmental conditions. However, most of the DU particles (73-96%) in all investigated samples were dissolved in 0.16 M HCl after one week indicating that a majority of the DU material is bioaccessible.

Characterization of U/Pu particles originating from the nuclear weapon accidents at Palomares, Spain, 1966 and Thule, Greenland, 1968.

Following the USAF B-52 bomber accidents at Palomares, Spain in 1966 and at Thule, Greenland in 1968, radioactive particles containing uranium (U) and plutonium (Pu) were dispersed into the environment. To improve long-term environmental impact assessments for the contaminated ecosystems, particles from the two sites have been isolated and characterized with respect to properties influencing particle weathering rates. Low (239)Pu/(235)U (0.62-0.78) and (240)Pu/(239)Pu (0.055-0.061) atom ratios in individual particles from both sites obtained by Inductively Coupled Plasma Mass Spectrometry (ICP-MS) show that the particles contain highly enriched U and weapon-grade Pu. Furthermore, results from electron microscopy with Energy Dispersive X-ray analysis (EDX) and synchrotron radiation (SR) based micrometer-scale X-ray fluorescence (micro-XRF) 2D mapping demonstrated that U and Pu coexist throughout the 1-50 microm sized particles, while surface heterogeneities were observed in EDX line scans. SR-based micrometer-scale X-ray Absorption Near Edge Structure Spectroscopy (micro-XANES) showed that the particles consisted of an oxide mixture of U (predominately UO(2) with the presence of U(3)O(8)) and Pu ((III)/(IV), (IV)/(V) or (III), (IV) and (V)). Neither metallic U or Pu nor uranyl or Pu(VI) could be observed. Characteristics such as elemental distributions, morphology and oxidation states are remarkably similar for the Palomares and Thule particles, reflecting that they originate from similar source and release scenarios. Thus, these particle characteristics are more dependent on the original material from which the particles are derived (source) and the formation of particles (release scenario) than the environmental conditions to which the particles have been exposed since the late 1960s.

Characterization of uranium and plutonium containing particles originating from the nuclear weapons accident in Thule, Greenland, 1968.

To improve long-term radioecological impact assessment for the contaminated ecosystem of Bylot Sound, Greenland, U and Pu containing particles have been characterized with respect to particle size, elemental distribution, morphology and oxidation states. Based on scanning electron microscopy with XRMA, particles ranging from about 20 to 40 microm were isolated. XRMA and mu-XRF mapping demonstrated that U and Pu were homogeneously distributed throughout the particles, indicating that U and Pu have been fused. Furthermore, mu-XANES showed that U and Pu in the particles were present as mixed oxides. U was found to be in oxidation state IV whereas Pu apparently is a mixture of Pu(III) and Pu(IV). As previous assessments are based on PuO2 only, revisions should be made, taking Pu(III) into account.

Oxidation states of uranium in depleted uranium particles from Kuwait.

The oxidation states of uranium in depleted uranium (DU) particles were determined by synchrotron radiation based mu-XANES, applied to individual particles isolated from selected samples collected at different sites in Kuwait. Based on scanning electron microscopy with X-ray microanalysis prior to mu-XANES, DU particles ranging from submicrons to several hundred micrometers were observed. The median particle size depended on sources and sampling sites; small-sized particles (median 13 microm) were identified in swipes taken from the inside of DU penetrators holes in tanks and in sandy soil collected below DU penetrators, while larger particles (median 44 microm) were associated with fire in a DU ammunition storage facility. Furthermore, the (236)U/(235)U ratios obtained from accelerator mass spectrometry demonstrated that uranium in the DU particles originated from reprocessed fuel (about 10(-2) in DU from the ammunition facility, about 10(-3) for DU in swipes). Compared to well-defined standards, all investigated DU particles were oxidized. Uranium particles collected from swipes were characterized as UO(2), U(3)O(8) or a mixture of these oxidized forms, similar to that observed in DU affected areas in Kosovo. Uranium particles formed during fire in the DU ammunition facility were, however, present as oxidation state +5 and +6, with XANES spectra similar to solid uranyl standards. Environmental or health impact assessments for areas affected by DU munitions should therefore take into account the presence of respiratory UO(2), U(3)O(8) and even UO(3) particles, their corresponding weathering rates and the subsequent mobilisation of U from oxidized DU particles.

Depleted uranium particles in selected Kosovo samples.

Selected soil samples, collected in Kosovo locations where DU ammunition was expended during the 1999 Balkan conflict, have been investigated by secondary ion mass spectrometry (SIMS), X-ray fluorescence imaging using a micro-beam (micro-XRF) and scanning electron microscopy equipped with an energy dispersive X-ray fluorescence detector (SEM-EDXRF), with the objective to test the suitability of these techniques to identify the presence of small DU particles and measure their size distribution and the 235U/238U isotopic ratio (SIMS). Although the results do not permit any legitimate extrapolation to all the sites hit by the DU rounds used during the conflict, they indicated that there can be "spots ' where hundreds of thousands of particles may be present in a few milligrams of DU contaminated soil. The particle size distribution showed that most of the DU particles were <5 microm in diameter and more than 50% of the particles had a diameter <1.5 microm. Knowledge on DU particles is needed as a basis for the assessment of the potential environmental and health impacts of military use of DU, since it provides information on possible re-suspension and inhalation.

Oxidation states of uranium in DU particles from Kosovo.

The oxidation states of uranium contained in depleted uranium (DU) particles were determined by synchrotron radiation based micro-XANES, applied to individual particles in soil samples collected at Ceja Mountain, Kosovo. Based on scanning electron microscopy (SEM) with XRMA prior to micro-XANES, DU particles ranging from submicrons to about 30 microm (average size: 2 microm or less) were identified. Compared to well-defined standards, all investigated DU particles were oxidized. About 50% of the DU particles were characterized as UO2, the remaining DU particles present were U3O8 or a mixture of oxidized forms (ca. 2/3 UO2, 1/3 U3O8). Since the particle weathering rate is expected to be higher for U3O8 than for UO2, the presence of respiratory U3O8 and UO2 particles, their corresponding weathering rates and subsequent remobilisation of U from DU particles should be included in the environmental or health impact assessments.