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.

Prussian Blue to reduce radiocaesium accumulation in fish in lakes affected by the Chornobyl accident.

Fish in lakes situated within the Chornobyl exclusion zone have been highly contaminated since the accident and have not been utilized as food for humans. In the present study, field experiments with less-contaminated silver Prussian carp (Carassius gibelio (Bloch, 1782)) caged in contaminated lake within the Chornobyl exclusion zone was performed from June to October 2021 to investigate the effectiveness of clean feed containing potassium ferric hexacyanoferrate (KFCF) KFe[Fe(CN)6], a kind of Prussian Blue as a countermeasure to reduce 137Cs accumulation in fish. The addition of clean feed containing 0.1% or 1% KFCF resulted respectively in 2.4 ± 0.4 or 4.2 ± 0.7 times lower activity concentration of 137Cs in muscle tissue of the carp compared to control fish with clean feed without KFCF and in 7-16 or 12-27 times lower activities compared to fish without additional clean feeding. After 18 weeks exposure, 137Cs levels in all the caged fish except for the control group were below the European permissible level (600 Bq kg-1) for consumption. In contrast, KFCF did not affect the intake of 90Sr in fish, although additional feed increased the growth rate and thereby accumulation in bone tissues. Hence, the use of clean feed containing KFCF is judged to be an effective and inexpensive countermeasure to reduce the 137Cs contamination of edible fish muscles.

Cobalt reduces the Δ9-desaturase index of sow milk.

The main objective of this study was to examine if cobalt (Co) reduces Δ(9) -desaturase indices in milk and blood lipids in sows. The experimental design consisted of a repeated measurement consisting of a pre-treatment period of a minimum of 9 days, a treatment period of 5 days and a post-treatment period of 6 days. Experimental animals consisted of 10 lactating sows; five sows had an intramuscular injection of 59 mg Co diluted in 5 ml 0.9% saline solution twice a day, whereas the other five had an intramuscular injection of 5 ml 0.9% saline solution twice a day as a control. Milk Δ(9) -desaturase indices for cis-9 18:1, cis-9 16:1 and cis-9 14:1 were significantly reduced (p < 0.0001) as a result of the Co-treatment, contrasting with the plasma Δ(9) -desaturase indices, which were unaffected. Potential mechanisms explaining how Co might reduce milk Δ(9) -desaturase indices are discussed. Moreover, the toxicological level of Co and potential implications of using Co-ethylenediaminetetraacetic acid as a liquid marker in digestibility experiments are addressed.

Uncertainties in short term prediction of atmospheric dispersion of radionuclides. A case study of a hypothetical accident in a nuclear floating power plant off the West coast of Norway.

Short-term predictions for dispersion of radionuclides in the atmosphere following releases from nuclear incidents are associated with uncertainties originating from meteorology, source term and parameterization. Characterization of these uncertainties is of key importance for preparedness, decision making during an accident and for the further uncertainty propagation in the subsequent modelling of human and ecosystem exposures. Increased traffic of nuclear-propulsion vessels in Norwegian territorial waters gives rise to growing concern of a potential nuclear accident along the coast of Norway. In the present study, we have quantified and inter-compared the uncertainties associated with the model outputs for a hypothetical loss of coolant accident with an ensuing fire in a nuclear vessel situated along the Norwegian coastline, applying two different atmospheric dispersion models: the SNAP Lagrangian particle model (SNAP-Severe Nuclear Accident Program) and the DIPCOT Lagrangian puff model (DIPCOT - Dispersion over Complex Terrain). The case highlights a situation with atmospheric transport from the offshore area to the coast of Western Norway, combined with large wet deposition in inland mountainous terrain, i.e. a common weather situation in this region. The meteorological data include an Ensemble Prediction System with nine ensemble members in addition to a deterministic base run. Five different 7 h emission scenarios with the same total released activity were considered. Hourly wind data at 10 m above ground for a 24 h period, showed that 36% of the wind direction and 41% of the wind speed data were outside the spread of the meteorological ensemble. About 55% and 13% of the measured values fell outside the ensemble for hourly 2 m above ground temperatures and 3 hourly accumulated precipitation, respectively, indicating that the ensemble did not cover all uncertainties in the meteorological fields. The maps of accumulated concentrations and depositions were qualitatively similar for the two models, but SNAP predicted higher accumulated concentration levels compared to DIPCOT for quite large areas, while DIPCOT yielded larger total depositions in the same areas. Furthermore, the direction, speed of movement and spatial extension of the radioactive plume from the accident varied considerably from one model to the other. The spread in the dispersion of the radionuclides ranged from a factor of about 1-3 in the source area to a factor of about 2-5 further away. The spreads due to meteorology and emission scenarios were of similar magnitude. Considering the ratio of the 50th percentiles of the two models, the spread varied by a factor of about 1-9, indicating that uncertainties arising from the formulation of the dispersion model could be as important or even larger than those associated with meteorology and emissions. Thus, it is recommended to include the uncertainty originating from the choice of the dispersion model into the overall uncertainty of short-term prediction of the dispersion of radionuclides and to exploit this further by generating an ensemble of several dispersion models.

Consequences for Norway from a hypothetical accident at the Sellafield reprocessing plant: Atmospheric transport of radionuclides.

The potential consequences for Norway should a nuclear accident at the Sellafield nuclear site occur, have been of concern for Norwegian authorities for several decades. Meteorological data from a 33-year period and the dispersion model 'SNAP' were used to evaluate meteorological conditions for which atmospheric transport of radionuclides from Sellafield to Norway would lead to the most severe impacts. The worst-case meteorological scenario for Norway, was found on 25th June 1989 for a low elevation (0-800 m) release and on 29th June 2001 for a higher elevation (800-1600 m) release. In both cases the western part of Norway was most affected. In general, the probability for depositions (>10 Bq/m2 of 137Cs) increased about 40% during the autumn and winter compared to the spring and summer months. An influence of climate change on the depositions was analysed, but not verified. Results from a number of simulations were also compared to identify how factors such as radioactive particle characteristics and initial release conditions could affect the predicted radionuclide deposition. The impact on predicted total depositions as well as hot-spot depositions by varying particle density and size as well as release elevation in worst-case scenario simulations amounted to about 40%-50%.

Intravenous injections of cobalt reduce fatty acid desaturation products in milk and blood of lactating cows.

The objective of this study was to determine whether intravenous infusion of Co affects levels of fatty acid desaturation products in bovine milk. Six cows were assigned to two replicated 3 × 3 Latin squares with 14-day periods. Treatment occurred on days 1 to 5 and depuration occurred on days 6-14. Two treatments were tested, the first consisting of per os supplementation of 3.5 g Co daily in the form of Co acetate and the second consisting of intravenous injection of 175 mg Co daily in the form of Co acetate diluted in saline solution. The third treatment was a control. Both Co treatments decreased cis-9 18:1 levels from approximately 18 to 14 g/100 g fatty acids, and increased 18:0 levels from 11 to 17 g/100 g fatty acids in milk fat (p < 0.001). The proportions of cis-9 10:1, cis-9 12:1, cis-9 14:1, cis-9 16:1 and cis-9 17:1 decreased (p < 0.001), whereas 17:0 and trans-11 18:1 increased (p < 0.001). In blood plasma, levels of cis (6,9,12) 18:3 (p < 0.001) and cis (8,11,14,17) 20:4 (p = 0.008) decreased after both the Co treatments. It is concluded that intravenous supply of Co reduces levels of fatty acid desaturation products in both bovine milk and blood.

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.

Validation of a fuel particle dissolution model with samples from the Red Forest within the Chernobyl exclusion zone.

The contamination in the near exclusion zone of the Chernobyl nuclear power plant (ChNPP) with 90Sr, 238-240Pu and 241Am is associated with irradiated nuclear fuel particles. Fit for purpose models enabling long term prediction of mobility and bioavailability of particle-associated radionuclides are crucial for radiation protection of humans and the environment, as well as for planning of remediation measures and future land use. In the present work, a dynamic fuel particle dissolution model developed in 1999-2002 is described and validated using data based on sampling in 2015. The model is based on the characterization of the radionuclide source term of the waste in a shallow sub-surface radioactive waste storage, trench #22, in the Chernobyl Pilot Site (CPS) located in the Red Forest, 2.5 km west of the ChNPP, as well as the description of physical and chemical properties of the fuel particles and subsequent radionuclide leaching into the soil solution. Transformation rate constants of the fuel particle dissolution model related to topsoil, radioactive waste trench and submerged materials, and drained cooling pond sediments, should largely control the mobility and bioavailability of radionuclides (e.g., solubility in the soil, migration to groundwater and transfer to plants). The predicting power of the Chernobyl fuel particle dissolution model with respect to radionuclide leaching dynamics was validated using samples from the same experimental site, showing that predicted particle leaching and subsequent mobility and bioavailability were within 46 ± 3% of the observed data. Therefore, linking source- and release-scenario dependent characteristics of radioactive particles to their potential weathering can provide information that can be implemented in impact assessments models for existing contaminated areas as well as for future events.

Using a chain of models to predict health and environmental impacts in Norway from a hypothetical nuclear accident at the Sellafield site.

When a nuclear accident occurs, decision makers in the affected country/countries would need to act promptly to protect people, the environment and societal interests from harmful impacts of radioactive fallout. The decisions are usually based on a combination of model prognoses, measurements, and expert judgements within in an emergency decision support system (DSS). Large scale nuclear accidents would need predictive models for the atmospheric, terrestrial, freshwater, and marine ecosystems, for the connections between these in terms of radionuclide fluxes, and for the various exposure pathways to both humans and biota. Our study showed that eight different models and DSS modules could be linked to assess the total human and environmental consequences in Norway from a hypothetical nuclear accident, here chosen to be the Sellafield nuclear reprocessing plant. Activity concentrations and dose rates from 137Cs for both humans and the environment via various exposure routes were successfully modelled. The study showed that a release of 1% of the total inventory of 137Cs in the Highly Active Liquor Tanks at Sellafield Ltd is predicted to severely impact humans and the environment in Norway if strong winds are blowing towards the country at the time of an accidental atmospheric release. Furthermore, since the models did not have built-in uncertainty ranges when this Sellafield study was performed, investigations were conducted to identify the key factors contributing to uncertainty in various models and prioritise the ones to focus on in future research.

Radioactive particles released from different sources in the Semipalatinsk Test Site.

A total of 456 nuclear tests were performed from 1949 to 1989 at the Semipalatinsk Test Site (STS) in Kazakhstan, as part of the nuclear weapon test program of the USSR. To identify if radionuclides such as 137Cs, 90Sr, 241Am, 239+240Pu were associated with radioactive particles, soil samples were collected at selected contaminated sites (i.e. Experimental field, Excavation sites, Fallout plume sections, Background global fallout area, and Degelen Mountain) within the STS. A series of techniques have been applied to identify the size distributions of radionuclides, the prevalence of radioactive particles in soils, and the degree of leachability of particle associated radionuclides by different agents. In addition, selected particles were characterized non-destructively using digital autoradiography, environmental scanning electron microscopy (ESEM) and synchrotron radiation microscopic X-ray techniques. Radioactive particles were identified at all sites; large vitrified particles were identified at epicenters, and the size of particles decreased along the plume with distance from the epicenters. The radioactive particles identified varied in composition, size and leachability. In general, 137Cs, 241Am, 239+240Pu were strongly associated with solid phases (90-99%) in soils, while 90Sr exhibited much greater variability. The fraction of 90Sr present in exchangeable forms was low close to epicenters, while the extractability increased along the plume as the particle size distribution decreased. The results suggest that at least four different types of radioactive particles are present at STS: 1) Relatively large spherical particles with a shiny glazed, melted surface with internal porous structure, and surface layers enriched in transuranic elements, identified at epicenters of detonations, 2) Vitrified irregular particles probably originating from debris of nuclear device with interactions from soil components, also identified at epicenters of detonations, 3) Particles with visually unchanged structure, containing micro-inclusions of fissile materials associated with soil components, also identified at epicenters; 4) Particles with amorphous structures associated with underground detonations, identified in soil in the vicinity of the entrance of the detonation tunnels at the Degelen Mountain. These were probably formed by secondary mechanisms due to sorption and fixation of radionuclides. Thus, the present work shows that the STS should be considered an important observatory site to link particle characteristics to specific sources and to release conditions as well as to ecosystem transfer of particle associated radionuclides.

Why is the multiple stressor concept of relevance to radioecology?

Purpose: A number of nuclear and radiological sources have contributed or are still contributing to the release of a series of stressors such as radionuclides in combination with trace metals and even organic chemicals. To assess the impact of mixed contamination, a limited number of stressors are usually evaluated one by one. We have therefore evaluated the benefit of using the multiple stressor concept focusing on key topics within radioecology such as the source term and deposition, ecosystem interactions and exposure, biological uptake and effects including adverse outcome pathways (AOPs), as a basis for assessing impact and risk. Materials and methods: We have extracted information from highly relevant scientific articles (e.g. Web of Science) describing multiple stressor exposure experiments where at least one stressor is ionizing radioactivity such as low dose gamma radiation or radionuclides (e.g. fission or activation products; uranium and daughter nuclides). In addition, experiences obtained during recent years at the author´s laboratories are included in the discussions, especially when it comes to speciation issues, combined effects, risk estimates, and AOPs. Results: The multiple stressor concept is not only related to the total concentration of a series of radionuclides and other stressors released from one source or from different sources, but also related to the presence of different physico-chemical forms of individual radionuclides. Due to interactions, the ecosystem transfer to biota is dynamic, and the application of toxicokinetics and toxicodynamics considerations seems most useful. Although there is a limited number of articles dealing with multiple stressors in which ionizing radiation is included as one of the stressors, deviation from concentration (dose) additive responses should probably be expected, especially under field conditions where additional abiotic as well as biotic interactions take place Conclusions: Following severe nuclear events, releases can be described as a massive multiple stressor exposure containing radionuclides combined with other stressors. Thus, advanced characterization technologies are needed for parameterization of the mixed stressor source term as input to ecosystem transport, dose, and impact models. To reduce uncertainties in assessments of these complex exposures, advanced technologies and computational efforts to link internal distributions to responses are also needed to understand how multiple stressor exposure could affect toxicokinetics and toxicodynamics, and why combined exposures could depart from additivity along the source-adverse outcome continuum.

A framework for exposure characterization and gamma dosimetry at the NMBU FIGARO irradiation facility.

PURPOSE: The FIGARO low dose 60Co gamma irradiation facility at the Norwegian University of Life Sciences, Ås, Norway, is dedicated to the study of effects on living organisms from acute or chronic ionizing radiation exposures, either alone or in combination with other stressors such as UV radiation, metals or radionuclides. Here, we present a framework of working guidelines and computer software for characterization of absorbed dose rates and accumulated doses to organisms exposed within the continuous gamma field at FIGARO. The aims of the framework are to ensure gamma exposures are well characterized, that results from exposures are correctly interpreted in terms of absorbed dose rates and accumulated doses, and that sufficient information is available so that exposures can be reproduced later or at other facilities. METHODS: The software of the framework includes a Geant4 application for Monte Carlo radiation transport simulations and tools for dose planning, recording and reporting. The working guidelines are prepared for expert users who provide simulated, calculated or estimated absorbed dose rates and for regular users who conduct exposure experiments and are responsible for record keeping. To demonstrate the developed framework, we use a case study where 14 freshwater microcosms are exposed to four levels of gamma dose rates at FIGARO. CONCLUSION: The framework guides users towards good dosimetry practices. Lessons learned could be transferable to other gamma irradiation facilities.

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.

Multiple stressor effects of radiation and metals in salmon (Salmo salar).

These experiments were designed to look at the cellular effects in key organs in Atlantic salmon (Salmo salar) after exposure in vivo to radiation and subtoxic levels of aluminum (Al) and cadmium (Cd), alone or in combination. Salmon (25g) were exposed to a single 0.5Gy dose of gamma-irradiation in water containing Cd, Al or Cd+Al. Three fish per group were sacrificed after 1h and the liver, pronephros, fin and gill of each was dissected. Small explants of each tissue were set up. After 2 days, the culture medium was harvested and filtered then placed on a reporter cell line for determination of stress signal activity (bystander effects). Radiation in combination with Cd and/or Al, caused bystander effects in tissues harvested from in vivo exposed salmon. The effects vary between different organs and are not consistently additive or synergistic for a given treatment. Tissue type appears to be critical. Liver cultures produce a toxic factor which is lethal to reporter cells, and therefore no liver data could be obtained. It is hoped that this stress signal response will prove to be a useful indicator of environmental stress in species inhabiting aquatic ecosystems.

No Fukushima Dai-ichi derived plutonium signal in marine sediments collected 1.5-57km from the reactors.

Based on AMS analysis, it is shown that no Pu signals from the Fukushima accident could be discerned in marine sediments collected 1.5-57km away from the Fukushima Da-ichi power plant (FDNPP), which were clearly influenced by accident-derived radiocesium. The 240Pu/239Pu atom ratios (0.21-0.28) were significantly higher than terrestrial global fallout (0.182 ± 0.005), but still in agreement with pre-FDNPP accident baseline data for Pu in near coastal seawaters influenced by global fallout and long-range transport of Pu from the Pacific Proving Grounds.

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.

Retention of radioactive particles and associated effects in the filter-feeding marine mollusc Mytilus edulis.

Radioactive particles are aggregates of radioactive atoms that may contain significant activity concentrations. They have been released into the environment from nuclear weapons tests, and from accidents and effluents associated with the nuclear fuel cycle. Aquatic filter-feeders can capture and potentially retain radioactive particles, which could then provide concentrated doses to nearby tissues. This study experimentally investigated the retention and effects of radioactive particles in the blue mussel, Mytilus edulis. Spent fuel particles originating from the Dounreay nuclear establishment, and collected in the field, comprised a U and Al alloy containing fission products such as (137)Cs and (90)Sr/(90)Y. Particles were introduced into mussels in suspension with plankton-food or through implantation in the extrapallial cavity. Of the particles introduced with food, 37% were retained for 70 h, and were found on the siphon or gills, with the notable exception of one particle that was ingested and found in the stomach. Particles not retained seemed to have been actively rejected and expelled by the mussels. The largest and most radioactive particle (estimated dose rate 3.18 ± 0.06 Gyh(-1)) induced a significant increase in Comet tail-DNA %. In one case this particle caused a large white mark (suggesting necrosis) in the mantle tissue with a simultaneous increase in micronucleus frequency observed in the haemolymph collected from the muscle, implying that non-targeted effects of radiation were induced by radiation from the retained particle. White marks found in the tissue were attributed to ionising radiation and physical irritation. The results indicate that current methods used for risk assessment, based upon the absorbed dose equivalent limit and estimating the "no-effect dose" are inadequate for radioactive particle exposures. Knowledge is lacking about the ecological implications of radioactive particles released into the environment, for example potential recycling within a population, or trophic transfer in the food chain.

Remobilisation of 109Cd, 65Zn and 54Mn from freshwater-labelled river sediments when mixed with seawater.

A major fraction of trace metals transported by rivers is associated with sediments, especially during flooding, when erosion and resuspension increase sediment loads. Upon contact with seawater in estuaries, changes in ionic strength and pH may remobilise trace metals from sediment surfaces into more bioavailable forms. The objective of the present work was to investigate time-dependent interactions between trace metals and freshwater sediments and their potential remobilisation upon contact with seawater. Two river sediments (one organic and one inorganic) were labelled with 109Cd2+, 65Zn2+ and 54Mn2+ radioactive tracers for periods up to 6 months. Sorption of tracers occurred rapidly (> or = 80% sorption, < 1 h), followed by a slower approach to pseudoequilibrium. Kd(6 months) were estimated as 460, 480 and 2200 ml/g (inorganic sediment) compared to 5300, 4000 and 1200 ml/g (organic sediment) for 109Cd, 65Zn and 54Mn, respectively. Remobilisation of tracers from labelled sediments was studied using sequential extractions. Artificial seawater extracts simulated an estuarine environment. Subsequent extractions provided information about more strongly sorbed tracer fractions within sediments. Remobilisation of 109Cd by seawater was significant (> 65%) and least affected by sediment type or freshwater labelling time. Redistribution of Cd to strongly bound phases was minimal (4% and 1% of 109Cd in strongly oxidisable fractions). Seawater remobilisation of 65Zn was significantly greater from the organic sediment (54%) compared to the inorganic sediment (8%), where a large fraction of 65Zn (14%) became irreversibly bound. Similarly, more 54Mn was remobilised by seawater from the organic sediment than the inorganic sediment (66% and 3% remobilised, respectively), i.e., 54Mn became more strongly bound in the inorganic sediment. A simple three-box model, based on first-order differential equations, was used to describe the interaction between tracers in spiked freshwater and two operationally defined sediment fractions ("seawater exchangeable" and "seawater unexchangeable") up to 6 months of freshwater labelling. Model simulations were fitted to experiment data and apparent rate constants were calculated using numerical optimisation methods. Sorption ratios from modelling data (i.e., k1/k2) were greater for organic compared to inorganic sediments, while fixation ratios were higher in inorganic sediments. In conclusion, trace metals can be remobilised from sediments on contact with seawater in estuaries. High organic content in sediments increased initial sorption of tracers but inhibited redistribution to more strongly bound fractions over time, resulting in greater remobilisation of tracers when in contact with seawater.

Mobility of dichlorprop in the soil-water system as a function of different environmental factors. I. A batch experiment.

Batch experiments were conducted to study the mobility of 14C-labelled dichlorprop in different soil types. Soils rich in organic carbon showed high sorption capacity compared to sand soil with low content of organic C. Soil to soil variations decreased when corrected for different content of organic C (Kd normalized to Koc). Data obtained in batch experiments fit into linear as well as Freundlich sorption isotherms (17 degrees C). Desorption of [14C]dichlorprop in the soil-water system increased with pH. A significant amount of dichlorprop may be considered as 'non-available' in soils with high organic C, even at relatively high pH-values. The octanol/water partitioning coefficient (Kow) for dichlorprop was inversely related to pH. In the pH range 4-7, the Kow-value varied from 114 to 0.6. The relationship between Koc and pH was similar to the relationship between Kow and pH and the data fitted the following equation: log Koc = 0.5 log Kow + 0.2 (r2 = 0.986).