Cs,Pu and Am in bottom sediments and surface water of Lake Päijänne,Finland

The concentrations and vertical distribution of ^239,240Pu, ²⁴¹Am and ¹³⁷Cs in the bottom sediments and water samples of Lake Päijänne were investigated. This lake is important, since the Päijänne area received a significant deposition from the Chernobyl fallout. Furthermore Lake Päijänne is the raw water source for the Helsinki metropolitan area. In addition no previous data on the distribution of plutonium and americium in the sediment profiles of Lake Päijänne exist. Only data covering the surface layer (0–1 cm) of the sediments are previously available. In the sediments the average total activities were 45 ± 15 Bq/m² and 20 ± 7 Bq/m² for ^239,240Pu and ²⁴¹Am, respectively. The average ²⁴¹Am/^239,240Pu ratio was 0.45 ± 0.14. The ²⁴¹Am/^239,240Pu ratio is lowest in the surface layer of the sediments and increases as a function of depth. The ²³⁸Pu/^239,240Pu ratio of the sediment samples varied between 0.012 ± 0.025 and 0.162 ± 0.079, decreasing as a function of depth. The average activity in water was 4.9 ± 0.9 mBq/m³ and 4.1 ± 0.2 mBq/m³ for ^239,240Pu and ²⁴¹Am, respectively. The ²⁴¹Am/^239,240Pu ratio of water samples was 0.82 ± 0.17. ^239,240Pu originating from the Chernobyl fallout calculated from the average total activities covers approximately 1.95 ± 0.01% of the total ^239,240Pu activity in the bottom sediments. The average total ¹³⁷Cs activity of sediment profiles was 100 ± 15 kBq/m² and 19.3 ± 1.4 Bq/m³ in water samples.     

The distribution and inventory of fallout plutonium in sediments of the Ligurian Sea near La Spezia,Italy

Pu concentrations in surface sediments of the Ligurian Sea are about ten times higher than in adjacent river sediments and are highly correlated with sediment porosities. The integrated inventory of ^239,240Pu in a sediment core is calculated to be 3·5 mCi km^?2, nearly twice the average input from fallout at these latitudes, apparently because Pu is removed from seawater by particle scavenging.The sedimentation rate is calculated from the depth of the ^239,240Pu maximum to be 0·52 ± 0·06 cmy^?1.     

238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in soils around nuclear research centre Rez, near Prague

Forty-four soil samples were taken around the nuclear research centre Rez, near Prague. The mean activity concentrations of 238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in uncultivated soil were 0.010, 0.26, 0.12, 2.7 and 23 Bq.kg(-1), respectively. Contents of radionuclides in cultivated soil were lower and in forest soil higher than in uncultivated soil. The mean activity ratios of 238Pu/239,240Pu, 241Am/239,240Pu, 90Sr/239,240Pu and 239,240Pu/137Cs in uncultivated soil were 0.041, 0.47, 10.9 and 0.013, respectively. The mean activity ratios in cultivated and forest soils were close to the values given above. It follows from the results that the source of 239,240Pu, 90Sr and 137Cs in the studied area is deposition from atmospheric nuclear tests, in the case of 137Cs also deposition from Chernobyl accident. The contribution of the research centre effluents was not proved for these radionuclides. Increased activity ratio of 241Am/239,240Pu indicates the presence of 241Am in the soils studied emanating from sources other than nuclear tests. Uniform distribution of the 241Am/239,240Pu activity ratio around the nuclear research centre and the absence of an area with evidently higher activity ratio, including at sites lying in the main wind direction, suggest that the additional activity of 241Am does not originate from the nuclear research centre. The additional source might be the deposition following the Chernobyl accident.     

Transfer of 241Am and 237Pu from euphausiid moults to a carbonate-rich marine sediment

Concentrations of ²⁴¹Am and ²³⁷Pu adsorbed onto moulted exoskeletons from the euphausiid Megancytiphanes norvegica decreased exponentially with 50% retention times of 3–7 d when moults were incubated in filtered seawater with small amounts of a carbonate-rich sediment. Over 95% of sediment weight was present as < 43 μm silt particles and 91 ± 4% of radioactivity lost from moults was recovered in this size fraction. Adsorption of both actinides (atoms μm⁻²) was greatest in the medium-fine sand fraction which had the highest carbonate content. These particles constituted <0·4% of total sediment dry weight but their reactivity (atoms μm⁻² surface: atoms μm⁻³ in solution) was 10³–10⁴ times higher than similar quotients for <43 μm particles. The enrichment shows that non-homogeneous distributions may arise between particle types when actinides such as ²⁴¹Am and ²³⁷Pu sorbed to surfaces of organic particles are transferred to sediments.     

Americium,plutonium and uranium contamination and speciation in well waters,streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site,Kazakhstan

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel′kem 1 and Tel′kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that ²⁴¹Am, ^239,240Pu and ²³⁸U concentrations in well waters within the study area are in the range 0.04–87 mBq dm⁻³, 0.7–99 mBq dm⁻³, and 74–213 mBq dm⁻³, respectively, and for ²⁴¹Am and ^239,240Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01 mBq dm⁻³, 0.08 mBq dm⁻³ and 0.32 mBq dm⁻³ for ²⁴¹Am, ^239,240Pu and ²³⁸U, respectively. The ²³⁵U/²³⁸U isotopic ratio in almost all well and stream waters is slightly elevated above the ‘best estimate’ value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53–85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11–42 μSv (mean 21 μSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel′kem explosions.     

Plutonium and americium in arctic waters,the North Sea and Scottish and Irish coastal zones

Plutonium and americium have been measured in surface waters of the Greenland and Barents Seas and in the northern North Sea from 1980 through 1984. Measurements in water and biota, Fucus, Mytilus and Patella, were carried out in North-English and Scottish waters in 1982 and Fucus samples were collected from the Irish coast in 1983. Fallout is found to dominate as a source of ^239+240Pu north of latitude 65°N, while for ²³⁸Pu a substantial fraction originates from European nuclear fuel reprocessing facilities. The ²³⁸Pu/^239+240Pu isotope ratio provides clear evidence of the transport of effluent plutonium from the latter to Spitsbergen waters. Fallout plutonium in Arctic waters has a residence time of the order of several years, while for Pu from Sellafield we estimate mean residence times of 11–15 months in Scottish waters and, tentatively, 1·5-3 y during transport from the North Channel (north of the Irish Sea) to Spitsbergen. ²⁴¹Am found in Arctic waters probably originates from the decay of fallout ²⁴¹Pu and, like Pu, tentatively has a residence time of the order of several years. Americium from Sellafield has an estimated mean residence time of 4–6 months in Scottish waters.     

A pore water study of plutonium in a seasonally anoxic lake

Data are presented here on the distribution of ^239,240Pu in the pore waters of two cores taken from a seasonally anoxic lake. The pore water ^239,240Pu profile exhibits a subsurface activity maximum of 230 ± 30 μBqkg^?1 in the 3–6 cm interval in June, as compared to an activity of 5 ± 3 μBqkg^?1 in the overlying water. The pore water ^239,240Pu profile in June follows the solid phase distribution pattern of ^239,240Pu and also the pore water distributions of Fe and Mn. Under more reducing conditions in August, pore water ^239,240Pu activities drop off to undetectable levels at all depths. This rapid change in the pore water ^239,240Pu activity reflects the dynamic nature of Pu diagenesis in these sediments. Potential diffusional fluxes of ^239,240Pu into the lake's hypolimnion in June are calculated to be on the order of 2·5 μBq cm^?2y^?1. This flux would not be significant in altering the solid phase ^239,240Pu inventory (2·8 × 10⁴μBqcm^?2).     

Aspects of the uptake of radionuclides by sheep grazing on an estuarine saltmarsh. 2. Radionuclides in sheep tissues

The transfer ¹³⁷Cs, ²³⁸Pu, ^239/240Pu and ²⁴¹Am to sheep which graze a saltmarsh in the Esk estuary, 7 km south of the sellafield reprocessing plant in west Cumbria (UK), has been estimated.The concentrations of gamma-emitting radionuclides and of ²³⁸Pu, ^239/240Pu and ²⁴¹Am were measured in liver, lung, muscle, kidney and bone from saltmarsh ewes and lambs. ¹³⁷Cs concentrations in the soft tissues were similar in liver, lung and muscle but were consistently higher in kidney and much lower in bone. The highest concentration of the transuranics was found in liver.Transfer coefficients and concentration factors were calculated for both ewes and lambs. The concentration of ¹³⁷Cs in the tissues of 5-month old lambs was higher than in those of their mothers. Therefore, a higher transfer coefficient was obtained for lamb muscle (1·8 × 10^?1 d kg^?1) than for ewe muscle (6·4 × 10^?2 d kg^?1). Concentration factors were consistently higher for ¹³⁷Cs than for the transuranics.     

Rapid remobilisation of plutonium from estuarine sediments

Plutonium remobilisation experiments, using contaminated Esk Estuary sediments and uncontaminated River Esk and North Sea waters, have successfully reproduced the observed non-conservative behaviour of dissolved Pu in the Esk Estuary, Cumbria, UK. Remobilisation is greatest at low salinites (<4%) and, under these conditions, Pu(III, IV) and Pu(V, VI) are released into solution in similar absolute amounts. The remobilisation process appears to be associated with a rapid (equilibrium achieved in 15 min) exchange reaction involving competition between Pu species, protons and major cations for the available surface sites. The experimental results show a systematic variation in distribution coefficients (i.e. K_d) for total Pu (7·2 × 10⁴−4·1 × 10⁶), Pu(III, IV) (1·0 × 10⁵−5·8 × 10⁶) and Pu(V, VI) (6·4 × 10³−5·5 × 10⁵).     

Anomalous concentrations of atmospheric plutonium-238 over Paris

Analysis of monthly rain samples collected in Paris reveals that ²³⁸Pu/ ^239,240Pu activity ratios, usually about 0·04, the fallout value, rose suddenly to 25 in October 1982. Abnormal ratios continued to be observed during the following months. Excess ²³⁸Pu from atmospheric nuclear tests can be eliminated as a possible cause. No correlation was found either with identified satellite re-entries or with atmospheric radioactive anomalies already detected in Northern Europe prior to the Chernobyl accident. Different potential industrial sources are discussed here, but the authors remain unable to identify the origin of the abnormally high ratio. This study shows that a careful investigation of ²³⁸Pu fallout is needed if environmental processes are to be traced via plutonium activity ratios.     

Deposition and distribution of Chernobyl fallout fission products and actinides in a Russian soil profile

In this article the distribution of fission products and actinides in a soil profile from Novo Bobovicky in Russia, which was contaminated due to the Chernobyl nuclear power plant accident, is described. The ground deposition of long-lived fission products determined by gamma-spectrometry was (recalculated to 26 April 1986) 1600 kBq (137)Cs/m(2), 900 kBq (134)Cs/m(2) and 60 kBq (125)Sb/m(2). Of these radionuclides (137)Cs shows the dominating activity at the present time. After 6.5 years 90% of the Cs and Sb activity was contained in the upper 4 cm. A (239,240)Pu ground deposition of 77.4+/-8.0 Bq/m(2) was determined by alpha-spectrometry. The (238)Pu/(239,240)Pu activity ratio of 0.30+/-0.03 and (241)Pu/(239,240)Pu activity ratio of 115+/-14 (in 1986) measured in the soil profile, indicates that the analysed Pu originates mainly from the Chernobyl accident. The average (234)U/(238)U activity ratio of 1.06+/-0.29 indicates that the uranium in this soil is dominated by naturally occurring uranium.The alpha- and beta-autoradiography revealed that the activity is mainly present in particulate form. It could further be observed that the spots containing alpha- or beta-activity originated from different particles. A comparison of alpha-autoradiography with the bulk Pu and Am activity showed that 92% of the alpha-activity was present as clearly detectable alpha-spots.The beta-active particles, located by beta-autoradiography were correlated with gamma-spectrometric measurements and contained only (137)Cs. These hot spots ranged from 0.02 to 0.15 Bq.It could be concluded that the vertical transport of (137)Cs and fuel fragments occurs mainly by movement of particles through the soil. It could also be concluded that the fuel fragments found, in this soil were depleted in respect to Cs, Sb and Eu.Comparison of the analysed (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu ratios with the ratios calculated with ORIGEN-S code gave an estimate of the average burn-up of the fuel particles to be in the range of 11-12 GWd/tU.The results presented in this article are valid for this single soil profile and should not be generalised unless validated in a more rigorous study of a larger number of soil profiles.     

Sources and distributions of Cs, Pu, Pu radionuclides in the north-western Barents Sea

Sediment deposits are the ultimate sink for anthropogenic radionuclides entering the marine environment. The major sources of anthropogenic radionuclides to the Barents Sea are fallout from nuclear weapons tests, long range transport from other seas, and river and non-point freshwater supplies. In this study we investigated activity concentrations, ratios, and inventories of the anthropogenic radionuclides, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu in dated sediment cores collected along a north-south transect in the northwestern Barents Sea. The data were used to evaluate the influence of different sources on the derived spatial and temporal patterns of anthropogenic radionuclides in seafloor sediment deposits. Activity concentrations of ¹³⁷Cs ranged from <0.1 Bq/kg to 10.5 Bq/kg while ^239,240Pu ranged from <0.01 Bq/kg to 2.74 Bq/kg and ²³⁸Pu activity concentrations ranged from <0.01 Bq/kg to 0.22 Bq/kg. Total inventories of ¹³⁷Cs ranged from 29.5 ± 1.5 Bq/m² to 152.7 ± 5.6 Bq/m² and for ^239,240Pu inventories (6 sediment layers only) ranged from 9.5 ± 0.3 Bq/m² to 29.7 ± 0.4 Bq/m². Source contributions varied among stations and between the investigated radionuclides. The ²³⁸Pu/^239,240Pu ratios up to 0.18 indicate discharges from nuclear fuel reprocessing plants as a main contributor of plutonium. Based on ²³⁸Pu/^239,240Pu ratio, it was calculated that up to 19-27% of plutonium is supplied from sources other than atmospheric global fallout. Taking into account Atlantic current flow trajectories and that both activity concentrations and inventories of plutonium negatively correlate with latitude, Sellafield is a major source for the Barents Sea. Concentrations and inventories of ¹³⁷Cs correlate positively with latitude and negatively with distance from the Svalbard archipelago. The ¹³⁷Cs concentrations are highest in an area of intensive melting of sea ice formed along the Siberian coast. Thus, sea ice and supplies from Svalbard may be important source of ¹³⁷Cs to the Barents Sea seafloor.     

Time pattern of off-site plutonium deposition from rocky flats plant by lake sediment analyses

A sediment core from a lake downwind of the Rocky Flats Plant, where nuclear weapons components are produced, was used to reconstruct a time pattern of off-site plutonium deposition. Core sections were dated by analyses of ¹³⁷Cs, ^239,240Pu, ²³⁸Pu, and ²⁴¹Am fallout from nuclear testing and ²³⁸Pu fallout from a satellite failure. A peak in transuranic concentrations occurred in late 1969 which was attributable to the Plant. This was confirmed by mass isotopic analysis of plutonium isotopes in selected core segments where the global fallout and Plant contributions could be differentiated. The 18 nCi ^239,240Pu per m² from the Plant that had accumulated in the sediment is reasonable when compared to soil analyses.     

Environmental radioactivity around tokai-works after the reactor accident at chernobyl

Following the reactor accident at Chernobyl, environmental samples of air, rain water and agricultural and marine products were collected and analyzed by gamma- and alpha-spectrometry. The highest concentrations of ¹³¹I in the environmental samples were as follows: 1·0×⁻¹ Bqm⁻³ (aerosol-associated in air); 3·0×10⁻¹ Bqm⁻³ (gaseous in air); 2·1×10² bq kg⁻¹ (plants); 1·4×10¹ Bq litre⁻¹ (milk). Other nuclides such as ⁹⁵Zr, ⁹⁵Nb, ¹⁰³Ru, ¹⁰⁶Ru, ¹²⁵Sb, ^129mTe, ¹³²I/¹³²Te, ¹³⁴Cs, ¹³⁷Cs, ¹⁴⁰Ba/¹⁴⁰La, ¹⁴¹Ce and ¹⁴⁴Ce were also observed in various environmental samples. ^110mAg was only detected in marine products such as cephalopoda and shellfish, ^239,240Pu and ²⁴¹Am originating from the accident were not identified.Based on the monitoring results at one dairy farm, we have derived an equation to model the transport of ¹³¹I from pasture grass to milk. This equation was then applied to the data from two other farms around Tokai-Works and the calculated ¹³¹I activities in milk were compared with those measured. The equation shows good predictive capabilities for quantification of the peak concentrations of ¹³¹I in milk but underestimates longer-term activities.     

Plutonium isotopes in surface air of Prague in 1986–2006

Monitoring of ^239,240Pu in surface air of Prague started in 1986 in connection with the Chernobyl accident. Measurable activities of 10–28 μBq m⁻³ were found from 29 April 1986 to 5 May 1986. In the most of the monitoring periods of 1987–1996, activities of ^239,240Pu in air were not measurable. Positive values for ^239,240Pu and ²³⁸Pu in air could be obtained after installation of an aerosol sampler with higher flow-rate in 1997. Activity concentrations of ^239,240Pu and ²³⁸Pu in Prague air in the most of quarters of 1997–2006 were in the range 0.53–5.06 and <0.16–1.10 nBq m⁻³, respectively. Seasonal fluctuations can be found in content of ^239,240Pu in air. Activity ratios of ²³⁸Pu/^239,240Pu in air are higher than those in top soil, so it can be supposed that ²³⁸Pu is coming to air of Prague also from other sources than resuspension of fallout from atmospheric nuclear tests.     

239,240Pu, 241Am and 232Th in lakes: The effects of seasonal anoxia

A pond which undergoes seasonal anoxia as a result of thermal stratification was studied to assess the possible release of actinide elements from anoxic sediments to the pond waters. Concentration profiles of ^239,240Pu, ²⁴¹Am, ²³²Th, iron and manganese in the water column show significant increases in concentration for all elements in the anoxic deep waters. However, calculated total inventories of the elements in the pond water indicate no apparent input of actinide elements to the system during summer stratification. Similar inventory calculations for ^239,240Pu in a previously studied system support the results of this study. The lack of a significant increase in pond inventories of actinide elements coupled with a lack of correspondence of concentration profiles of the actinide elements to the seasonal Fe and Mn concentrations profiles argues that the increases in concentrations observed for these elements in anoxic bottom waters result from the downward transport of material already in the water column rather than release from the sediments.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part I: external gamma radiation and radionuclide concentrations in intertidal sediments, soil and air

Previous projects specifically aimed at performing radiological assessments in the vicinity of North Wales, investigating the presence and transfer of radionuclides from sea to land, were in 1986 and 1989. Since then, changes have occurred in the radioactive discharges from the British Nuclear Group Sellafield site. Annual discharges of (137)Cs, (238)Pu, (239,340)Pu and (241)Am have decreased markedly whereas, up until recent years, discharges of (99)Tc have increased. It is therefore desirable to quantify current transfer processes of radionuclides in the North Wales region and thus provide an update on 15-year-old studies. A field campaign was conducted collecting soil samples from 10 inland transects and air particulates on air filters from three High Volume Air Samplers, along the northern coast of Wales at Amlwch, Bangor Pier and Flint. Complementary field data relating to external gamma dose rates were collected at the soil sites. The field data generated for (137)Cs, (238)Pu, (239,340)Pu and (241)Am were consistent with what had been reported 15 years previously. Therefore, there has been no increase in the supply of these Sellafield-derived radionuclides to the terrestrial environment of the North Wales coast. The (99)Tc data in sediments were consistent with reported values within annual monitoring programmes, however, a relatively high activity concentration was measured in one sediment sample. This site was further investigated to determine the reason why such a high value was found. At present there is no clear evidence as to why this elevated concentration should be present, but the role of seaweed and its capacity in accumulating (99)Tc and transferring it to sediment is of interest. The analysis of the field samples for (99)Tc, (137)Cs, (238)Pu, (239,240)Pu and (241)Am has provided a data set that can be used for the modelling of the transfer of anthropogenic radionuclides from sea to land and its subsequent radiological implications and is reported in an accompanying paper.     

Accumulation of anthropogenic radionuclides in cryoconites on Alpine glaciers

Cryoconites are airborne sediments which accumulate on the surface of glaciers. In samples of cryoconites a temperate Austrian glacier high activity concentrations of anthropogenic radionuclides were found, which stem from global and Chernobyl fallouts. Radionuclides identified were ¹³⁷Cs, ¹³⁴Cs, ²³⁸Pu, ^239+240Pu, ⁹⁰Sr, ²⁴¹Am, ⁶⁰Co, ¹⁵⁴Eu, ²⁰⁷Bi, and ¹²⁵Sb.     

Scavenging of 234Th in the Eastern Irish Sea

Measurements of the disequilibria of ²³⁴Th/²³⁸U in seawater and in suspended particulate and seabed sediment in the eastern Irish Sea reveal that the residence time of dissolved ²³⁴Th (0·5–7·7 days) is controlled by the concentration of particles in suspension (0·4–6·9 mg litre⁻¹, which reflects the rate of sediment resuspension (0·5–5·9 kg m⁻²y⁻¹). The residence time of ²³⁴Th with respect to removal to the seabed is longer (7–50 d) and is less dependent on variations in the suspended load. Anthropogenic sources of ²³⁸U contribute up to 8–15% of the water column production of ²³⁴Th. Enhanced scavenging occurs near the coast and there appears to be a net horizontal flux of ²³⁴Th within this region.     

Polonium-210 in mussels and its implications for environmental alpha-autoradiography

Alpha-autoradiographic and radiochemical studies of the distributions of transuranic nuclides in the tissues and organs of mussels collected from the vicinity of the British Nuclear Fuels plc reprocessing plant at Sellafield, Cumbria, England, appeared to require assessment also of baseline alpha-activities of natural ²¹⁰ Po levels. Results for the latter were found to be in excess of the anthropogenic activities of Pu and Am isotopes. To ensure that the levels of ²¹⁰ Po in Cumbrian mussels were not artificially enhanced by local discharges and in the absence of published data, mussels from remote British and French coastal sites were also analyzed. General similarities in ²¹⁰Po concentrations (111 to 459 Bq kg⁻¹ dry) found in mussels soft parts suggest that the ²¹⁰Po levels in the Ravenglass mussels (279 Bq kg⁻¹) are natural and largely unsupported by ²¹⁰Pb; however these levels are as much as four times greater than the present day ^239+240Pu concentrations in the same samples. As the transuranic nuclide content of Cumbrian mussels produces a major component of the local critical group radiation exposure from the Sellafield discharges, this finding places in some perspective the significance of the baseline natural radionuclide concentrations in generating total exposure of the public. More specifically, these findings severely limit the usefulness of alpha-autoradiographic studies for transuranic nuclides performed on such samples. Because of the recently lower concentrations of alpha-emitting transuranic nuclides (mainly ²³⁸Pu, ^239+240Pu and ²⁴¹Am) in the Ravenglass environment, natural ²¹⁰Po is now a major contributor to alpha-track distributions in autoradiographic studies.