Vertical distributions of 239+240Pu activities and 240Pu/239Pu atom ratios in sediment cores: implications for the sources of Pu in the Japan Sea

The vertical distributions of 239+240Pu-specific activities and 240Pu/239Pu atom ratios in sediment cores of the Japan Sea were investigated. For comparison, the 239+240Pu-specific activities and 240Pu/239Pu atom ratios in the surface layer of bottom sediments in the Sea of Okhotsk were also determined. The 239+240Pu-specific activities in the surface layer sediments varied from 0.43 to 2.65 mBq/g in the Japan Sea. The lowest value was seen in the eastern Japan Basin, while the highest value was found in a sample collected from a coastal area off Hokkaido in the northern Japan Sea. It was found that the 240Pu/239Pu atom ratios in the surface sediments for the Japanese side of the Japan Sea ranged from 0.15 to 0.22. The 240Pu/239Pu atom ratios in the surface sediments collected from the Yamato Basin and Japan Basin were typically close to the global fallout value of 0.18, but higher 240Pu/239Pu atom ratios (0.20-0.22) were seen in samples from the northern Japan Sea. Vertical profiles of 240Pu/239Pu atom ratios revealed that these atom ratios were higher than the global fallout value in the deeper layers in the sediment cores from the northern Japan Sea on the Hokkaido coast and the Yamato Basin. In addition, the sediment cores from the northern Japan Sea near the Soya Strait and in the Ishikari Estuary had a constant vertical distribution of 240Pu/239Pu atom ratios with a value around 0.20. The results obtained in this work support the hypothesis that the prevailing ocean currents transported Pu derived from the Pacific Proving Grounds to the Japan Sea, and this contributed to the general elevated Pu inventory in the Japan Sea.     

137Cs, 239+240Pu and 240Pu/239Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas

Surface seawater samples were collected along the track of the R/V Hakuho-Maru cruise (KH-96-5) from Tokyo to the Southern Ocean. The (137)Cs activities were determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas, the eastern Indian Ocean, the Bay of Bengal, the Andaman Sea, and the South China Sea. The (137)Cs activities showed a wide variation with values ranging from 1.1 Bq m(-3) in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m(-3) in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of (137)Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of (137)Cs from the surface waters were roughly estimated from the two data sets of Miyake et al. [Miyake Y, Saruhashi K, Sugimura Y, Kanazawa T, Hirose K. Contents of (137)Cs, plutonium and americium isotopes in the Southern Ocean waters. Pap Meteorol Geophys 1988;39:95-113] and this study to be 0.016 yr(-1) in the Sulu and Indonesian Seas, 0.033 yr(-1) in the Bay of Bengal and Andaman Sea, and 0.029 yr(-1) in the South China Sea. These values were much lower than that in the coastal surface water of the western Northwest Pacific Ocean. This was likely due to less horizontal and vertical mixing of water masses and less scavenging. (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were also determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas and the South China Sea. The (240)Pu/(239)Pu atom ratios ranged from 0.199+/-0.026 to 0.248+/-0.027 on average, and were significantly higher than the global stratospheric fallout ratio of 0.18. The contributions of the North Pacific Proving Grounds close-in fallout Pu were estimated to be 20% for the western North Pacific Ocean, 39% for the Sulu and Indonesian Seas and 42% for the South China Sea by using the two end-member mixing model. The higher (240)Pu/(239)Pu atom ratios could be attributed to close-in fallout Pu delivered from the Enewetak and Bikini Atolls by ocean currents of branches of the North Equatorial Current to the Southeast Asian seas.     

Distribution of 137Cs, 238Pu and 239+240 Pu in sediments of the southeastern Brazilian shelf-SW Atlantic margin

In this work levels of 137Cs, 238Pu and 239+240 Pu as well as activity ratios of anthrophogenic radionuclides in sediment samples from the southeastern Brazilian shelf are presented. Instrumental gamma spectrometry was used to determine 137Cs and alpha spectrometry to determine 238Pu and 239+240 Pu after a radiochemical procedure. The levels ranged from 0.30 to 1.79 Bq kg(-1) for 137Cs, from 15 to 150 mBq kg(-1) for 238Pu and, from 18 to 117 mBq kg(-1) for 239+240 Pu. There was a bathymetric differentiation in the radionuclides distribution. 137Cs values were generally higher in the samples collected at water depths of less than 100 m. On the other hand, plutonium isotopes exhibit higher values at greater depths. The mean ratio of 239+240 Pu/137Cs obtained was 0.112+/-0.072 which is in agreement with the value reported for the Atlantic from atmospheric fallout of nuclear explosions in the past. The 238Pu/230+240 Pu ratios varied widely (from 0.339 to 2.088) and showed the influence of the SNAP-9A accident in the 238Pu levels for this area. The main goal of this work was to present unpublished anthropogenic radionuclide levels and activity ratios related to the contamination of the southeastern Brazilian shelf.     

Plutonium isotopes in seas around the Korean Peninsula

239+240Pu concentrations and 240Pu/239Pu atom ratios in coastal seas adjacent to the Korean Peninsula were determined, during the period 1999 to 2002, to assess the current distribution and to identify sources of Pu isotopes. 239+240Pu concentrations in surface waters ranged from 3.1 to 22.3 mBq m(-3) with higher concentrations in winter than in summer. 239+240Pu concentrations in seawaters around the Korean Peninsula are greater than that in the western North Pacific. 240Pu/239Pu atom ratios ranged from 0.18 to 0.33 with an average value of 0.25+/-0.03, which is significantly higher than the global fallout average. The 240Pu/239Pu atom ratios of the 2000 m deep entire water column in the south western part of the East Sea (Sea of Japan) was comparable to that observed in waters near Bikini Atoll. The higher 240Pu/239Pu atom ratios than that of global fallout may be explained by the hypothesis that the earlier input signal of low 240Pu/239Pu atom ratio (0.18-0.19) of global fallout plutonium in seas adjacent to the Korean Peninsula is being gradually diluted by the high 240Pu/239Pu atom ratio plutonium transported from the tropical Pacific Proving Grounds via prevailing ocean current.     

Temporal record of Pu isotopes in inter-tidal sediments from the northeastern Irish Sea

A depth profile of ²³⁹Pu and ²⁴⁰Pu specific activities and isotope ratios was determined in an inter-tidal sediment core from the Esk Estuary in the northeastern Irish Sea. The study site has been impacted with plutonium through routine radionuclide discharges from the Sellafield nuclear reprocessing plant in Cumbria, NW England. A pronounced sub-surface maximum of ~ 10 kBq kg^-1 was observed for ^239 + 240Pu, corresponding to the peak in Pu discharge from Sellafield in 1973, with a decreasing trend with depth down to ~ 0.04 kBq kg^-1 in the deeper layers. The depth profile of ^239 + 240Pu specific activities together with results from gamma-ray spectrometry for ¹³⁷Cs and ²⁴¹Am was compared with reported releases from the Sellafield plant in order to estimate a reliable sediment chronology. The upper layers (1992 onwards) showed higher ^239 + 240Pu specific activities than would be expected from the direct input of annual Sellafield discharges, indicating that the main input of Pu is from the time-integrated contaminated mud patch of the northeastern Irish Sea. The ²⁴⁰Pu/²³⁹Pu atom ratios ranged from ~ 0.03 in the deepest layers to > 0.20 in the sub-surface layers with an activity-weighted average of 0.181. The decreasing ²⁴⁰Pu/²³⁹Pu atom ratio with depth reflects the changing nature of operations at the Sellafield plant from weapons-grade Pu production to reprocessing spent nuclear fuel with higher burn-up times in the late 1950s. In addition, recent annual ²⁴⁰Pu/²³⁹Pu atom ratios in winkles collected during 2003-2008 from three stations along the Cumbrian coastline showed no significant spatial or temporal differences with an overall average of 0.204, which supports the hypothesis of diluted Pu input from the contaminated mud patch.     

Characterization of Pu concentration and its isotopic composition in a reference fallout material

Because there is no reference material for fallout plutonium isotope monitoring, preparation of such a material is necessary for quality control of fallout radionuclides analysis for atmospheric environmental studies. In this work, we report the characterization of Pu activity and its isotopic composition in a reference fallout material prepared by the Meteorological Research Institute (MRI), Japan. This material was prepared from samples collected at 14 stations throughout Japan in 1963-1979, with reference values of ¹³⁷Cs, ⁹⁰Sr and ^239 + 240Pu activities. We analyzed the activities of ^239 + 240Pu and ²⁴¹Pu, and the atom ratios of ²⁴⁰Pu/²³⁹Pu and ²⁴¹Pu/²³⁹Pu using an isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The ^239 + 240Pu activities in this fallout material using acid leaching and total digestion were 6.56 ± 0.20 mBq/g and 6.79 ± 0.16 mBq/g, respectively. Atom ratios of ²⁴⁰Pu/²³⁹Pu were 0.1915 ± 0.0030 and 0.1922 ± 0.0044, respectively. Both ²⁴⁰Pu/²³⁹Pu and ²⁴¹Pu/²³⁹Pu atom ratios were slightly higher than those of global fallout, which could be attributed to the deposition of fallout radionuclides resulting from the Chinese nuclear weapons tests conducted in the 1970s. The dominant host phases of ^239 + 240Pu were found to be organic matter-sulfides (70%) with a relative high ²⁴⁰Pu/²³⁹Pu atom ratio, and Fe-Mn oxides (19%) using a sequential extraction method.     

Radionuclide behaviour and transport in a coniferous woodland ecosystem: vegetation, invertebrates and wood mice, Apodemus sylvaticus

Activity concentrations of radionuclides (134Cs, 137Cs, 238Pu, 239 + 240Pu and 241Am) were measured in vegetation, invertebrates and wood mice, Apodemus sylvaticus, collected in Lady Wood, a coniferous woodland in the vicinity of the British Nuclear Fuels reprocessing plant at Sellafield, Cumbria, UK. Vegetation was of low diversity and biomass with activity concentrations ranging from 1 to 5 Bq kg-1 (134Cs), 0.3-0.5 Bq kg-1 (238Pu), 0.8-8 Bq kg-1 (239 + 240Pu), and 0.6-16 Bq kg-1 (241Am), dry wt. Caesium-137 activity concentrations were high compared to the reference site in Cheshire, varying between 65 and 280 Bq kg-1. Marked inter-specific and temporal differences in radionuclide activity concentrations were recorded for invertebrate populations. Caesium-137, 238Pu, 239 + 240Pu and 241Am activity concentrations in detritivorous invertebrates were consistently higher than in all other invertebrate groups reflecting contamination of the leaf litter. The activity concentrations in detritivores increased during the autumn and winter, reflecting changes in diet as food sources varied throughout the year. Activity concentrations in invertebrates caught in Lady Wood were generally an order of magnitude higher than for the reference site. Activity concentrations in wood mice varied between 7 and 150 Bq kg-1 (137Cs), 0.1-0.3 Bq kg-1 (238Pu), 0.1-0.6 Bq kg-1 (239 + 240Pu) and 0.2-0.4 Bq kg-1 (241Am). There were clear differences in the activity concentration of 137Cs (P < 0.01), 239 + 240Pu (P < 0.05) and 241Am (P < 0.05) in animals caught in Lady Wood compared to the reference site. However, the activity concentrations for 238Pu were similar at both sites, reflecting a low gastrointestinal transfer. Seasonal variation in activity concentrations was observed for 137Cs, 238Pu and 241Am. This variation is attributed to changes in the age structure of the population and diet throughout the year.     

Temporal variation of Pu/Pu atom ratio and Pu inventory in water columns of the Japan Sea

The ^239+240Pu concentrations and ²⁴⁰Pu/²³⁹Pu atom ratios were determined by alpha spectrometry and double-focusing SF-ICP-MS for seawater samples obtained in 1984 and 1993 from the Yamato and Tsushima Basins of the Japan Sea in the western North Pacific margin. The total ^239+240Pu inventories in the whole water columns were approximately doubled during the period from 1984 to 1993 in the two basins. The increasing rates were estimated to be 5.1 Bq m⁻² yr⁻¹ in the Yamato Basin and 4.2 Bq m⁻² yr⁻¹ in the Tsushima Basin and they corresponded to ~ 0.02% of the annual ^239+240Pu inflow rate into the Japan Sea through the Tsushima Strait. The mean ²⁴⁰Pu/²³⁹Pu atom ratios were ~ 0.240 and significantly higher than the mean global fallout ratio of 0.18. Furthermore, there were no temporal or spatial variations of ²⁴⁰Pu/²³⁹Pu atom ratios during this period in the Japan Sea. The total ^239+240Pu inventories originating from the close-in fallout increased from 17.6 Bq m⁻² to 34.6 Bq m⁻² in the Yamato Basin and from 20.1 Bq m⁻² to 34.6 Bq m⁻² in the Tsushima Basin; however, the relative percentage of ~ 40% from the close-in fallout was unchanged during this period. A likely mechanism for the increasing Pu inventory would be the continuous inflow of the Tsushima Current from the western North Pacific, and the removal of Pu from surface waters by scavenging onto the settling particles, followed by regeneration of Pu from the settling particles during the downward transport.     

Territory contamination with the radionuclides representing the fuel component of Chernobyl fallout

The data obtained through a series of experiments were used to specify the correlation of activities of the fuel component radionuclides of Chernobyl fallout and to create the maps of the 30-km Chernobyl zone terrestrial density of contamination with 154Eu, 238Pu, 239+240Pu and 241Am (on 01.01.2000). In the year 2000, total inventories of the fuel component radionuclides in the upper 30-cm soil layer of the 30-km Chernobyl zone in Ukraine (outside the ChNPP industrial site, excluding the activity located in the radioactive waste storages and in the cooling pond) were estimated as: 90Sr--7.7 x 10(14) Bq; 137Cs--2.8 x 10(15) Bq; 154Eu--1.4 x 10(13) Bq; 238Pu--7.2 x 10(12) Bq; 239+240Pu--1.5 x 10(13) Bq; 241Am--1.8 x 10(13) Bq. These values correspond to 0.4-0.5% of their amounts in the ChNPP unit 4 at the moment of the accident. The current estimate is 3 times lower than the previous widely-cited estimates. Inventories of the fuel component radionuclides were also estimated in other objects within the 30-km zone and outside it. This allowed more accurate data to be obtained on the magnitude of a relative release of radionuclides in the fuel particles (FP) matrix during the Chernobyl accident outside the ChNPP industrial site. It amounts to 1.5+/-0.5% of these radionuclides in the reactor, which is 2 times lower than the previous estimates. Two-thirds of the radionuclides release in the FP was deposited on the territory of Ukraine.     

Large particle flux of 239+240Pu on the continental margin of the East China Sea

Settling particles were collected from three locations in the East China Sea continental margin and analyzed for 239+240Pu. Two types of sediment traps were used, cylindrical traps and conical time-series traps. Surface sediment samples collected from five locations were also analyzed for 239+240Pu. Data from cylindrical traps showed there was a clear tendency for total mass fluxes to increase with depth at all three stations, and there was an especially large increase near the bottom. 239+240Pu concentrations in settling particles increased with depth from 1.76 mBq/g at 97-m depth to 3.0 mBq/g at 120-m depth and ranged from approximately 3 to 4 mBq/g at depths greater than 120 m. 239+240Pu concentrations collected in the near-bottom traps were approximately two times higher than those in the underlying surface sediments. Like total mass fluxes there was a clear tendency for 239+240Pu fluxes to increase with depth at every station, and the highest 239+240Pu fluxes were observed near the bottom. 239+240Pu concentrations in the time-series traps had little variation throughout the sampling period, though the total mass fluxes showed a large variation. A high variability of 239+240Pu fluxes occurred in very short period of time (1/2 day). The large fluxes of 239+240Pu might be attributed to episodic lateral transport of particles that flow down the continental slope with the nepheloid layer which was considered to be significant for 239+240Pu transport on the continental slope in the East China Sea.     

Spatial and temporal variations of plutonium isotopes (238Pu and 239,240Pu) in sediments off the Rhone River mouth (NW Mediterranean)

The dispersion and fate of the Rhone River inputs to the Gulf of Lions (Northwestern Mediterranean Sea) have been studied through the spatial and temporal distributions of plutonium isotopes in continental shelf sediments. Plutonium isotopes ((238)Pu and (239,240)Pu) are appropriate tracers to follow the dispersion of particulate matter due both to their high affinity for particles and their long half-lives. In the Rhone River valley, plutonium isotopes originate from both the weathering of the catchment basin contaminated by global atmospheric fallout, and the liquid effluents released from the Marcoule reprocessing plant since 1961. This work presents a first detailed study on (238)Pu and (239,240)Pu distributions in sediments from the Rhone prodelta to the adjacent continental shelf, since the decommissioning of Marcoule in 1997. The vertical distribution of Pu isotopes has been analysed in a 4.75 m long core sampled in 2001 at the Rhone mouth. Despite this length, plutonium is found at the last 10 cm, manifesting the high sedimentation rate of the prodeltaic area and its ability for trapping fine-grained sediments and associated contaminants. The highest (238)Pu and (239,240)Pu concentrations reached 1.26 and 5.97 Bq kg(-1) respectively and were found within the layer 280-290 cm. The (238)Pu/(239,240)Pu activity ratios (AR) demonstrated an efficient and huge trapping of the Pu isotopes derived from Marcoule. The fresh sediments, located on the top of the core, show lower plutonium activity concentrations and lower (238)Pu/(239,240)Pu ratios. This decrease is in close relation with the shut down of the Marcoule reprocessing plant in 1997. In 2001, plutonium isotopes were also analysed in 21 surface sediments located offshore and concentrations ranged from 0.03 to 0.17 Bq kg(-1) for (238)Pu and from 0.33 to 1.72 Bq kg(-1) for (239,240)Pu. The (238)Pu/(239,240)Pu AR ranged from 0.24 close to the river mouth to 0.06 southwards, indicating the decreasing influence of the Marcoule releases (global fallout AR 0.03-0.05 and Marcoule AR 0.30). This is in good agreement with the main direction spread of the Rhone River plume and the bottom current. This dataset has been compared to those obtained in the same area in 1984 and 1990 in order to follow the time trend in Pu concentrations. This comparison highlights the decrease with time in plutonium concentrations close to the Rhone River mouth, but further away this reduction is not so evident.     

Multitracer study of anthropogenic contamination records in the Camargue, Southern France

Contaminants are supplied to the coastal zone by the atmosphere, rivers and point sources like wastewaters or industrial area. Wetlands retain many of these contaminants and can be used to reconstruct sources and magnitudes of contaminant inputs. Radionuclides ((137)Cs, (210)Pb, (239)Pu and (240)Pu) and stable lead isotope ((206)Pb, (207)Pb) profiles were investigated in two cores collected in wetlands of the Rh?ne River delta, south of France (Camargue), to estimate the recent sediment accumulation rates and reconstruct the deposition of pollutants during the last century. One site was affected by storm or flood deposition from the Rh?ne river and showed the influence of Marcoule reprocessing plant releases on the plutonium isotopic ratios. The other site appears suitable for the reconstruction, even if mixing is evidenced at the surface by the radionuclides profiles. Plutonium isotopic ratios are characteristic of global fallout and the (210)Pb inventory of 4240 Bq m(-2) is approximately 30% higher than atmospheric deposit estimation. The pollutant lead inventory is 139 microg cm(-2), slightly higher than previous estimation from direct fallout. This difference can be partly due to an over-collection at this site (due to canopy cover) but also to variations with time in the deposition.     

First results on U levels in global fallout

The global fallout ²³⁶U level in soil was deduced from measurements of ²³⁶U, ^239+240Pu and ¹³⁷Cs in surface soils which are solely influenced by global fallout. A total of 12 soil cores from the depths of 0-10, 0-20 and 0-30 cm were collected at a flat forest area in Japan. Concentrations of ^239+240Pu and ²³⁸U were determined by α-particle spectrometry, while the ²³⁶U/²³⁸U ratio was measured with accelerator mass spectrometry (AMS). Consistent ²³⁶U/²³⁹Pu ratios between 0.212 and 0.253 were found. Using this ratio, the total global fallout of ²³⁶U on the earth is estimated to be as much as ca. 900 kg. This knowledge will contribute to the promotion of research on U isotopes, including ²³⁶U, for the fields of geo-resources, waste management and geochemistry.     

Solid-solution partitioning of plutonium in surface waters at the Atomic Weapons Establishment Aldermaston (UK)

The Atomic Weapons Establishment (AWE) at Aldermaston (Berkshire, UK) has provided and maintained the warheads for the UK's nuclear deterrent for more than 50 years. Whilst the site is radiologically safe, in a few locations the soil contains specific activities of plutonium (Pu) above background arising from a legacy of historic operations. Run-off water (a mixture of rainwater and groundwater) from part of the site is routed into a water management system, and after analysis and radiological assessment, released into local streams. Water and sediment samples have been collected from a number of closely spaced locations within this system to assess the solid-solution partitioning of Pu. Survey work was complemented by batch type desorption experiments to assess redissolution from 'contaminated' sediment into 'uncontaminated' water. The survey data indicate that specific activities of both dissolved and particle bound 239 + 240Pu varied by roughly two orders of magnitude, ranging from approximately 0.7 microBq kg(-1) up to approximately 44 microBq kg(-1), and approximately 1.2 Bq kg(-1) up to approximately 400 Bq kg(-1), respectively, consistent with water originating from different parts of the site. Apparent Kd values varied by an order of magnitude (from 0.7-16 x 10(6)) with an average value of 4 x 10(6). Results from the desorption experiments indicated the extent of redissolution was very small and the derived Kd's corroborated values obtained from the survey work. Kd's given here are compared with other literature values, and are the greatest reported to date. Results are also provided describing the variation in water quality parameters in shallow groundwater samples. Alkalinity values ranged from 120 to 388 mg l(-1) CaCO3 with an average value of 195 mg l(-1) CaCO3. Corresponding values for pH were 6.6-8.3 with an average of 7.5. Over half of the samples were estimated to be supersaturated with respect to calcite. It is suggested that the state of calcite saturation may be responsible for the high Pu Kd. As a consequence of the high particle reactivity, migration of Pu contamination, both within and away from the AWE Aldermaston site, is likely to be very restricted.     

Arctic Ocean sea ice drift origin derived from artificial radionuclides

Since the 1950s, nuclear weapon testing and releases from the nuclear industry have introduced anthropogenic radionuclides into the sea, and in many instances their ultimate fate are the bottom sediments. The Arctic Ocean is one of the most polluted in this respect, because, in addition to global fallout, it is impacted by regional fallout from nuclear weapon testing, and indirectly by releases from nuclear reprocessing facilities and nuclear accidents. Sea-ice formed in the shallow continental shelves incorporate sediments with variable concentrations of anthropogenic radionuclides that are transported through the Arctic Ocean and are finally released in the melting areas. In this work, we present the results of anthropogenic radionuclide analyses of sea-ice sediments (SIS) collected on five cruises from different Arctic regions and combine them with a database including prior measurements of these radionuclides in SIS. The distribution of ¹³⁷Cs and ^239,240Pu activities and the ²⁴⁰Pu/²³⁹Pu atom ratio in SIS showed geographical differences, in agreement with the two main sea ice drift patterns derived from the mean field of sea-ice motion, the Transpolar Drift and Beaufort Gyre, with the Fram Strait as the main ablation area. A direct comparison of data measured in SIS samples against those reported for the potential source regions permits identification of the regions from which sea ice incorporates sediments. The ²⁴⁰Pu/²³⁹Pu atom ratio in SIS may be used to discern the origin of sea ice from the Kara-Laptev Sea and the Alaskan shelf. However, if the ²⁴⁰Pu/²³⁹Pu atom ratio is similar to global fallout, it does not provide a unique diagnostic indicator of the source area, and in such cases, the source of SIS can be constrained with a combination of the ¹³⁷Cs and ^239,240Pu activities. Therefore, these anthropogenic radionuclides can be used in many instances to determine the geographical source area of sea-ice.     

Feasibility of using U to reconstruct close-in fallout deposition from the Hiroshima atomic bomb

The first results on the feasibility of using ²³⁶U to reconstruct the level and spatial distribution of close-in fallout deposition from the Hiroshima A-bomb are reported, coupled with the use of global fallout ¹³⁷Cs and ^239 + 240Pu. The results for global fallout ²³⁶U in soil samples (0-30 cm) from Ishikawa prefecture showed that the deposition density of ²³⁶U from the global fallout can be accurately evaluated using AMS. All deposited ²³⁶U, ¹³⁷Cs and ^239 + 240Pu appeared to have been recovered using 30-cm cores. It was also noted from the depth profiles for ²³⁶U/^239 + 240Pu and ²³⁶U/¹³⁷Cs ratios that the downward behavior of ²³⁶U in the soil was apparently similar to that of ^239 + 240Pu, while the ¹³⁷Cs was liable to be retained in upper layers compared with ²³⁶U and ^239 + 240Pu. The accumulated levels were 1.78 × 10¹³ atoms m^− 2 for ²³⁶U, 4340 Bq m^− 2 for ¹³⁷Cs and 141 Bq m^− 2 for ^239 + 240Pu. The ratios of ²³⁶U/¹³⁷Cs and ²³⁶U/^239 + 240Pu were (4.10 ± 0.12) × 10⁹ and (1.26 ± 0.04) × 10¹¹ atoms Bq^− 1, respectively. Results of ²³⁶U, ¹³⁷Cs and ^239 + 240Pu measurements for the seven soil cores (0-30 cm) from Hiroshima were discussed on the basis of ratios of ²³⁶U/¹³⁷Cs and ²³⁶U/^239 + 240Pu by comparing with those from the background area in Ishikawa, indicating that the global fallout dominates the current level of ²³⁶U accumulation in soil in the Black-rain area around Hiroshima after the Hiroshima bomb, and the contribution of the close-in fallout ²³⁶U produced by the Hiroshima A-bomb seems difficult to observe.     

Reconstructing historical radionuclide concentrations along the east coast of Ireland using a compartmental model

A mathematical model is presented that simulates the annually averaged transport of radionuclides, originating from the BNFL reprocessing plant at Sellafield, throughout the Irish Sea. The model, CUMBRIA77, represents the processes of radionuclide transport and dispersion in the marine environment and allows predictions of radionuclide concentration in various environmental media, including biota, to be made throughout the whole of the Irish Sea. In this paper we describe the use of the model to reconstruct the historical activity concentrations of 137Cs and 239+240Pu in a variety of environmental media in the western Irish Sea and along the Irish east coast back to 1950. This reconstruction exercise is of interest because only limited measurements of 137Cs and 239+240Pu activity are available prior to the 1980s. The predictions were compared to the available measured data to validate their accuracy. The results of the reconstruction indicate that activity concentrations of 137Cs in the western Irish Sea follow a similar, though slightly delayed and smoothed, profile to the discharges from the Sellafield site, with concentrations at the time of peak discharge (the mid-1970s) being around an order of magnitude higher than those measured in the 1980s and 1990s. By contrast, the concentrations of 239+240Pu at the time of peak discharges were similar to those presently measured. These differences reflect the distinct marine chemistries of the two nuclides, in particular the higher propensity of plutonium to bind to sediments leading to extended transport times. Despite these differences in behaviour the doses to Irish seafood consumers from 137Cs remain significantly higher than those from 239+240Pu.     

238Pu and 239+240Pu inventory and distribution through the lower Rhone valley terrestrial environment (Southern France)

Because of atmospheric global fallout due to thermonuclear tests performed between 1945 and 1980 and to the American SNAP 9A satellite explosion in 1964, plutonium's long-lived alpha emitter isotopes ((238)Pu, (239)Pu and (240)Pu) can be found everywhere in the environment. In the soils of the lower Rhone valley, over a surface area of approximately 11,000 km(2), existing results allow estimation of the total inventory resulting from this origin of 551 GBq as regards these radionuclides. The Marcoule Nuclear Reprocessing Plant (NRP) has been releasing (238)Pu and (239+240)Pu into the environment for over 40 years in the region and is as such a second likely source for Pu input. This article gives a global review of plutonium distribution in this particular region. It is shown that releases from Marcoule, although accounting for less than 2% of the total Pu inputs into the terrestrial environment, are responsible for localised and measurable Pu enrichments close to the facility (+2.8 GBq), and in the Rhone delta where sediments from the river settled during the past floods (+0.1 GBq). Irrigating with water from the Rhone River also allowed the transfer of approximately 3.8 GBq of (238)Pu and (239+240)Pu to the soils for the whole 1960-1998 period. These inputs, distributed over wide irrigated surface areas, do not induce significant increases of soil Pu-activity levels. In a second section, this study confirms that most of the plutonium existing in the terrestrial environment is accumulated in the soil. Less than 0.1% of the activities exist currently in the plant compartments, and the flows exported by agricultural productions are very low, although we are interested here in a French region where agriculture prevails.     

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.     

239 + 240Pu and 137Cs concentrations in fish, cephalopods, crustaceans, shellfish, and algae collected around the Japanese coast in the early 1990s

Marine organisms, i.e. fish, cephalopods, crustaceans, shellfish, and algae, were collected in the early 1990s along the Sea of Japan coast and the Japanese Pacific coast and analyzed for their 239 + 240Pu and 137Cs concentrations. The 239 + 240Pu concentrations in muscle of fish were below 0.4 mBq/kg wet wt. and the lowest among the analyzed marine organisms. Most 137Cs concentrations in muscle of fish ranged from 100 to 300 mBq/kg wet wt. Higher concentrations of 239 + 240Pu, ranging from 1.6 to 5.7 mBq/kg wet wt., were observed in viscera of cephalopods than in their muscle. The 239 + 240Pu concentrations in whole soft tissues of bivalves varied approximately one order of magnitude from 0.8 to 6.1 mBq/kg wet wt., while 137Cs concentrations had little variation, being approximately 60 mBq/kg wet wt. The 239 + 240Pu concentrations in algae had a wide variation, ranging from 1.7 to 42.3 mBq/kg wet wt., and were higher than those of the other marine organisms. No statistically significant difference in mean concentrations of 239 + 240Pu was detected among the whole soft tissues of bivalves, viscera of cephalopods and crustaceans, and whole bodies of cephalopods and crustaceans within the 95% confidence limit. The mean concentrations of 137Cs became higher in the order, cephalopods and crustaceans and bivalves, algae, viscera of fish, muscles of fish. The mean concentrations of 239 + 240Pu were comparable for algae collected along the Japan Sea coast and the Pacific coast. Furthermore, the difference in mean concentrations of 137Cs in algae between the Japan Sea coast and the Pacific coast was not statistically significant within the 95% confidence limit. These results can be considered to indicate no definite influence from radioactive dumping into the Japan Sea by the former USSR and Russia with respect to radioactive pollution of marine organisms collected along the Japanese coast.