Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005

A radioactivity survey was launched in 1991 to determine the background levels of ^239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ^239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ^239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ^239+240Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ^239+240Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.     

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.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

Environmental study of fallout plutonium in soils from the piemonte region (North-West Italy)

The distributions of ²³⁸Pu and ^239+240Pu in surface soils from the Piemonte region were measured and the main factors influencing Pu concentrations investigated. Rainfall, altitude and the concentration of organic matter play an important role, while other soil parameters (pedology, lithology and geomorphology) are of lesser significance. Contour maps of the surface soil concentrations of ²³⁸Pu and ^239+240Pu are reported.     

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.     

Temporal variation of Cs and Pu in the sea of Japan

Concentrations of the anthropogenic ¹³⁷Cs and ^239,240Pu in surface water of the Sea of Japan were in the ranges of 2·7–3·8 mBq l^-1 and 1·3–8·0 μBq l^-1, respectively, in 1993–1994, which are in the same order of magnitude as those in the North Pacific. The time-series data indicated a marked increase of surface ¹³⁷Cs in 1986 and 1987 after the major radioactive dumping and the Chernobyl fallout in 1986 and then rapidly decreased thereafter. The apparent half-residence time of ¹³⁷Cs in the surface water was estimated to be about 3 years for excess ¹³⁷Cs and 16 years for a rather long time-scale transport, respectively. For ^239,240Pu in the surface water, no systematic temporal variation was observed over the past two decades, which may reflect rapid recycling of deeper Pu. The results revealed that most of the recent radioactivity in water columns of the Sea of Japan was of global fallout origin from atmospheric nuclear testing and partly the Chernobyl fallout. No clear signal about the effect of radioactivity from Russian dumping was observed.     

Spatial and temporal distribution of Pu in the Northwest Pacific Ocean using modern coral archives

Historical ²³⁹Pu activity concentrations and ²⁴⁰Pu/²³⁹Pu atom ratios were determined in skeletons of dated modern corals collected from three locations (Chuuk Lagoon, Ishigaki Island and Iki Island) to identify spatial and temporal variations in Pu inputs to the Northwest Pacific Ocean. The main Pu source in the Northwest Pacific is fallout from atmospheric nuclear weapons testing which consists of global fallout and close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands. PPG close-in fallout dominated the Pu input in the 1950s, as was observed with higher ²⁴⁰Pu/²³⁹Pu atom ratios (> 0.30) at the Ishigaki site. Specific fallout Pu contamination from the Nagasaki atomic bomb and the Ivy Mike thermonuclear detonation at the PPG were identified at Ishigaki Island from the ²⁴⁰Pu/²³⁹Pu atom ratios of 0.07 and 0.46, respectively. During the 1960s and 1970s, global fallout was the major Pu source to the Northwest Pacific with over 60% contribution to the total Pu. After the cessation of the atmospheric nuclear tests, the PPG again dominated the Pu input due to the continuous transport of remobilised Pu from the Marshall Islands along the North Equatorial Current and the subsequent Kuroshio Current. The Pu contributions from the PPG in recent coral bands (1984 onwards) varied over time with average estimated PPG contributions between 54% and 72% depending on location.     

Upward movement of plutonium to surface sediments during an 11-year field study

An 11-year lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The ²⁴⁰Pu/²³⁹Pu and ²⁴²Pu/²³⁹Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments.     

Concentration and characterization of plutonium in soils of Hubei in central China

To study the Pu concentration and isotope ratio distributions present in China, the ^239+240Pu total activities and ²⁴⁰Pu/²³⁹Pu atom ratios in core soil samples from Hubei Province in central China were investigated using Accelerator Mass Spectrometry (AMS). The activities ranged from 0.019 to 0.502 mBq g⁻¹ and the ^239+240Pu inventories of 45 and ∼55 Bq m⁻² agree well with that expected from global fallout. The ²⁴⁰Pu/²³⁹Pu atom ratios in the soil ranged from 0.172 to 0.220. The ratios are similar to typical global fallout values. Hence, any close-in fallout contribution from the Chinese nuclear weapons tests, mainly conducted in the 1970s, must have either been negligible or had a similar ²⁴⁰Pu/²³⁹Pu ratio to that of global fallout. The top 10 cm layer of the soil contributes ∼90% of the total inventory and the maximum concentrations appeared in the 2-4 cm or 4-6 cm layers. It is suggested that climatic conditions and organic content are the two main factors that affect the vertical migration of plutonium in soil.     

Human bones obtained from routine joint replacement surgery as a tool for studies of plutonium, americium and ⁹⁰Sr body-burden in general public

The paper presents a new sampling method for studying in-body radioactive contamination by bone-seeking radionuclides such as ⁹⁰Sr, ^239+240Pu, ²³⁸Pu, ²⁴¹Am and selected gamma-emitters, in human bones. The presented results were obtained for samples retrieved from routine surgeries, namely knee or hip joints replacements with implants, performed on individuals from Southern Poland. This allowed to collect representative sets of general public samples. The applied analytical radiochemical procedure for bone matrix is described in details. Due to low concentrations of ²³⁸Pu the ratio of Pu isotopes which might be used for Pu source identification is obtained only as upper limits other then global fallout (for example Chernobyl) origin of Pu. Calculated concentrations of radioisotopes are comparable to the existing data from post-mortem studies on human bones retrieved from autopsy or exhumations. Human bones removed during knee or hip joint surgery provide a simple and ethical way for obtaining samples for plutonium, americium and ⁹⁰Sr in-body contamination studies in general public.     

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 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.     

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.     

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.     

The distribution of plutonium,Americium and curium isotopes in pond and stream sediments of the Savannah river plant,South Carolina,USA

The concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am and ²⁴⁴Cm were determined in sediment samples from five streams and two ponds on the Savannah River Plant (SRP) and in four sediment samples from the Savannah River above and below the plant site. The following concentration ranges were determined: ²³⁸Pu, 0·07–386 fCi g⁻¹; ^239,240Pu, 0·37–1410 fCi g⁻¹; ²⁴¹Am, 0·1–4360 fCi g⁻¹; ²⁴⁴Cm, <0·01–392 fCi g⁻¹. Comparisons of the elemental and isotopic ratios of the sediments show that the majority of the sediments studied have been impacted upon by plant operations and that sediments outside the plant boundary in the Savannah River have only been influenced by aerial releases. Atom ratios of ²⁴⁰Pu/²³⁹Pu indicate that up to 86% of the Pu in these sediments is derived from plant operations. However, comparisons of the concentration data with values for other impacted sediments near nuclear facilities indicate that the levels are relatively small. Finally, <13% of the Pu, Am or Cm in pond sediments is associated with humic or fulvic acids, indicating that little of the material should be remobilized in oxic environments through organic complexation.     

Assessing radiation impact at a protected coastal sand dune site: an intercomparison of models for estimating the radiological exposure of non-human biota

This paper presents the application of three publicly available biota dose assessment models (the ERICA Tool, R&D128/SP1a and RESRAD-BIOTA) to an assessment of the Drigg coastal sand dunes. Using measured ⁹⁰Sr, ⁹⁹Tc, ¹³⁷Cs, ²³⁸Pu, ^239+240Pu and ²⁴¹Am activity concentrations in sand dune soil, activity concentration and dose rate predictions are made for a range of organisms including amphibians, birds, invertebrates, mammals, reptiles, plants and fungi. Predicted biota activity concentrations are compared to measured data where available. The main source of variability in the model predictions is the transfer parameters used and it is concluded that developing the available transfer databases should be a focus of future research effort. The value of taking an informed user approach to investigate the way in which models may be expected to be applied in practice is highlighted and a strategy for the future development of intercomparison exercises is presented.     

Vertical distribution of anthropogenic radionuclides in cores from contaminated floodplains of the Yenisey River

The Mining and Chemical Industrial Combine, Zheleznogorsk (MCIC, previously known as Krasnoyarsk-26) on the River Yenisey has contaminated the surrounding environment with anthropogenic radionuclides as a result of discharges of radioactive wastes. The purpose of this study was to investigate the vertical distribution of anthropogenic contamination (¹³⁷Cs and plutonium) within floodplain areas at different distances from the discharge point. Sites were chosen that display different characteristics with respect to periodic inundation with river water. Cs-137 activity concentrations were in the range 23–3770 Bq/kg (dry weight, d.w.); Pu-239,240 activity concentrations were in the range <0.01–14.2 Bq/kg (d.w.). Numerous sample cores exhibited sub-surface maxima which may be related to the historical discharges from the MCIC. Possible evidence indicating the deposition of earlier discharges at MCIC in deeper core layers was observed in the ²³⁸Pu:^239,240Pu activity ratio data: a Pu signal discernible from global fallout could be observed in numerous samples. Cs-137 and Pu-239,240 activity concentrations were correlated with the silt fraction (% by mass <63 μm) though no significant correlation was observed between (grain-size) normalised ¹³⁷Cs activity concentrations and distance downstream from the MCIC.     

Using sequential extraction techniques to assess the partitioning of plutonium and neptunium-237 from multiple sources in sediments from the Ob River (Siberia)

Sequential extraction techniques have been developed to assess partitioning of anthropogenic radionuclides (²⁴⁰Pu, ²³⁹Pu, and ²³⁷Np), originating from a variety of sources, as identified by using bulk sediment isotopic composition. Sediments were leached sequentially with a series of six chemical treatments designed to approximate different environmental processes that may occur or to selectively extract trace metals contained in different solid phases of the sediments (i.e., exchangeable, reducible, carbonate, organic, acid leachable, and refractory). Results indicate the majority of Pu and Np is similarly distributed within many of the extracted fractions, with the largest percentage (66–97%) of both elements being observed in sediments treated with buffered citrate dithionite (CDB), which targets easily reduced constituents such as Mn and Fe hydrous oxides. While these results do indicate an association of Pu and Np with redox sensitive elements, the environmental implications are unclear given that the CDB treatment is more extreme than naturally occurring conditions. Minor amounts of Np partition differently from Pu in sediments. The NH₄-acetate treatment, which is designed to liberate trace metals that are loosely adsorbed onto the surfaces of sedimentary materials such as hydrated iron oxides and humic substances, or present at exchangeable sites in clay minerals, mobilized ∼12% of the total Np while Pu levels were below detection. The H₂O₂ treatment, which is designed to liberate trace metals bound to organic matter, mobilized ∼8 and ∼1% of Np and Pu, respectively. These results indicate that a minor portion of the total Np may be affected by environmental conditions that have little or no effect on Pu. Between 7 and 24% of the Pu was observed in treatments designed to liberate Pu and Np that are tightly bound to lithogenic phases or refractory silicates. The ²⁴⁰Pu/²³⁹Pu observed in accessible and refractory fractions ranged between 0.11 and 0.18. With the exception of one sample, the ²⁴⁰Pu/²³⁹Pu isotope ratios measured in the refractory fractions are essentially identical having a mean ratio value of 0.123 ± 0.001 (1σ). The ²⁴⁰Pu/²³⁹Pu ratios provide isotopic evidence that suggests a portion of non-fallout contamination has a refractory nature. The presence of similarly low ²⁴⁰Pu/²³⁹Pu ratios in refractory fractions of sediments from the Ob and Irtysh Rivers suggests the existence of a source of refractory Pu which is consistent with refractory “hot particles” derived from surface tests at the Semipalitinsk test site.     

Pu/Cs ratios in the water column of the North Pacific: a proxy of biogeochemical processes

Anthropogenic radionuclides in seawater have been used as transient tracers of processes in the marine environment. Especially, plutonium in seawater is considered to be a valuable tracer of biogeochemical processes due to its particle-reactive properties. However, its behavior in the ocean is also affected by physical processes such as advection, mixing and diffusion. Here we introduce Pu/¹³⁷Cs ratio as a proxy of biogeochemical processes and discuss its trends in the water column of the North Pacific Ocean. We observed that the ^239,240Pu/¹³⁷Cs ratio in seawater exponentially increased with increasing depth (depth range: 100–1000 m). This finding suggests that the profiles of the ^239,240Pu/¹³⁷Cs ratios in shallower waters directly reflect biogeochemical processes in the water column. A half-regeneration depth deduced from the curve fitting the observed data, showed latitudinal and longitudinal distributions, also related to biogeochemical processes in the water column.     

Plutonium bioaccumulation in seabirds

The aim of the paper was plutonium (²³⁸Pu and ^239+240Pu) determination in seabirds, permanently or temporarily living in northern Poland at the Baltic Sea coast. Together 11 marine birds species were examined: 3 species permanently residing in the southern Baltic, 4 species of wintering birds and 3 species of migrating birds. The obtained results indicated plutonium is non-uniformly distributed in organs and tissues of analyzed seabirds. The highest plutonium content was found in the digestion organs and feathers, the smallest in skin and muscles. The plutonium concentration was lower in analyzed species which feed on fish and much higher in herbivorous species. The main source of plutonium in analyzed marine birds was global atmospheric fallout.