Application of a magnetic extraction technique to assess radionuclide-mineral association in Cumbrian shoreline sediments

An assessment has been made of the association of (239+240)Pu, 241Am and 210Po (in secular equilibrium with 210Pb) with iron minerals using a magnetic extraction technique. Grab samples of beach sand from the Cumbrian (UK) coastline were subjected to successive extractions with an approximately 0.1 T ferrite magnet and an approximately 0.3 T rare-earth magnet procedure to separate magnetic iron oxide minerals. Radionuclide concentrations in the magnetic extracts were enhanced (by approximately 4-6-fold) relative to the residue. Those in the approximately 0.1 T magnet extracts were broadly similar to those in the antiferromagnetic material extracted by the approximately 0.3 T magnet, despite the very large differences in magnetic property values between the two fractions (one to two orders of magnitude). The percentage of magnetic material in terms of mass was small and therefore, the majority of these radionuclides (on average 88%) were associated with the residue. Removal of stable Fe was incomplete. Given that the radionuclides may also bind to paramagnetic (nonmagnetic) Fe minerals, the data were extrapolated by normalising the results to quantitative Fe removal. This yielded average values of 37%, 45% and 46% for (239+240)Pu, 241Am and 210Po(210Pb), respectively, as upper limits for the fraction associated with magnetic + nonmagnetic Fe minerals. There are significant uncertainties inherent in quantifying data from this extraction technique. Nevertheless, it seems reasonable to conclude that radionuclide association with Fe minerals is unlikely to have a significant impact upon the physical dispersion of sediment contaminated by Sellafield discharges in the Irish Sea. However, it may be an important factor in governing Pu redox and redissolution behaviour.     

Behaviour and transport of radionuclides in soil and vegetation of a sand dune ecosystem

A sand dune ecosystem in the vicinity of the British Nuclear Fuels reprocessing plant at Sellafield, Cumbria, UK was used to examine the spatial, temporal and depth distributions of 134Cs, 137Cs, 238Pu, 239 + 240Pu and 241Am in soil and in two species of vegetation (Festuca rubra, Ammophila arenaria). Core samples showed evidence of the accumulation of radionuclides derived mainly from sea-to-land transfer. Accumulated deposits of radioactivity (0-0.1 m) lie within the range: 1.1-3.4 Bq kg-1 (134Cs), 260-440 Bq kg-1 (137Cs), 31-40 Bq kg-1 (238Pu), 150-215 Bq kg-1 (239 + 240Pu) and 190-240 Bq kg-1 (241Am). Soil profiles showed greater activity concentrations in their deeper regions and this is attributed to leaching of radionuclides in percolating drainage water accentuated by the coarse texture, low organic matter and clay mineral content of coastal sands. Radionuclide activity concentrations in F. rubra and A. arenaria were similar, in the ranges 20-70 Bq kg-1 (137Cs), 1-5 Bq kg-1 (238Pu), 10-30 Bq kg-1 (239 + 240Pu) and 10-65 Bq kg-1 (241Am). Clear temporal and spatial variations were observed in both species of vegetation, reflecting the weather conditions antecedent to the sampling period and the influence of sea-to-land transfer. Concentration ratios (vegetation:soil) for activity concentrations in the two species were similar, in the ranges: 0.05-0.14 (137Cs), 0.025-0.097 (238Pu), 0.022-0.057 (239 + 240Pu) and 0.025-0.212 (241Am).     

Factors affecting 210Po and 210Pb activity concentrations in mussels and implications for environmental bio-monitoring programmes

The activity of ²¹⁰Po and ²¹⁰Pb was determined in mussels of the same size (3.5-4.0 cm shell length) sampled monthly over a 17-month period at the Atlantic coast of Portugal. Average radionuclide concentration values in mussels were 759 ± 277 Bq kg⁻¹ for ²¹⁰Po (range 460-1470 Bq kg⁻¹ dry weight), and 45 ± 19 Bq kg⁻¹ for ²¹⁰Pb (range 23-96 Bq kg⁻¹ dry weight). Environmental parameters and mussel biometric parameters were monitored during the same period. Although there was no seasonal variation of radionuclide concentrations in sea water during the study period, the concentration of radionuclide activity in mussels varied seasonally displaying peaks of high concentrations in winter and low concentrations in summer. Analysis of radionuclide data in relation to the physiological Condition Index of mussels revealed that ²¹⁰Po and ²¹⁰Pb activities in the mussel (average activity per individual) remained nearly constant during the investigation period, while mussel body weight fluctuated due to fat storage/expenditure in the soft tissues. Similar variation of radionuclide concentrations was observed in mussels transplanted from the sea coast into the Tejo Estuary. However, under estuarine environmental conditions and with higher food availability throughout the year, transplanted mussel Condition Index was higher than in coastal mussels and average radionuclide concentrations were 210 ± 75 Bq kg⁻¹ (dry weight) for ²¹⁰Po and 10 ± 4 Bq kg⁻¹ (dry weight) for ²¹⁰Pb, therefore lower than in coastal mussels with similar shell length. It is concluded that the apparent seasonal fluctuation and inter-site difference of radionuclide concentrations were mostly caused by mussel body weight fluctuation and not by radionuclide body burden fluctuation. This interpretation can be extended to the apparent seasonal fluctuation in concentrations of lipophilic and lipophobic contaminants in mussels, and provides an explanation for occasional high concentrations of ²¹⁰Po and man-made contaminants measured in mussels far from pollution sources.     

Seasonal and spatial variability of Po,U and Pu levels in the river catchment area assessed by application of neural-network based classification

The present study deals with the application of self-organizing maps (SOM) in order to model, classify and interpret seasonal and spatial variability of ²¹⁰Po, ²³⁸U and ^239+240Pu levels in the Vistula river basin. The data set represents concentration values for 3 alpha emitters (²¹⁰Po, ²³⁸U and ^239+240Pu) measured in surface water samples collected at 19 different sampling locations (8 in major Vistula stream while 11 in right or left Vistula tributaries) during four seasons (winter, spring, summer and autumn) in the framework of a one-year quality monitoring study. The advantages of an SOM algorithm, its classification and visualization ability for environmental data sets, are stressed. The neural-network based classification made it possible to reveal specific patterns related to both seasonal and spatial variability. In the middle and upper part of Vistula catchment as well as in the right-shore tributaries, concentrations of ²¹⁰Po and ²³⁸U during summer and winter are the lowest. Concentrations of ²¹⁰Po and ²³⁸U increase significantly during spring and autumn in the Vistula river catchment, especially in the delta of Vistula river. High concentration of anthropogenic originated ^239+240Pu indicates “site-specific” character of pollution in two large left-shore tributaries located in the middle part of the Vistula drainage area. Efficient classification of sampling locations could lead to an optimization of river radiochemical sampling networks and to a better tracing of natural and anthropogenic changes along Vistula river stream.     

Accumulation of 210Po in Baltic invertebrates

This paper presents the results of an investigation of the ²¹⁰Po contents of Baltic marine invertebrates. The ²¹⁰Po concentrations fall within the range 11·3–78·9 Bq kg⁻¹ (dry wt), the higher values relating to polychaeta, priapulida and malacostraca and the lower levels to bivalvia. It is demonstrated that ¹⁰Po is non-uniformly distributed within the isopod Mesidotea entomon and the bivalve Mya arenaria. The ²¹⁰Po contents of the internal organs decreasing in the order-hepatopancreas > alimentary tract > gill > muscle. Moreover, the results indicate the dominant role of the digestive organs of these invertebrates in controlling absorption and elimination of ²¹⁰Po.     

Variation of the activity concentrations and fluxes of natural (210Po, 210Pb) and anthropogenic (239,240Pu, 137Cs) radionuclides in the Strait of Gibraltar (Spain)

The activity concentrations and fluxes of natural (210Pb, 210Po) and anthropogenic (239,240Pu, 137Cs) radionuclides have been determined in the different water masses crossing the Strait of Gibraltar. New data have been gathered during four multidisciplinary and multinational sampling campaigns, performed between 1997 and 1999 within the framework of the CANIGO-FLUGIST Project. Mean activity concentrations of 210Po (1.53+/-0.34 Bq m(-3), n = 30) and 210Pb (1.16+/-0.50 Bq m(-3), n = 31) in the Atlantic water entering the Mediterranean basin are about double those measured in the Mediterranean outflow, namely 0.84+/-0.34 Bq m(-3) (n = 22) for 210Po and 0.66+/-0.34 Bq m(-3) (n = 22) for 210Pb. The opposite trend is observed for 231,240Pu, with average concentrations of 9.9+/-3.0 mBq m(-3) (n = 29) in the incoming Atlantic flow and 22.0+/-3.0 mBq m(-3) (n = 22) in the outpouring Mediterranean water. In the case of 137Cs, the same concentrations were quantified in the waters moving inwards (2.52+/-0.28 Bq m(-3), n = 27) and outwards (2.14+/-0.52 Bq m(-3), n = 21) from the Mediterranean Sea. On this basis, the Mediterranean basin experiences a net annual input flux of 14 TBq of 210Pb and 19 TBq of 210Po, and a net annual loss of 0.34 TBq of 239,240Pu, while--at present--137Cs input and output fluxes appear to be balanced.     

Plutonium in sheep faeces as an indicator of deposition on vegetation

In order to study the deposition on vegetation of plutonium arising from the testing of nuclear weapons and discharges from nuclear facilities, sheep faeces were collected from the South-west and North of England. The plutonium content of faeces has been shown to be a reproducible and sensitive indicator of deposition on herbage and, with this technique, plutonium discharged from the Sellafield Works of British Nuclear Fuels LImited can be detected 60 km from the site. On moorland pastures the concentration of ^239+240Pu in faeces, expressed as activity per gram of ash, is roughly equal numerically to the deposit of plutonium on 1 m² of vegetation.Some of the plutonium ingested by a grazing sheep is absorbed and the highest concentrations are found in liver. The liver of a sheep grazing on pasture where the ^239+240Pu concentration in faeces was about 2 pCi (74 mBq) g⁻¹ of ash, was found to contain <1% of the Generalised Derived Limit for mutton and offal, and the meat <0·001%.     

Assessment of the global fallout of plutonium isotopes and americium-241 in the soil of the central region of Saudi Arabia

A radiochemical technique for determination of plutonium isotopes and 241Am in soil samples is tested against IAEA-standard reference materials to determine its accuracy and precision for reliable results. The technique is then used in the investigation of topsoil samples, collected from the natural environment of the central region of Saudi Arabia, to assess the effect of fallout accumulation of these radionuclides in the region. Plutonium and americium were sequentially separated from all other components of the sample by anion-exchange chromatography and co-precipitated with Nd3+ as fluorides. The precipitates were mounted on membrane filters and measured using a high-resolution alpha-spectrometer. The results of the analysis of the reference materials showed satisfactory sensitivity and precision of the technique. The results of the analyzed soil samples show activity levels ranging from < LLD to 0.089 and from 相似文献   

Airborne radioactivity on the Scottish Solway coast

A brief survey of the concentrations of radionuclides in surface air at five locations along the Scottish shoreline of the Irish Sea has been made in response to concern that airborne resuspension of marine radioactivity may be causing an inhalation hazard. Airborne concentrations of ⁴⁰K, ¹⁰⁶Ru, ¹³⁷Cs, ¹⁴⁴Ce, ²³⁸Pu, ^{239 + 240}Pu and ²⁴¹Am are reported. Plutonium isotopic ratios indicate the presence of radioactivity of marine origin attributable to low-level waste disposals from the fuel-reprocessing plant at Sellafield in Cumbria. Calculation of the dose resulting from inhalation shows that the risks to members of the public are negligible. Suggestions are made for development of these studies in future.     

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.     

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.     

Levels and transfer of Po and Pb in Nordic terrestrial ecosystems

Recent developments regarding environmental impact assessment methodologies for radioactivity have precipitated the need for information on levels of naturally occurring radionuclides within and transfer to wild flora and fauna. The objectives of this study were therefore to determine activity concentrations of the main dose forming radionuclides ²¹⁰Po and ²¹⁰Pb in biota from terrestrial ecosystems thus providing insight into the behaviour of these radioisotopes. Samples of soil, plants and animals were collected at Dovrefjell, Central Norway and Olkiluoto, Finland. Soil profiles from Dovrefjell exhibited an approximately exponential fall in ²¹⁰Pb activity concentrations from elevated levels in humus/surface soils to “supported” levels at depth. Activity concentrations of ²¹⁰Po in fauna (invertebrates, mammals, birds) ranged between 2 and 123 Bq kg⁻¹ d.w. and in plants and lichens between 20 and 138 Bq kg⁻¹ d.w. The results showed that soil humus is an important reservoir for ²¹⁰Po and ²¹⁰Pb and that fauna in close contact with this media may also exhibit elevated levels of ²¹⁰Po. Concentration ratios appear to have limited applicability with regards to prediction of activity concentrations of ²¹⁰Po in invertebrates and vertebrates. Biokinetic models may provide a tool to explore in a more mechanistic way the behaviour of ²¹⁰Po in this system.     

Technologically enhanced 210Pb and 210Po in iron and steel industry

Iron and steel manufacture has been ranked as the largest industrial source of environmental contamination in the USA; the wastes generated in their production processes contain heavy elements that can be a source of contamination, and natural radionuclides that can produce an occupational and/or public radiological impact. In this work the potential occupational effective dose rate (μSv/y) due to inhalation in four integrated steel-making factories from Egypt has been evaluated, by assuming a well defined scenario and with basis in the ²¹⁰Pb and ²¹⁰Po activity concentrations determined in ore and wastes collected in the aforementioned factories. Activity concentrations, in Bq/kg, of ²¹⁰Pb and ²¹⁰Po, and leachable Pb and Fe were measured using gamma-ray spectrometry based on HPGe detector, alpha particle spectrometry based on PIPS detector, and inductively coupled plasma-mass spectrometry (ICP-MS). Levels of ²¹⁰Pb and ²¹⁰Po in the range of <DL-4238 and 1-5660 Bq/kg, respectively, were found. According to the assumed scenarios, the occupational exposures by inhalation are much lower than the recommended annual effective dose limit, although the environmental impact due to waste storage and/or use should be considered based on case by case evaluation.     

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.     

Assessment of Po and Pb in marine biota of the Mallipattinam ecosystem of Tamil Nadu, India

To provide baseline data on background radiation levels for the future assessment of the impact of nuclear and thermal power stations, a systematic study was carried out in the Mallipattinam ecosystem of Tamil Nadu, India. Mallipattinam is located between the Kudankulam and Kalpakkam nuclear power plants and near to Tuticorin thermal power plant. Water, sediments, seaweeds, crustaceans, molluscs, and fish were collected to measure the concentrations of ²¹⁰Po and ²¹⁰Pb. The concentrations of ²¹⁰Po and ²¹⁰Pb in most samples are comparable to values reported worldwide. In fish, the concentrations of ²¹⁰Po and ²¹⁰Pb are in the range 16-190 Bq kg⁻¹ and 8-153 Bq kg⁻¹, respectively. The concentration factors of ²¹⁰Po and ²¹⁰Pb for the biotic components ranges from 10³ to 10⁶.     

Polonium-210 and lead-210 in the terrestrial environment: a historical review

The radionuclides ²¹⁰Po and ²¹⁰Pb widely present in the terrestrial environment are the final long-lived radionuclides in the decay of ²³⁸U in the earth’s crust. Their presence in the atmosphere is due to the decay of ²²²Rn diffusing from the ground. The range of activity concentrations in ground level air for ²¹⁰Po is 0.03-0.3 Bq m⁻³ and for ²¹⁰Pb 0.2-1.5 Bq m⁻³.In drinking water from private wells the activity concentration of ²¹⁰Po is in the order of 7-48 mBq l⁻¹ and for ²¹⁰Pb around 11-40 mBq l⁻¹. From water works, however, the activity concentration for both ²¹⁰Po and ²¹⁰Pb is only in the order of 3 mBq l⁻¹.Mosses, lichens and peat have a high efficiency in capturing ²¹⁰Po and ²¹⁰Pb from atmospheric fallout and exhibit an inventory of both ²¹⁰Po and ²¹⁰Pb in the order of 0.5-5 kBq m⁻² in mosses and in lichens around 0.6 kBq m⁻². The activity concentrations in lichens lies around 250 Bq kg⁻¹, dry mass.Reindeer and caribou graze lichen which results in an activity concentration of ²¹⁰Po and ²¹⁰Pb of about 1-15 Bq kg⁻¹ in meat from these animals. The food chain lichen-reindeer or caribou, and Man constitutes a unique model for studying the uptake and retention of ²¹⁰Po and ²¹⁰Pb in humans. The effective annual dose due to ²¹⁰Po and ²¹⁰Pb in people with high consumption of reindeer/caribou meat is estimated to be around 260 and 132 μSv a⁻¹ respectively.In soils, ²¹⁰Po is adsorbed to clay and organic colloids and the activity concentration varies with soil type and also correlates with the amount of atmospheric precipitation. The average activity concentration levels of ²¹⁰Po in various soils are in the range of 20-240 Bq kg⁻¹.Plants become contaminated with radioactive nuclides both by absorption from the soil (supported Po) and by deposition of radioactive fallout on the plants directly (unsupported Po). In fresh leafy plants the level of ²¹⁰Po is particularly high as the result of the direct deposition of ²²²Rn daughters from atmospheric deposition. Tobacco is a terrestrial product with high activity concentrations of ²¹⁰Po and ²¹⁰Pb. The overall average activity concentration of ²¹⁰Po is 13 ± 2 Bq kg⁻¹. It is rather constant over time and by geographical origin.The average median daily dietary intakes of ²¹⁰Po and ²¹⁰Pb for the adult world population was estimated to 160 mBq day⁻¹ and 110 mBq day⁻¹, corresponding to annual effective doses of 70 μSv a⁻¹ and 28 μSv a⁻¹, respectively. The dietary intakes of ²¹⁰Po and ²¹⁰Pb from vegetarian food was estimated to only 70 mBq day⁻¹ and 40 mBq day⁻¹ corresponding to annual effective doses of 30.6 μSv a⁻¹ and 10 μSv a⁻¹, respectively. Since the activity concentration of ²¹⁰Po and ²¹⁰Pb in seafood is significantly higher than in vegetarian food the effective dose to populations consuming a lot of seafood might be 5-15 fold higher.     

Plutonium and americium inventories in atmospheric fallout and sediment cores from Blelham Tarn, Cumbria (UK)

The objective of this paper is to report on the results of a study of 238Pu, 239 + 240Pu and 241Am inventories onto Blelham Tarn in Cumbria (UK). The atmospheric fallout inventory was obtained by analysing soil cores and the results are in good agreement with the literature: 101 Bq m(-2) for 239 + 240Pu; 4.5 Bq m(-2) for 238Pu and 37 Bq m(-2) for 241Am. The sediment core inventory for the whole lake is compared to the atmospheric fallout inventory. The sediment activity is 60-80% higher than the estimated fallout activity, showing a catchment area contribution and in particular the stream input.     

Radioisotope contaminations from releases of the Tomsk-Seversk nuclear facility (Siberia, Russia)

Soils have been sampled in the vicinity of the Tomsk-Seversk facility (Siberia, Russia) that allows us to measure radioactive contaminations due to atmospheric and aquatic releases. Indeed soils exhibit large inventories of man-made fission products including 137Cs (ranging from 33,000 to 68,500 Bq m(-2)) and actinides such as plutonium (i.e. 239+240Pu from 420 to 5900 Bq m(-2)) or 241Am (160-1220 Bq m(-2)). Among all sampling sites, the bank of the Romashka channel exhibits the highest radioisotope concentrations. At this site, some short half-life gamma emitters were detected as well indicating recent aquatic discharge in the channel. In comparison, soils that underwent atmospheric depositions like peat and forest soils exhibit lower activities of actinides and 137Cs. Soil activities are too high to be related solely to global fallout and thus the source of plutonium must be discharges from the Siberian Chemical Combine (SCC) plant. This is confirmed by plutonium isotopic ratios measured by ICP-MS; the low 241Pu/239Pu and 240Pu/239Pu atomic ratios with respect to global fallout ratio or civil nuclear fuel are consistent with weapons grade signatures. Up to now, the influence of Tomsk-Seversk plutonium discharges was speculated in the Ob River and its estuary. Isotopic data from the present study show that plutonium measured in SCC probably constitutes a significant source of plutonium in the aquatic environment, together with plutonium from global fallout and other contaminated sites including Tomsk, Mayak (Russia) and Semipalatinsk (Republic of Kazakhstan). It is estimated that the proportion of plutonium from SCC source can reach 45% for 239Pu and 60% for 241Pu in the sediments.     

Po-210 and Pb-210 as atmospheric tracers and global atmospheric Pb-210 fallout: a review

Over the past ∼5 decades, the distribution of ²²²Rn and its progenies (mainly ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po) have provided a wealth of information as tracers to quantify several atmospheric processes that include: i) source tracking and transport time scales of air masses; ii) the stability and vertical movement of air masses iii) removal rate constants and residence times of aerosols; iv) chemical behavior of analog species; and v) washout ratios and deposition velocities of aerosols. Most of these applications require that the sources and sink terms of these nuclides are well characterized.Utility of ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po as atmospheric tracers requires that data on the ²²²Rn emanation rates is well documented. Due to low concentrations of ²²⁶Ra in surface waters, the ²²²Rn emanation rates from the continent is about two orders of magnitude higher than that of the ocean. This has led to distinctly higher ²¹⁰Pb concentrations in continental air masses compared to oceanic air masses. The highly varying concentrations of ²¹⁰Pb in air as well the depositional fluxes have yielded insight on the sources and transit times of aerosols. In an ideal enclosed air mass (closed system with respect to these nuclides), the residence times of aerosols obtained from the activity ratios of ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb are expected to agree with each other, but a large number of studies have indicated discordance between the residence times obtained from these three pairs. Recent results from the distribution of these nuclides in size-fractionated aerosols appear to yield consistent residence time in smaller-size aerosols, possibly suggesting that larger size aerosols are derived from resuspended dust. The residence times calculated from the ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb activity ratios published from 1970’s are compared to those data obtained in size-fractionated aerosols in this decade and possible reasons for the discordance is discussed with some key recommendations for future studies.The existing global atmospheric inventory data of ²¹⁰Pb is re-evaluated and a ‘global curve’ for the depositional fluxes of ²¹⁰Pb is established. A current global budget for atmospheric ²¹⁰Po and ²¹⁰Pb is also established. The relative importance of dry fallout of ²¹⁰Po and ²¹⁰Pb at different latitudes is evaluated. The global values for the deposition velocities of aerosols using ²¹⁰Po and ²¹⁰Pb are synthesized.     

Characterization of Pu concentration and its isotopic composition in soils of Gansu in northwestern China

The total ^239+240Pu activities and ²⁴⁰Pu/²³⁹Pu atom ratios in surface soil samples (0–5 cm) in the Kumtag Desert in western Gansu Province, and in a soil core sample in Lanzhou were investigated using a sector-field ICP-MS. In the surface soil samples, ^239+240Pu activities in fine particles (<150 μm) were 1.3–2.1 times of those in coarse particles (150 μm–1 mm) which ranged from 0.005 to 0.157 mBq/g. Atom ratios of ²⁴⁰Pu/²³⁹Pu in the surface soils ranged from 0.168 to 0.192 with a mean of 0.182 ± 0.008. The mean ratio was similar to the typical global fallout value although the Kumtag Desert was believed to have received close-in fallout derived from Chinese nuclear weapons tests mainly conducted in the 1970s. Furthermore, the mean ²⁴⁰Pu/²³⁹Pu atom ratio observed in the soil core sample in Lanzhou was similar to the typical global fallout value. In the soil core sample, ^239+240Pu activities in the various layers ranged from 0.012 to 0.23 mBq/g, and the inventory of ^239+240Pu (32.4 Bq/m², 0–23 cm) was slightly lower than that expected from global fallout (42 Bq/m²) at the same latitude. Rapid downward migration of Pu isotopes was observed in Lanzhou soil core sample layers. The contribution of the 10-cm deep top layers of surface soils to total inventory was only 17%, while the contribution of deeper layers (10–23 cm) was as high as 83%. The ^239+240Pu activity levels and ²⁴⁰Pu/²³⁹Pu atom ratios in soils in Gansu Province, China are similar to those in atmospheric deposition samples collected in the spring in recent years in Japan.