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.     

137Cs budget during the period of 1960s in a small drainage basin on the Loess Plateau of China

A sediment profile with a thickness of 28.12 m in a failed reservoir in a small catchment of the Yuntaishan Gully in the Loess Plateau of China consisted of 44 flood couplets deposited during the period from 1960 to 1970 with total volume of 2.36 x 10(6)m(3). Specific sediment yields for a flood event varied from 300 t km(-2) to 14,400 t km(-2) and annual sediment yields varied from 2500 t km(-2) in 1966 to 40,000 t km(-2) in 1964 with a mean value of 12,700 t km(-2)a(-1) for the period. Average annual (137)Cs concentrations of the sediments increased from 0.92 Bq kg(-1) in 1960 to 4.82 Bq kg(-1) in 1963, then decreased to 1.53 Bq kg(-1) in 1970. The total (137)Cs activity in the reservoir sediments was 9.22 x 10(9) Bq, which accounted for 31.9% of the total (137)Cs fallout precipitation of 2.89 x 10(10) Bq within the catchment during the period. The proportion of the (137)Cs loss from the catchment to the (137)Cs fallout precipitation within the catchment in a year varied between 8.01% and 66.8%, and it was 20.9% for the peak (137)Cs deposition year of 1963 and 52.0% in 1964. By analysis of the (137)Cs budget in the catchment for the (137)Cs peak precipitation period from 1962 to 1964, the (137)Cs surface enrichment coefficient Gamma should be much less than 0.23. And for calculation of soil losses on the cultivated land in the inter-gully area by using the Mass Balance Model II, the value of Gamma should be 0.05-0.1.     

(137)Cs concentration in zooplankton and its relation to taxonomic composition in the western North Pacific Ocean

To study the role of zooplankton in the transport of (137)Cs in the ocean, zooplankton samples were collected in October 2005 and June 2006 in the western North Pacific Ocean. The peak zooplankton biomass was observed in the surface layer, and gelatinous plankton was more abundant in October 2005 than in June 2006 reflecting exchange of water masses. The concentrations of (137)Cs in zooplankton varied from 11 to 24 mBq kg wet(-1) and were higher in October 2005 than in June 2006. The elevated abundance of gelatinous zooplankton probably led to higher concentration of (137)Cs in zooplankton in October 2005. Annual export fluxes of (137)Cs by ontogenetic vertical migrant copepods were estimated to be 0.8 and 0.6 mBq m(-2) year(-1) at 200 and 1000 m depths, respectively; this suggested that transport of (137)Cs by zooplankton may be no trivial pathway.     

The extremely high 137Cs inventory in the Sulu Sea: a possible mechanism

Large-volume seawater samples were collected in the Sulu and South China Seas and their (137)Cs activities were determined by gamma-ray spectrometry using a low background type high-purity Ge detector. Vertical distributions of (137)Cs activity showed an exponential decrease in the South China Sea, whereas a subsurface maximum at 200m depth and monotonic decrease below 300m were observed in the Sulu Sea. A significant difference in intermediate water (137)Cs activities in the 500-2000m depth was observed between the Sulu and South China Seas, i.e., the (137)Cs activities in the Sulu Sea were remarkably higher than those in the South China Sea. The difference in the (137)Cs inventory below 500m was approximately 1200Bqm(-2) between the Sulu and South China Seas. The (137)Cs total inventory of 3200Bqm(-2) in the Sulu Sea was 5.7 times higher than that expected from global fallout. A possible mechanism controlling this extremely high (137)Cs total inventory may be inflows of the (137)Cs rich water masses through the Luzon Strait, lateral transport across the Mindoro Strait into the Sulu Sea, and then subduction into the deep layer in the basin.     

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.     

A 10-year study of the 137Cs distribution in soil and a comparison of Cs soil inventory with precipitation-determined deposition

During a 10-year period, 1988-1998, surface soil samples have been collected at Blentarp in southern Sweden and analysed for 137Cs from the Chernobyl accident and from the nuclear weapons tests. The distance between the sampling plots on the different sampling occasions has been no more than 3 m. The results show that the depth distribution of 137Cs is very similar for each of the sampling occasions, indicating that the caesium migration at this site is very small. The total activity measured in the soil cores is in agreement with the calculated activity of 137Cs deposited at the site after nuclear weapons tests and the Chernobyl accident, based on air activity concentration and the amount of precipitation. The calculated deposition of 137Cs originating from the bomb tests amounts to 1.41 kBq m-2 for the period 1962-1986, which is in agreement with the activity of nuclear weapons fallout measured in the soil samples (1.60 kBq m-2 as a mean value of the first four years of sampling). The calculated activity of 137Cs of Chernobyl origin was 0.79 kBq m-2, which agrees well with the value of 0.79 kBq m-2 measured in the soil samples in 1988.     

Present background levels of surface 137Cs and (239,240)Pu concentrations in the Pacific

The present levels of anthropogenic radionuclides, 137Cs and (239,240)Pu, in surface waters of the Pacific are estimated using the HAM database, which is a comprehensive data set of 137Cs, (239,240)Pu and other anthropogenic radionuclides. The time-series data of surface 137Cs and (239,240)Pu suggests that surface 137Cs and (239,240)Pu concentrations in the Pacific since 1971 decrease exponentially in each sea area, although the temporal changes of surface 137Cs and (239,240)Pu differed between sea areas of the Pacific. The calculated 137Cs concentrations in the Pacific surface waters in 2000 are homogeneous in the Pacific, comparing with that in the 1960s and 1970s, although they are still high in the North Pacific and low in the South Pacific. The biogeochemical and physical processes are significant factors to control present levels of surface (239,240)Pu concentrations, which are high in the Subarctic and equatorial Pacific and low in the mid-latitude region of the eastern North Pacific.     

90Sr, 137Cs and (239,240)Pu concentration surface water time series in the Pacific and Indian Oceans--WOMARS results

Under an IAEA's Co-ordinated Research Project "Worldwide Marine Radioactivity Studies (WOMARS)" 90Sr, 137Cs and (239,240)Pu concentration surface water time series in the Pacific and Indian Oceans have been investigated. The Pacific and Indian Oceans were divided into 17 latitudinal boxes according to ocean circulation, global fallout patterns and the location of nuclear weapons test sites. The present levels and time trends in radionuclide concentrations in surface water for each box were studied and the corresponding effective half-lives were estimated. For the year 2000, the estimated average 90Sr, 137Cs and (239,240)Pu concentrations in surface waters of the Pacific and Indian Oceans varied from 0.1 to 1.5 mBq/L, 0.1 to 2.8 mBq/L, and 0.1 to 5.2 microBq/L, respectively. The mean effective half-lives for 90Sr and 137Cs in surface water were 12+/-1 years for the North, 20+/-1 years for the South and 21+/-2 years for the Equatorial Pacific. For (239,240)Pu the corresponding mean effective half-lives were 7+/-1 years for the North, 12+/-4 years for the South and 10+/-2 years for the Equatorial Pacific. For the Indian Ocean the mean effective half-lives of 137Cs and (239,240)Pu were 21+/-2 years and 9+/-1 years, respectively. There is evidence that fallout removal rates before 1970 were faster than those observed during recent decades. The estimated surface water concentrations of 90Sr, 137Cs and (239,240)Pu in latitudinal belts of the Pacific and Indian Oceans for the year 2000 may be used as the average levels so that any new contribution from nuclear facilities, nuclear weapons test sites, radioactive waste dumping sites and from possible nuclear accidents can be identified.     

Derivation of 137Cs deposition density from measurements of 137Cs inventories in undisturbed soils

The 137Cs inventories in undisturbed soils were measured for 292 locations across the territory of Vietnam. The logarithmic inventory values were regressed against characteristics of sampling sites, such as geographical coordinates, annual rainfall and physico-chemical parameters of soil. The regression model containing latitude and annual rainfall as determinants could explain 76% of the variations in logarithmic inventory values across the territory. The model part was interpreted as the logarithmic 137Cs deposition density. At the 95% confidence level, 137Cs deposition density could be predicted by the model within +/- 7% relative uncertainty. The latitude mean 137Cs deposition density increases northward from 237 Bq m(-2) to 1097 Bq m(-2), while the corresponding values derived from the UNSCEAR (1969) global pattern are 300 Bq m(-2) and 600 Bq m(-2). High 137Cs inputs were found in high-rainfall areas in northern and central parts of the territory.     

Foliar uptake of Cs from the water column by aquatic macrophytes

A transplant experiment was performed to determine the relative importances of root uptake from the sediments and foliar uptake from the water column in determining the accumulation of ¹³⁷Cs by aquatic macrophytes. Uncontaminated individuals of three species, Brasenia schreberi, Nymphaea odorata and Nymphoides cordata, were transplanted into pots containing either contaminated sediments (i.e. 1.2 Bq ¹³⁷Cs g⁻¹ dry mass) or uncontaminated sediments (i.e. < 0.1 Bq g⁻¹ dry mass) and immersed in Pond B, a former reactor cooling pond where ¹³⁷Cs concentrations in surface waters range from 0.4 to 0.8 Bq liter⁻¹. The plants in uncontaminated sediments rapidly accumulated ¹³⁷Cs from the water column and after 35 days of immersion had ¹³⁷Cs concentrations in leaves that were: (1) not statistically significantly different from those for plants in contaminated sediments; and (2) similar to those for the same species growing naturally in Pond B. The similarity in ¹³⁷Cs concentrations between naturally-occurring plants and those in pots with uncontaminated sediments suggests that foliar uptake from the water column is the principal mode of Cs accumulation by these species in Pond B.     

137Cs in freshwater fish in Finland since 1986--a statistical analysis with multivariate linear regression models

The accident at the Chernobyl nuclear power plant in 1986 significantly elevated the 137Cs levels of fish in Finnish lakes. About 6200 fish samples from 390 lakes comprising 20 species have been analysed for 137Cs since 1986. The sizes of the lakes varied from a few hectares to about 1000 km2. Activity concentrations of 137Cs in fish still varied widely in 2003, from 16 to 6400 Bq/kg fresh weight. This paper presents the results of statistical analyses with multivariate linear regression models carried out on the empirical data collected since 1986. The statistical analysis resulted in separate models for two time periods describing temporal changes of 137Cs in fish. The explanatory variables were fish species with various feeding habits, the size class of the lake, municipal division, drainage area, time since the deposition and deposition level of the municipality. The calculated values for 137Cs in fish did not differ statistically significantly from the observed values in the validation data. The explanatory variables explained 58% (the first time period) and 72% (the second time period) of the total variability of 137Cs in fish.     

Simulating transport of non-Chernobyl (137)Cs and (90)Sr in the North Atlantic-Arctic region

The spatial and temporal distributions of the anthropogenic radionuclides (137)Cs and (90)Sr, originating from nuclear bomb testing and the Sellafield reprocessing plants in the Irish Sea, are simulated using a global version of the Miami Isopycnic Coordinate Ocean Model (MICOM). The physical model is forced with daily atmospheric re-analysed fields for the period 1950 to present. Comparison of temporal evolution of observed and simulated concentrations of (137)Cs have been conducted for the regions east of Scotland, west of central Norway and at the entrance of the Barents Sea. It follows that the radionuclides from the Sellafield discharge reach the Barents Sea region after 4-5 years, in accordance with observations. The simulation provides a detailed distribution and evolution of the radionuclides over the integration time. For the Atlantic waters off the coast of Norway and in the southern Barents Sea, the atmospheric fallout dominates over the Sellafield release up to the mid 1960s and from the early 1990s, whereas Sellafield is the main source for the two radionuclides in the 1970s and 1980s. It is furthermore argued that model systems like the one presented here can be used for future prediction of radioactive contaminations in the Nordic Seas and the Arctic Ocean, for instance under various global warming scenarios.     

Behavior of 137Cs in soils of transitional bogs

Specific features of ¹³⁷Cs accumulation, transformation, and migration in humus-peaty and peaty-gley soils of transitional bogs are discussed with reference to the southwestern part of the Russian Federation, which was most heavily contaminated after the Chernobyl accident. The influence of physicochemical soil properties and concentrations of typomorphic elements on these processes is characterized. It is concluded that bog soils accumulate ¹³⁷Cs in the form of hardly movable compounds and, as a consequence, transitional bogs are transformed into critical ecosystems.     

Transfer of 137Cs and 60Co from irrigation water to a soil-tomato plant system

An experiment has been performed at the nuclear power plant of Garigliano (Caserta, Italy), aiming at the measurement of transfer factors of 137Cs and 60Co radionuclides from the irrigation water to a soil-plant system, with particular attention to the influence on such transfers of the irrigation technique (ground or aerial). Tomato plants were irrigated weekly with water contaminated with 137Cs and 60Co (about 375 Bq/m2 week), using both irrigation techniques. After 13 weeks, fruits, leaves, stems, roots and soil were sampled, and radionuclide concentrations were measured by high-resolution gamma spectroscopy. It was found that the activity allocated to the plant organs is significantly dependent upon the irrigation technique, amounting to 2.1% and 1.6% of the activity given in the cultivation for aerial treatment and 0.4% and 0.3% for the ground treatment, for 137Cs and 60Co respectively. The activity absorbed by plants is allocated mainly in leaves (> 55%), while less then 10% is stored in the fruits, for both irrigation techniques. Transfer factors (soil-plant and irrigation water-plant) of tomato plants and of weeds have been determined for 137Cs and 60Co, as well as for natural 40K in the soil.     

Temporal variations of natural and anthropogenic radionuclides in sea otter skull tissue in the North Pacific Ocean

Marine mammals being among the top predators in the food web tend to accumulate organic and inorganic contaminants from the environment. The body burden of contaminants in these species could reflect their foods and thus contaminant levels could serve as proxies on the changes of ecosystem. A pilot study was carried out to investigate the possibility of radionuclide leakage at Amchitka using a suite of sea otter (Enhydra lutris) skulls collected near Amchitka nuclear test-sites before (1950s) and after the testing (1990s), and at Adak, another Aleutian Island, about 300 km from Amchitka, where the potential impact of radionuclide leakage from Amchitka is expected to be negligible. In addition, the naturally occurring and anthropogenic radionuclide content on the sea otter skull was also utilized to investigate if there was any significant ecosystem changes in the environment. Concentration of 210Pb in sea otter bones collected during the 1950s was significantly higher than those collected in the 1990s. We propose that among the various factors that could cause this higher enrichment in 210Pb, changes in the sea otter prey is the most likely one. Comparison of the 137Cs, 90Sr, 239,240Pu concentrations appear not to be significantly higher in sea otter skulls collected in 1990s from Amchitka where the underground tests in 1965-71 than those from Adak, although significant differences were detected among different groups collected at various times.     

137Cs in marine samples from the Brazilian southeastern coastal region

The present work presents the results of ¹³⁷Cs concentration in seawater, fish and sediments samples collect in 11 sampling points, crossing the Brazilian Southeastern coastal region, from Vitória (ES) to Santos (SP), on a routine basis from 1997 to 2002. This monitoring program was carried out by the Instituto de Radioproteção e Dosimetria (IRD/CNEN/MCT), in cooperation with the Instituto de Estudos do Mar Almirante Paulo Moreira (IEAPM/Brazilian Navy), aiming at determining artificial radionuclides in marine samples. Additionally to the ¹³⁷Cs results, ⁹⁰Sr concentrations in fish samples from 1998 to 2002 are also reported.The ¹³⁷Cs in seawater follows a lognormal distribution, with a geometric mean of 1.8 Bq m^-3 and a geometric standard deviation of 1.4 (n=54), decay corrected to June/2002. For ¹³⁷Cs levels in fish samples a geometric mean of 0.19 Bq kg⁻¹ and a geometric standard deviation of 2.9 (n=39), decay corrected to June/2002, with a range of 0.03 to 1.7 Bq kg⁻¹, were obtained. Based on the ¹³⁷Cs mean concentration in fish as well as in seawater, a transfer factor of 1 × 10² was calculated, which is quite in agreement with the recommended value found in the Safety Report Serie 19.     

Frequency distributions of 137Cs in fish and mammal populations

We collected fish and mammals in several radioactively contaminated locations in the Chornobyl Exclusion Zone and analyzed them for 137Cs content. Frequency distributions were built for populations of channel catfish, yellow-necked mice and bank voles. We combined our data with similar data from several other studies to demonstrate the relationship between the standard deviations and means of 137Cs of fish and mammal populations. The frequency distributions of 137Cs in populations of fish and mammals are not normal, as indicated by the strong relationship between standard deviation and mean. Distributions for mammals are more skewed than those for fish. Fish and mammals probably use their environments in fundamentally different ways. The highest concentrations and thus greatest risks are therefore confined to relatively few individuals in each population.     

Ecological half-life of 137Cs in lichens in an alpine region

About 17 years after the Chernobyl accident, lichen samples were collected in an alpine region in Austria (Bad Gastein), which was heavily contaminated by the Chernobyl fallout. Measured 137Cs activity concentrations in selected lichens (Cetraria islandica, Cetraria cucullata, and Cladonia arbuscula) ranged from 100 to 1100 Bq kg(-1) dry weight, depending on lichen species and sampling site. Ecological half-lives for 137Cs in different lichen samples, obtained by comparison with earlier measurements of the same lichen species at the same site, ranged from 2 to 6 years, with average values between 3 and 4 years. Comparison with earlier studies indicated that ecological half-lives hardly changed during the last 10 years, suggesting that ecological clearance mechanisms (e.g. washout or soil transfer) did not vary substantially at the selected sampling area.     

Levels of 137Cs in muddy sediments on the seabed in the Bay of Cadiz (Spain). Part II. Model of vertical migration of (137)Cs

This second part of the study reports the development of a model to describe the vertical migration of the artificial radioisotope (137)Cs in the sediment column on the seabed of the Bay of Cadiz. The application of the model provides an overall picture of the process of sedimentation in the Inner Bay of Cadiz. The spatial distribution of the rate of sedimentation enables us to study the sources of sediments and the means by which the sediments have been transported. A method has been derived from the rate of sedimentation to perform the dating of the layers of sediment. The model describes the behaviour of (137)Cs in the area under study, taking into account the time of residence in the zones that are the source of accumulation, the origin of the sedimentary material, together with the diffusion of the radionuclide in the sediment of the seabed.