137Cs and (239+240)Pu levels in the Asia-Pacific regional seas

137Cs and (239+240)Pu data in seawater, sediment and biota from the regional seas of Asia-Pacific extending from 50 degrees N to 60 degrees S latitude and 60 degrees E to 180 degrees E longitude based on the Asia-Pacific Marine Radioactivity Database (ASPAMARD) are presented and discussed. 137Cs levels in surface seawater have been declining to its present median value of about 3 Bq/m3 due mainly to radioactive decay, transport processes, and the absence of new significant inputs. (239+240)Pu levels in surface seawater are much lower, with a median of about 6 mBq/m3. (239+240)Pu appears to be partly scavenged by particles and is therefore more readily transported down the water column. As with seawater, (239+240)Pu concentrations are lower than 137Cs in surface sediment. The median 137Cs concentration in surface sediment is 1.4 Bq/kg dry, while that of (239+240)Pu is only 0.2 Bq/kg dry. The vertical profiles of both 137Cs and (239+240)Pu in the sediment column of coastal areas are different from deep seas which can be attributed to the higher sedimentation rates and additional contribution of run-offs from terrestrial catchment areas in the coastal zone. Comparable data for biota are far less extensive than those for seawater and sediment. The median 137Cs concentration in fish (0.2 Bq/kg wet) is higher than in crustaceans (0.1 Bq/kg wet) or mollusks (0.1 Bq/kg wet). Benchmark values (as of 2001) for 137Cs and (239+240)Pu concentrations in seawater, sediment and biota are established to serve as reference values against which the impact of future anthropogenic inputs can be assessed. ASPAMARD represents one of the most comprehensive compilations of available data on 137Cs and (239+240)Pu in particular, and other anthropogenic as well as natural radionuclides in seawater, sediment and biota from the Asia-Pacific regional seas.     

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.     

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.     

Equilibrium of radiocesium with stable cesium within the biological cycle of contaminated forest ecosystems

Concentrations of (137)Cs and stable Cs were determined in plant, mushroom, lichen and soil samples collected at two forest sites with different contamination levels in Belarus in 1998. The concentration of (137)Cs in soil was the highest in near-surface organic layers (Of and Oh horizons) and decreased with depth in the mineral layers, whereas the concentrations of stable Cs were almost constant in the soil profile. The levels of (137)Cs and stable Cs in biological samples varied depending both on the species and the plant part sampled. Even though different species and parts of the same species were included, the concentration ratios of (137)Cs to stable Cs were fairly constant for samples collected at the same forest site, and were in the same order of magnitude as the (137)Cs to stable Cs ratios for the organic soil layers. This finding suggests that (137)Cs, mainly deposited on the forest ecosystems from the Chernobyl accident in 1986, was well mixed with stable Cs within the biological cycle in the forest ecosystems by 1998. The transfer factor for each biological sample of (137)Cs was almost the same as that of stable Cs, if they were calculated based on the concentrations in the Of + Oh layer. This suggests that the stable-Cs-based transfer factor could be used as equilibrium transfer factor of (137)Cs for different types of biological samples in the forest.     

Comparative estimations of 137Cs distribution in a boreal forest in northern Sweden using a traditional sampling approach and a portable NaI detector

Field-portable detectors have been frequently used in routine monitoring and hazard assessment studies. However, there have been few thorough attempts to evaluate their potential as an alternative to the traditional procedure of collecting samples and analysing them in the laboratory. Thus, in this study the two approaches were compared in terms of their utility for monitoring (137)Cs activity in the Ny?nget catchment in northern Sweden. The objectives were: (i) to determine the (137)Cs activity in soils associated with three types of vegetation, (ii) to map the geographical distribution of (137)Cs using the portable NaI detector connected to a GPS system (GDM-40), (iii) to identify (137)Cs anomalies in the catchment, and (iv) to compare the measurements obtained with the NaI detector and traditional sampling followed by laboratory analysis. Our results demonstrate that the GDM-40 has very good potential for making (137)Cs inventories and for detecting (137)Cs anomalies within large areas. The GDM-40 measurements identified differences between different hydrological areas that were not determined with the soil sampling method. The GDM-40 method is much faster than a traditional soil sampling method. However, soil sampling cannot be totally excluded because it is needed to calibrate the GDM-40. The agreement between the (137)Cs activity values obtained by the two approaches was 20% which is good in the field where so many factors vary.     

Preliminary evaluation of (135)Cs/(137)Cs as a forensic tool for identifying source of radioactive contamination

Ratios of the fission products (135)Cs and (137)Cs were determined in soil and sediment samples contaminated from three different sources, to assess the use of (135)Cs/(137)Cs as an indicator of source of radioactive contamination. Soil samples from the Chernobyl exclusion zone were found to have to be heavily depleted in (135)Cs ((135)Cs/(137)Cs approximately 0.45), indicative of a high thermal neutron flux at the source. Sludge samples from a nuclear waste treatment pond were found to have a (135)Cs/(137)Cs ratio of approximately 1, whereas sediment collected downstream from a nuclear reactor was highly variable in both (137)Cs activity and (135)Cs/(137)Cs ratio. Comparison of these preliminary results of variability in radiocaesium isotope ratios with reports of Pu isotope ratios suggests (135)Cs/(137)Cs similarly varies with fuel and reactor conditions, and may be used to corroborate other methods of characterizing radioactive contamination.     

Radiocesium storage in soil microbial biomass of undisturbed alpine meadow soils and its relation to 137Cs soil-plant transfer

This study focuses on radiocesium storage in soil microbial biomass of undisturbed alpine meadow sites and its relation to the soil-to-plant transfer. Soil and plant samples were taken in August 1999 from an altitude transect (800-1600m.a.s.l.) at Gastein valley, Austria. Soil samples were subdivided into 3-cm layers for analyses of total, K(2)SO(4)-extractable and microbially stored (137)Cs. Microbial biomass was measured by the fumigation extraction method, and fungal biomass was quantified using ergosterol as biomarker molecule. In general, the quantity of (137)Cs stored in the living soil microbial biomass was relatively small. At the high-altitude meadows, showing high amounts of fungal biomass, microbially stored (137)Cs amounted to 0.64+/-0.14kBqm(-2) which corresponds to about 1.2-2.7% of the total (137)Cs soil inventory. At lower altitudes, microbial (137)Cs content was distinctly smaller and in most cases not measurable at all using the fumigation extraction method. However, a positive correlation between the observed soil-to-plant aggregated transfer factor, microbially stored (137)Cs and fungal biomass was found, which indicates a possible role of fungal biomass in the storage and turnover of (137)Cs in soils and in the (137)Cs uptake by plants.     

Application of the Weibull extrapolation to 137Cs geochronology in Tokyo Bay and Ise Bay, Japan

Considerable doubt surrounds the nature of processes by which 137Cs is deposited in marine sediments, leading to a situation where 137Cs geochronology cannot be always applied suitably. Based on extrapolation with Weibull distribution, the maximum concentration of 137Cs derived from asymptotic values for cumulative specific inventory was used to re-establish 137Cs geochronology, instead of original 137Cs profiles. Corresponding dating results for cores in Tokyo Bay and Ise Bay, Japan, by means of this new method, are in much closer agreement with those calculated from 210Pb method than the previous method.     

A rapid method for 90Sr determination in the presence of 137Cs in environmental samples

A rapid method for the determination of 90Sr in the presence of 137Cs using the Cherenkov radiation technique is described. The contribution of 137Cs to gross Cherenkov radiation (90Y + 137Cs) was examined for 137Cs /90Sr ratios ranging from 0.09 to 2.50 for 137Cs activities ranging from 2 to 1,211 Bq. Results from direct Cherenkov radiation measurement and results after radiochemical separation of 90Y from 90Sr for samples containing both 90Sr and 137Cs were compared. Errors below 5% were obtained for 137Cs /90Sr ratios lower than 1, when no separation was performed, independently of the activity level. However, errors between 10% and 35% were obtained for 137Cs/90Sr ratios higher than 1. In order to determine 90Sr activity in the presence of 137Cs using the Cherenkov technique, a multiple linear regression analysis model was established to correct the data for 137Cs content. The mathematical correction proposed was validated using 66 artificially contaminated lettuce samples in a laboratory experiment by taking into account the activity levels of 137Cs and 90Sr and the radionuclide ratios. Comparison of mathematically corrected radionuclide ratios with the results obtained without correction shows that, for radionuclide ratios higher than 1, error values for measuring 90Sr activity using the mathematical model were much smaller than when no radiochemical separation was performed. On the other hand, for ratios lower than 1, error values when measuring 90Sr activity with radiochemical separation were smaller than when mathematical correction was performed. In spite of this, the mathematical correction is an appropriate way of reducing the time needed to determine radiostrontium using the Cherenkov radiation technique. The method proposed could be a powerful tool for environmental research whenever the contents of 90Sr and 137Cs have to be determined.     

Deposition of 137Cs in Rokkasho, Japan and its relation to Asian dust

Biweekly atmospheric depositions of (137)Cs were measured in Rokkasho, Aomori, Japan from March 2000 to March 2006 to study recent (137)Cs deposition. Although the deposition level was generally lower than the detectable limit, deposition samples collected in spring occasionally had measurable levels of (137)Cs. The annual (137)Cs deposition from 2001 to 2005 was 0.04-0.69 Bq m(-2) with a mean value of 0.27 Bq m(-2). Depositions of insoluble Al, Fe and Ti were strongly correlated with the (137)Cs deposition, suggesting that suspension of soil particles was the main source of the recent (137)Cs deposition. Asian dust events were coincident with some of the significant (137)Cs depositions in spring. It was found that the ratios of (137)Cs/Al and Fe/Al could be used as indices for discriminating Asian dust from suspension of the local surface soil. Backward trajectory analysis suggested southern Mongolian and northeastern China regions as sources of the significant (137)Cs depositions.     

Long-term flux of Chernobyl-derived 137Cs from soil to French rivers: a study on sediment and biological indicators

Sediment and aquatic plants were collected annually since the early 1990s in the main French rivers, upstream of nuclear power plants. These time series were used in order to assess the parameters of a compartmental model describing the Chernobyl-derived (137)Cs flux from soil to rivers. In order to reduce the dispersal of (137)Cs measured activities in sediment samples due to the granulometric heterogeneity, a correction method was set up using sediment test-fractions artificially enriched with specific diameter particles. The method was based on (137)Cs affinity for fine particles, especially clays, and thus clay and fine silt contents of each sample was analysed. Corrected sediment data showed (1) that the method efficiently reduced the variability; and (2) that (137)Cs activities in French rivers decreased with a half-life of 4 to 6 years since 1987 (after correction by radioactive decay). A similar half-life value was obtained for aquatic plants pointing out that this half-life is related to the gradual decay of the flux from soil to rivers, not to the indicator itself. Comparing our results with similar ones published by other authors, it appeared possible that this kinetic varies with the time period over which the study is conducted, the longer the period the lower is the kinetic.     

Radionuclide tracing of water masses and processes in the water column and sediment in the Algerian Basin

Caesium-137 and (239,240)PU were analysed in the water column along the Algerian coast. The (137)Cs activity concentration in surface water increased from the west to the east from 1.6 to 3.3 mBq L(-1), documenting a presence of Modified Atlantic Water (MAW) in the region. Higher concentrations observed in deep waters may be due to an intrusion of Levantine Intermediate Water (LIW), which has been carrying higher levels of (137)Cs from Chernobyl accident. The (239,240)Pu sub-surface concentration peaked at about 250 m water depth as a result of biogeochemical processes in the water column. The observed (239,240)Pu/(137)Cs activity ratio at the surface (0.003) was significantly lower than that in global fallout (0.04). This decrease exceeds that expected from radioactive decay of (137)Cs, and confirms that Pu due to its adsorption on sinking particles is more effectively removed from surface layers than is (137)Cs. An increase of the (239,240)Pu/(137)Cs activity ratio with depth suggests that (239,240)Pu, similarly as (137)Cs, should be also transported by advection to maintain the observed ratios in deep waters. An intrusion of LIW may enhance therefore both the (137)Cs and (239,240)Pu concentrations in deep waters. The average (238)Pu/(239+240)Pu activity ratio in seawater was 0.03+/-0.02, confirming a global fallout origin of Pu in the Algerian Basin. Caesium-137 and (239,240)Pu inventories in the water column were estimated to be from 2.7+/-0.5 kBq m(-2) to 3.8+/-0.7 kBq m(-2), and from 13.8+/-2.6 Bq m(-2) to 41+/-7B qm(-2), respectively. The (137)Cs massic activities in surface sediment were almost constant, the average activity was 9.0+/-0.8 Bq kg(-1). Sedimentation rates obtained using the (210)Pb method were from 0.1 to 0.7 cm y(-1), and resulting penetration depths of (137)Cs in the sediment cores were from 15 to over 40 cm. The (137)Cs peaks found in the sediment cores were associated with the Chernobyl accident (1986) and global fallout (1964). The (137)Cs inventories in the sediment were increasing from the west (180 Bq m(-2)) to the east (350 Bq m(-2)).     

A new method to account for the depth distribution of 137Cs in soils in the calculation of external radiation dose-rate

This work reports a new method for calculating the external dose-rate as a function of height above land that has been contaminated with a surface deposition of (137)Cs. Unlike previous work this method accounts for vertical migration of (137)Cs using the Advection Dispersion Equation (ADE) with appropriate parameters. The results have been successfully verified with field measurements from the (137)Cs contaminated regions within the Republic of Belarus. The method also correctly predicts the observed variation of dose-rate with elevation above the soil surface and it is shown how this method can be used to predict the reduction in surface dose-rate after remediation measures such as deep ploughing have taken place.     

A simplified 137Cs transport model for estimating erosion rates in undisturbed soil

(137)Cs is an artificial radionuclide with a half-life of 30.12 years which released into the environment as a result of atmospheric testing of thermo-nuclear weapons primarily during the period of 1950s-1970s with the maximum rate of (137)Cs fallout from atmosphere in 1963. (137)Cs fallout is strongly and rapidly adsorbed by fine particles in the surface horizons of the soil, when it falls down on the ground mostly with precipitation. Its subsequent redistribution is associated with movements of the soil or sediment particles. The (137)Cs nuclide tracing technique has been used for assessment of soil losses for both undisturbed and cultivated soils. For undisturbed soils, a simple profile-shape model was developed in 1990 to describe the (137)Cs depth distribution in profile, where the maximum (137)Cs occurs in the surface horizon and it exponentially decreases with depth. The model implied that the total (137)Cs fallout amount deposited on the earth surface in 1963 and the (137)Cs profile shape has not changed with time. The model has been widely used for assessment of soil losses on undisturbed land. However, temporal variations of (137)Cs depth distribution in undisturbed soils after its deposition on the ground due to downward transport processes are not considered in the previous simple profile-shape model. Thus, the soil losses are overestimated by the model. On the base of the erosion assessment model developed by Walling, D.E., He, Q. [1999. Improved models for estimating soil erosion rates from cesium-137 measurements. Journal of Environmental Quality 28, 611-622], we discuss the (137)Cs transport process in the eroded soil profile and make some simplification to the model, develop a method to estimate the soil erosion rate more expediently. To compare the soil erosion rates calculated by the simple profile-shape model and the simple transport model, the soil losses related to different (137)Cs loss proportions of the reference inventory at the Kaixian site of the Three Gorge Region, China are estimated by the two models. The over-estimation of the soil loss by using the previous simple profile-shape model obviously increases with the time period from the sampling year to the year of 1963 and (137)Cs loss proportion of the reference inventory. As to 20-80% of (137)Cs loss proportions of the reference inventory at the Kaixian site in 2004, the annual soil loss depths estimated by the new simplified transport process model are only 57.90-56.24% of the values estimated by the previous model.     

Foliar and root uptake of 134Cs, 85Sr and 65Zn in processing tomato plants (Lycopersicon esculentum Mill.)

Rice is a staple food in Japan and other Asian countries, and the soil-to-plant transfer factor of 137Cs released into the environment is an important parameter for estimating the internal radiation dose from food ingestion. Soil and rice grain samples were collected from 20 paddy fields throughout Aomori Prefecture, Japan in 1996 and 1997, and soil-to-polished rice transfer factors were determined. The concentrations of 137Cs, derived from fallout depositions, stable Cs and K in paddy soils were 2.5-21 Bq kg(-1), 1.2-5.3 and 5000-13000 mg kg(-1), respectively. The ranges of 137Cs, stable Cs and K concentration in polished rice were 2.5-85 mBq kg(-1) dry wt., 0.0005-0.0065 and 580-910 mg kg(-1) dry wt., respectively. The geometric mean of soil-to-polished rice transfer factor of 137Cs was 0.0016, and its 95% confidence interval was 0.00021-0.012. The transfer factor of 137Cs was approximately 3 times higher than that of stable Cs at 0.00056, and they were well correlated. This implied that fallout 137Cs, mostly deposited up to the 1980s, is more mobile and more easily absorbed by plants than stable Cs in the soil, although the soil-to-plant transfer of stable Cs can be used for predicting the long-term transfer of 137Cs. The transfer factors of both 137Cs and stable Cs decreased with increasing K concentration in the soil. This suggests that K in the soil was a competitive factor for the transfers of both 137Cs and stable Cs from soil-to-polished rice. However, the transfer factors of 137Cs and stable Cs were independent of the amount of organic materials in soils.     

Bioaccumulation of 137Cs in pelagic food webs in the Norwegian and Barents Seas

Knowledge and documentation of the levels of radioactive contamination in fish stocks important to Norwegian fisheries is of major importance to Norwegian consumers and fish export industry. In the present study, the bioaccumulation of caesium-137 ((137)Cs) has been investigated in marine food webs in the Barents and Norwegian Seas. The contents of (137)Cs in the different organisms were generally low (<1 Bq kg(-1) wet weight), but a marked bioaccumulation was apparent: The concentration of (137)Cs was about 10-fold higher in the harbour porpoise Phocoena phocoena, representing the upper level of the food web, than in the amphipod Themisto sp., representing the lower level of the food web. The Concentration Factors (CF=Bq kg(-1) wet weight/Bq l(-1) seawater) increased from 10+/-3 for a mixed sample of krill and amphipods to 165+/-5 for harbour porpoises.     

Suspended particle adhesion on aquatic plant surfaces: implications for 137Cs and 133Cs uptake rates and water-to-plant concentration ratios

Suspended particle adhesion on aquatic biota can significantly increase the apparent concentration of radionuclides above their endogenous value, leading to an overestimation of the uptake rate and concentration ratios. This study is an attempt to assess quantitatively the importance of suspended particle adhesion on periphyton samples (biological material coating submerged surfaces). The concentrations of 137Cs and stable Cs (133Cs) in periphyton, suspended particles and filtered water were measured to determine the net water-to-periphyton concentration ratios for 137Cs and stable Cs. The net amount of 133Cs (or 137Cs) taken up by periphyton was calculated by subtracting from the total amount of 133Cs (or 137Cs) on the collected material (periphyton + inorganic particles), the 133Cs (or 137Cs) due to the inorganic particles adhering to periphyton. The mass of suspended particles adhering to the periphyton surface was calculated using scandium as an indicator of the mineral fraction of the suspended particles. The relationship between the concentration ratios for 137Cs and stable Cs and suspended particle adhesion on periphyton external surfaces is discussed.     

A process-based model for the partitioning of soluble, suspended particulate and bed sediment fractions of plutonium and caesium in the eastern Irish Sea

A dynamic model of plutonium behaviour in the marine environment has been developed, representing the oxidation state distribution and partitioning of plutonium between the soluble, colloidal, suspended particulate and seabed sediment fractions. With simple re-parameterisation, this model can also be applied to (137)Cs. The model, which is calibrated and validated against field data, has been used to predict concentrations of Pu(alpha) and (137)Cs in both water and seabed sediments from the vicinity of the Sellafield Ltd. reprocessing plant in Cumbria, UK. The model predicts that sediment reworking and transport are the key environmental processes as the Sellafield Pu(alpha) and (137)Cs discharge continues to decline. Inventory calculations generated by the model are consistent with previous estimations. For a hypothetical post-discharge scenario, the concentrations of these radionuclides in both seawater and surface sediments are predicted to decrease sharply, concurrent with a downward vertical migration of the activity retained in sediments.     

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.     

129I/127I, 129I/137Cs and 129I/99Tc in the Norwegian coastal current from 1980 to 1998

Discharges of the nuclides 129I, 137Cs and 99Tc from the nuclear reprocessing facilities at Sellafield (UK) and La Hague (France) are very useful as oceanic tracers. On the basis of 129I/127I, 137Cs and 99Tc measurements in archived seaweeds, the ratios of 129I/127I, 129I/137Cs and 129I/99Tc have been estimated in seawater at two locations (Utsira and Kiberg) in the Norwegian Coastal Current from 1980 to 1998. These ratios, which vary up to two orders of magnitude over this period, are potentially very interesting for determining "transit times" in the Arctic and North Atlantic oceans. While the long-term trends in these ratios are quite clear, measurements in monthly and bimonthly samples show considerable structure. Further studies are required to determine the exact origin of this structure, which may be a limiting factor in the time resolution that can be obtained with these parameters.