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 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.     

Correlations between potassium, rubidium and cesium ((133)Cs and (137)Cs) in sporocarps of Suillus variegatus in a Swedish boreal forest

An analysis of sporocarps of ectomycorrhizal fungi Suillus variegatus assessed whether cesium (¹³³Cs and ¹³⁷Cs) uptake was correlated with potassium (K) or rubidium (Rb) uptake. The question was whether intraspecific correlations of Rb, K and ¹³³Cs mass concentrations with ¹³⁷Cs activity concentrations in sporocarps were higher within, rather than among, different fungal species, and if genotypic origin of sporocarps within a population affected uptake and correlation. Sporocarps (n = 51) from a Swedish forest population affected by the fallout after the Chernobyl accident were studied. The concentrations were 31.9 ± 6.79 g kg⁻¹ for K (mean ± SD, dwt), 0.40 ± 0.09 g kg⁻¹ for Rb, 8.7 ± 4.36 mg kg⁻¹ for ¹³³Cs and 63.7 ± 24.2 kBq kg⁻¹ for ¹³⁷Cs. The mass concentrations of ¹³³Cs correlated with ¹³⁷Cs activity concentrations (r = 0.61). There was correlation between both ¹³³Cs concentrations (r = 0.75) and ¹³⁷Cs activity concentrations (r = 0.44) and Rb, but the ¹³⁷Cs/¹³³Cs isotopic ratio negatively correlated with Rb concentration. Concentrations of K and Rb were weakly correlated (r = 0.51). The ¹³³Cs mass concentrations, ¹³⁷Cs activity concentrations and ¹³⁷Cs/¹³³Cs isotopic ratios did not correlate with K concentrations. No differences between, within or, among genotypes in S. variegatus were found. This suggested the relationships between K, Rb, ¹³³Cs and ¹³⁷Cs in sporocarps of S. variegatus is similar to other fungal species.     

Effect of liming on the behaviour of (90)Sr and (137)Cs in a lake ecosystem

Liming of lakes is considered one possible remedial action to reduce the accumulation of radionuclides into fish in the case of a radiological accident. These responses were tested in field conditions in a small acidified lake that was divided into two parts: one limed with CaCO₃ and the other half left as an unlimed control. The transfer of ⁹⁰Sr from water into fish decreased on average by 50% during the first year after liming. However, at the same time the ⁹⁰Sr concentration in water increased, reaching a maximum within 6 months after liming. Approximately 50% more ⁹⁰Sr was detected in water in the limed part of the lake than on control side during the first year. ⁹⁰Sr was most probably released from the sediment as the Ca concentration and pH of the water increased. As a result of these two processes, which counterbalanced each other (increased release of ⁹⁰Sr into water from sediment and decreased transfer of ⁹⁰Sr from water into fish), the ⁹⁰Sr concentration in fish did not notably differ between the limed and control sides of the lake. Liming may only be suitable as a remedial action if carried out immediately after a radiological accident, before significant amounts of radionuclides have been deposited in lake sediments. In the case of ¹³⁷Cs, the effect of liming was less pronounced. ¹³⁷Cs activity concentration in water increased in the first year by 20% and uptake by fish decreased by 20%.     

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.     

Concentrations of (137)Cs in summer pasture plants that reindeer feed on in the reindeer management area of Finland

Samples of summer pasture plants that reindeer feed on were collected in order to study ¹³⁷Cs concentrations in different plant species and in species nested in certain site types, and to study the regional distribution of ¹³⁷Cs in the Finnish reindeer management area. Plant species were categorized by the site types of mineral soil forest (xeric heath forest and mesic heath forest) and peatland. A third category called ’other plant species’ included plants with various site types, poorly determined species and species with poor statistics. The ¹³⁷Cs concentrations in different site types differed significantly. The mean ¹³⁷Cs concentrations of the whole reindeer management area in the xeric heath forest plant species was 44 ± 27 Bq/kg dw, in the mesic heath forest plant species 75 ± 59 Bq/kg dw and in the peatland plant species 219 ± 150 Bq/kg dw. The peatland species uptake ¹³⁷Cs more efficiently than plant species of mineral soil forests. A particularly efficient collector of ¹³⁷Cs was Trichophorum sp. It is suggested that Trichophorum sp. could be used as an indicator species for reindeer summer fodder plants. The highest concentrations of ¹³⁷Cs were found in Southern Lapland and the lowest in Northern Lapland. Today, the concentrations of ¹³⁷Cs in summer pasture plants that reindeer feed on in Finland are at such a level that there is no need to avoid any plant species. In the case of future nuclear fallout, reindeer grazing in peatlands would increase concentrations of ¹³⁷Cs in reindeer meat.     

Cs,Co and K uptake by lettuce plants in two distributions of soil contamination

¹³⁷Cs and ⁶⁰Co, two of the radionuclides more representative of discharges from nuclear facilities, are of interest for radiological protections because of their great mobility in biosphere and affinity with biological systems. The aim of the present work is the investigation of the possible influence of the vertical distribution of ¹³⁷Cs and ⁶⁰Co in soil upon their uptake by lettuce as function of plant's growth. An experiment ad hoc has been carried out in field conditions. The results show that (i) the transfer of ¹³⁷Cs and ⁶⁰Co from soil to lettuce is independent by their distribution in soil, (ii) the soil–plant transfer factors of ¹³⁷Cs and ⁶⁰Co show a similar trend vs. growth stage, (iii) the ⁴⁰K transfer factor trend is different from those of anthropogenic radionuclides, and (iv) ¹³⁷Cs and ⁶⁰Co specific activities are about 1 Bq/kg, in the mature vegetable with soil activity from 9 to 21 kBq/m².     

Analysis of Factors Determining Accumulation of 137Cs by Woody Plants

The accumulation of ¹³⁷Cs by coniferous (Pinus sylvestris) and deciduous (Betula pendula) trees was studied in the area contaminated with radioactive products after the Chernobyl accident. The availability of ¹³⁷Cs to woody plants is determined by its vertical distribution in the soil profile, the proportion of its exchangeable form, and the distribution of tree roots in the soil. The index of biological availability of ¹³⁷C in the soil is proposed, and its linear dependence on the coefficients of ¹³⁷Cs transfer to wood is demonstrated.     

Determination of Cs in the water system of a pre-Alpine lake

The aim of this study was to measure the ¹³⁷Cs activity derived from the Chernobyl accident in the water system of Lake Wallersee, a pre-Alpine lake in Austria within an area highly contaminated by the Chernobyl fallout.     

Plutonium, 137Cs and 90Sr in selected invertebrates from some areas around Chernobyl nuclear power plant

Results are presented for ¹³⁷Cs, ⁹⁰Sr and plutonium activity concentrations in more than 20 samples of terrestrial invertebrates, including species of beetles, ants, spiders and millipedes, collected in the highly contaminated area of the Chernobyl exclusion zone. The majority of samples were collected in Belarus, with some also collected in the Ukraine. Three other samples were collected in an area of lower contamination. Results show that seven samples exceed an activity concentration of 100 kBq/kg (ash weight - a.w.) for ¹³⁷Cs. The maximum activity concentration for this isotope was 1.52 ± 0.08 MBq/kg (a.w.) determined in ants (Formica cynerea). Seven results for ⁹⁰Sr exceeded 100 kBq/kg (a.w.), mostly for millipedes. Relatively high plutonium activity concentrations were found in some ants and earth-boring dung beetles. Analyses of activity ratios showed differences in transfer of radionuclides between species. To reveal the correlation structure of the multivariate data set, the Partial Least-Squares method (PLS) was used. Results of the PLS model suggest that high radiocesium activity concentrations in animal bodies can be expected mainly for relatively small creatures living on the litter surface. In contrast, high strontium activity concentrations can be expected for creatures which conduct their lives within litter, having mixed trophic habits and a moderate lifespan. No clear conclusions could be made for plutonium.     

Determining floodplain sedimentation rates using Cs in a low fallout environment dominated by channel- and cultivation-derived sediment inputs, central Queensland, Australia

Fallout ¹³⁷Cs has been widely used to determine floodplain sedimentation rates in temperate environments, particularly in the northern hemisphere. Its application in low fallout, tropical environments in the southern hemisphere has been limited. In this study we assess the utility of ¹³⁷Cs for determining rates of floodplain sedimentation in a dry-tropical catchment in central Queensland, Australia. Floodplain and reference site cores were analysed in two centimetre increments, depth profiles were produced and total ¹³⁷Cs inventories calculated from the detailed profile data. Information on the rates of ¹³⁷Cs migration through local soils was obtained from the reference site soil cores. This data was used in an advection–diffusion model to account of ¹³⁷Cs mobility in floodplain sediment cores. This allowed sedimentation rates to be determined without the first year of detection for ¹³⁷Cs being known and without having to assume that ¹³⁷Cs remains immobile following deposition. Caesium-137 depth profiles in this environment are demonstrated to be an effective way of determining floodplain sedimentation rates. The total ¹³⁷Cs inventory approach was found to be less successful, with only one of the three sites analysed being in unequivocal agreement with the depth profile results. The input of sediment from catchment sources that have little, or no, ¹³⁷Cs attached results in true depositional sites having total inventories that are not significantly different from those of undisturbed reference sites.     

Adsorption models of Cs radionuclide and Sr (II) on some Egyptian soils

Distribution of cesium (¹³⁴Cs and ¹³⁷Cs) and strontium (Sr-II) between soil/water phases depends on many factors such as concentration of these ions between phases, the cation exchange capacity (CEC) of the soil as well as its clay content, chemical composition (especially Na, K, Ca, and Mg ions), grain size distribution, calcite, iron oxide content, and organic coatings. Distribution coefficients (Kd) of cesium (labeled with ¹³⁷Cs) and strontium were measured on the grain size distributions ≥32 μm of four soil samples. These soils were obtained from four different locations within Inshas site in Egypt and three groundwater samples were obtained from the same site locations. X-ray diffraction showed that the soil samples consisted mainly of quartz mixed with the minor amounts of kaolonite and clay minerals. Sorption experiments were carried out at strontium aqueous concentrations range 10⁻⁷ to 10⁻⁴ mol l⁻¹. The CEC and Kds for cesium and strontium were measured at the same metal concentrations range. Distribution coefficients of cesium were found to be influenced by the composition of the soil, while the distribution coefficients of strontium were found to depend on calcium concentrations in the soil/groundwater system. The aim of this study was to determine the safety assessment of disposal ¹³⁷Cs radionuclide and Sr(II) in the aquifer regions inside the Inshas site. Sequential extraction tests showed that, strontium was associated with the carbonate fractions and majority of cesium was sorbed on the iron oxides and the residue.     

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.     

Time-dependency of the Cs contamination of wild boar from a region in Southern Germany in the years 1998 to 2008

Following the Chernobyl accident, ¹³⁷Cs contamination levels of wild boar in some districts of Southern Germany are still exceeding thousands of Bq kg⁻¹. While the long term ¹³⁷Cs concentration in forest plants, mushrooms, and roe deer meat has decreased significantly, for wild boar it has remained constant during the last decade. Between 1998 and 2008, we analysed the muscle meat of 656 wild boars shot in the district (“Landkreis”) Ravensburg. The ¹³⁷Cs activity concentration showed considerable variability from less than 5 up to 8266 Bq kg⁻¹ and it followed a seasonal pattern, which is attributed to changes in dietary habits, fodder availability, meteorological conditions and specific behaviour of ¹³⁷Cs in wild boar organism. T_ag values for wild boars from the district Ravensburg varied from 0.008 to 0.062 m² kg⁻¹ during 2000–2008.     

Recent changes in Red Lake (Romania) sedimentation rate determined from depth profiles of Pb and Cs radioisotopes

This work presents a first estimation of the sedimentation rate for the Red Lake (Romania). The sediment accumulation rates were determined by two well-known methods for recent sediment dating: ²¹⁰Pb and ¹³⁷Cs methods. Both techniques implied used the gamma emission of the above-mentioned radionuclides. The ²¹⁰Pb and ¹³⁷Cs concentrations in the sediment were measured using a gamma spectrometer with a HpGe detector, Gamma-X type. Activities ranging from 41 ± 7 to 135 ± 34 Bq/kg were found for ²¹⁰Pb and from 3 ± 0.5 to 1054 ± 150 Bq/kg for ¹³⁷Cs. The sediment profile indicates acceleration in sedimentation rate in the last 18 years. Thus, the sedimentation process for the Red Lake can be divided in two periods, the last 18 years, and respectively, the period before that. Using the Constant Rate of ²¹⁰Pb Supply method values between 0.18 ± 0.04 and 1.85 ± 0.5 g/cm² year (0.32 ± 0.08 and 2.83 ± 0.7 cm/year) were obtained. Considering both periods, an average sedimentation rate of 0.87 ± 0.17 g/cm² year (1.17 cm/year) was calculated. Considering an average depth of 5.41 m for the lake and the sedimentation rate estimated for the last 18 years, it could be estimated that the lake will disappear in 195 years.     

Inventories of Pu, Cs, and excess Pb in sediments from freshwater and brackish lakes in Rokkasho, Japan, adjacent to a spent nuclear fuel reprocessing plant

We investigated the vertical profiles of ^239+240Pu, ¹³⁷Cs, and excess ²¹⁰Pb (²¹⁰Pb_ex) in sediment core samples obtained from two freshwater lakes and two brackish lakes situated near the first commercial spent nuclear fuel reprocessing plant in Rokkasho, Japan, before the final test of the plant using actual spent nuclear fuel. The inventory of ^239+240Pu in those lakes was larger than that in soil in Rokkasho, which indicated the inflow of ^239+240Pu from the catchment area in addition to direct deposition on the lake surfaces. The ¹³⁷Cs inventory in sediments of the brackish lakes was lower than that in the soil, which showed that part of the ¹³⁷Cs was removed from the sediments by the brackish water or that it was not deposited into the sediments, because of the high solubility of Cs in brackish water. The ¹³⁷Cs inventory in sediments of the freshwater lakes was higher than that of the brackish lakes, and comparable with that in soil except for one core sample out of four. The ^239+240Pu/¹³⁷Cs ratio in freshwater lake sediments was higher than that in soil, and that indicated that part of the ¹³⁷Cs was lost from the sediments. The low inventory of ¹³⁷Cs may be attributable to competition for absorption sites in sediments with ammonium ions formed in the reducing environment which occurs from summer to fall in the sediments. Those data will be used as background data on the artificial radionuclides in the lakes to assess the effect of released radionuclides on their concentrations.     

Laboratory studies of the diffusive transport of Cs and Co through potential waste repository soils

Tests using reconstituted samples have been performed to assess the diffusive transport of ¹³⁷Cs and ⁶⁰Co through natural regolith materials from a region in South Australia being considered for a radioactive waste repository. A double diffusion cell apparatus made of polycarbonate resin was developed to estimate the effective diffusion (D_e) and sorption coefficients (K_d) that allowed large withdrawals from the source and collector cells and has enabled tests with low concentrations of radioactivity. An alternative to porous stainless steel filter plates has also been used to reduce uncertainty in test interpretation. Analysis of the transient data used a staged method of the Laplace transform to take into consideration the volume of the samples withdrawn from the apparatus during testing. At test completion samples were cut into slices and analysed for radionuclide concentration. Data obtained from the sliced samples confirmed that both numerical and experimental data produced acceptable mass balance. The D_e values obtained in this study were of the order of 10⁻⁶ cm² s⁻¹ for both species, higher than previously published data. The K_d values from the diffusion and batch sorption tests were in reasonable agreement for ¹³⁷Cs, but an order of magnitude different for ⁶⁰Co. The sorption of the latter radionuclide was strongly pH dependent, and this dependency during diffusion tests would benefit from further investigation.     

Long-term dynamics of radioactive <Superscript>90</Superscript>Sr and <Superscript>137</Superscript>Cs contamination of small mammals in the Chernobyl zone

Between 1986 and 1994, a decrease in nonalimentary ⁹⁰Sr and ¹³⁷Cs intake and changes in the accessibility of radionuclides in the soil-plant link of their cycle resulted in a 10-to 100-fold decrease in their specific activity (SA) in the bodies of small mammals inhabiting the Chernobyl zone, and a similar decrease was observed in the radionuclide transition factor (TF) in the soil-animal chain. Between 1995 and 2005, no consistent increase or decrease in SA or TF could be revealed against the background of a combined effect of different physicochemical and ecological factors. It is suggested that subsequent changes in the level of radioactive contamination of small mammals will generally reflect only the dynamics of physical ⁹⁰Sr and ¹³⁷Cs decay, but, nevertheless, seasonal and local variations in this level will be significant.     

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.