Activity ratios of 137Cs, 90Sr and 239+240Pu in environmental samples

Both global and Chernobyl fallout have resulted in environmental contamination with radionuclides such as 137Cs, 90Sr and 239+240Pu. In environmental samples, 137Cs and 239+240Pu can be divided into the contributions of either source, if also the isotopes 134Cs and 238Pu are measurable, based on the known isotopic ratios in global and Chernobyl fallout. No analogous method is available for 90Sr. The activity ratios of Sr to Cs and Pu, respectively, are known for the actual fallout mainly from air filter measurements; but due to the high mobility of Sr in the environment, compared to Cs and Pu, these ratios generally do not hold for the inventory many years after deposition. In this paper we suggest a method to identify the mean contributions of global and Chernobyl fallout to total Sr in soil, sediment and cryoconite samples from Alpine and pre-Alpine regions of Austria, based on a statistical evaluation of Sr/Cs/Pu radionuclide activity ratios. Results are given for Sr:Cs, Sr:Pu and Cs:Pu ratios. Comparison with fallout data shows a strong depletion of Sr against Cs and Pu.     

137Cs and 90Sr transfer to milk in Austrian alpine agriculture

The alpine regions of Austria were among the most contaminated territories outside of the former USSR after the Chernobyl accident. In the investigated province of Salzburg the median (137)Cs surface deposition was 31.4 kBq m(-2) with maximum values exceeding 90 kBq m(-2) (May 1986). To quantify the transfer of (137)Cs and (90)Sr from vegetation to milk in these seminatural conditions nine seasonally grazed alps were identified and vegetation and milk sampled during summer 2002 and summer 2003. Mean+/-SD milk transfer coefficients (fm) for (137)Cs and (90)Sr were 0.0071+/-0.0009 d l(-1), and 0.0011+/-0.0004 d l(-1), respectively; which for (137)Cs is markedly higher than those fm values found in intensive agricultural systems. Transfer kinetics for (137)Cs into cow milk were approximated using a 2-compartment model with a short and a long-term component. Fitting the model to empirical data results in reliable estimates of the time constant of the short-term component, biological half-life 1.06+/-0.28 d, whereas the estimates of the long-term component are subject to high uncertainties.     

Inventory and vertical migration of 90Sr fallout and 137Cs/90Sr ratio in Spanish mainland soils

In this paper the inventory of ⁹⁰Sr in 34 points distributed along the Spanish peninsular territory is presented. Obtained values range between 173 Bq/m² and 2047 Bq/m². From these data set and those ¹³⁷Cs data obtained in a previous work the ¹³⁷Cs/⁹⁰Sr activity ratio has been established, laying this value between 0.9 and 3.6. Also the migration depth of both radionuclides has been analysed obtaining for ¹³⁷Cs an average value 57% lower than that obtained for ⁹⁰Sr.Additionally, this paper presents the results obtained in 11 sampling points in which the activity vertical profile has been measured. These profiles have been analysed to state the behaviour of strontium in soils and after, by using a convective-diffusive model, the parameters of the model which governs the vertical migration of ⁹⁰Sr in the soil, v (apparent convection velocity) and D (apparent diffusion coefficient) have been evaluated. Mean values obtained are 0.20 cm/year and 3.67 cm²/year, respectively.     

The transfer of 137Cs and 90Sr from feed to rabbits

Radiological assessment of the impact of nuclear weapons testing on the local population in the Semipalatinsk Test Site (STS) requires comprehensive site-specific information on radionuclide behaviour in the environment. However, information on radionuclide behaviour in the conditions of the STS is rather sparse and, in particular, there are no data in the literature on parameters of radionuclide transfer from feed to rabbit products which have been identified as contributors to internal dose to the inhabitants. The transfer of (137)Cs and (90)Sr to rabbit meat was studied under laboratory conditions in a controlled experiment with 32 locally bred rabbits maintained in the Kazakh Agricultural Research Institute. The equilibrium transfer coefficients for (137)Cs and (90)Sr from feed to rabbit meat were estimated to be 0.4 d kg(-1) and 0.15 d kg(-1), respectively. The biological half-lives were estimated to be 0.1 d for (137)Cs and 0.14 d for (90)Sr. Whereas for (137)Cs the distribution in the body is relatively homogeneous, there are large differences between the organs and tissues for (90)Sr for which, as expected, the highest concentrations were found in bone.     

Uptake and distribution of 137Cs and 90Sr in salix viminalis plants

Agricultural areas in middle and northern parts of Sweden were contaminated with radionuclides after the Chernobyl accident in 1986. Alternative crops in these areas are biomass plantations with fast-growing Salix clones for energy purposes. The uptake and internal distribution of 137Cs and 90Sr in Salix viminalis were studied. Plants were grown in microplots under field conditions. The soils in the experimental site had been contaminated in 1961 with 35.7 and 13.4 MBq m(-2) of 137Cs and 90Sr, respectively. The experiment was carried out during three years. The plots were fertilised with 60 kg N ha(-1) and three treatments of K, consisting of 0, 80 and 240 kg K ha(-1) during the first two years. The activity concentration of 137Cs in the different plant parts varied between 140 and 20,000 Bq kg(-1) and was ranked in the following order: lowest in stems < cuttings < leaves < roots. The fine roots (0-1 mm) had the highest 137Cs activity concentration. One-year-old stems had higher 137Cs activity concentrations than two-year-old stems. The activity concentration of 137Cs in the plants was significantly affected by K-supply and was higher in the 0 kg K treatment than in the 80 or 240kg K treatment. Leaves contained more 90Sr than stems and cuttings.     

Ecological half-lives of 90Sr and 137Cs in terrestrial and aquatic ecosystems

This paper describes the long-term behaviour of (90)Sr and (137)Cs in foods, feeds and a variety of environmental media. The long-term behaviour is quantified by means of the ecological half-life which integrates all processes that cause a decrease of activity in a given medium such as leaching, fixation and erosion. A large number of long-term time series of concentrations of radiocaesium and radiostrontium in these media have been identified and re-evaluated using a standardised statistical procedure to establish reference data sets of ecological half-lives. By example of undisturbed soils and marine water bodies it is shown that the ecological half-life concept is questionable if the distribution of the radionuclide of interest within the medium studied is non-uniform and if mixing and transport processes within this medium, therefore, are of considerable importance during the time period of observation.     

137Cs and 90Sr behavioural regularities in the southeastern part of the Baltic Sea

Variations in 137Cs concentrations were investigated over the period 1986-1997 in the southeastern part of the Baltic Sea, following the Chernobyl power plant accident. The rate of "self-cleaning" was demonstrated to be very slow, the average concentration of 137Cs in 1996 being almost the same as that measured directly after the accident, in 1986. Measurements of both 137Cs and 90Sr concentrations generally revealed homogeneous distributions in this region of the Baltic Sea, though patchy distributions did develop under some hydrometeorological conditions. Specifically, the 137Cs concentration distribution became heterogeneous with values varying in the range 60-92 Bq/m3 under south-southwesterly wind conditions whilst the 90Sr concentration distribution developed similar characteristics with values ranging from 15 to 64 Bq/m3 under east-southeasterly wind conditions. In addition, in coastal waters, over extensive periods of north-northwesterly winds in 1995, 137Cs concentrations increased to values 1.5-2 times the overall average concentration, which was registered in 1986 and 1996. These data therefore reveal a continuing significant pollution of the waters of the Baltic Sea resulting from the Chernobyl power plant accident, a pollution compounded by the slow rate of radionuclide self-cleaning and significant probability of sudden regional concentration increase.     

Intra-cultivar variability of the soil-to-grain transfer of fallout 137Cs and 90Sr for winter wheat

Differences between the root uptake of fallout radionuclides by different cultivars ('inter-cultivar' variability) growing on the same field may be influenced not only by genetic differences of the cultivars, but also by the spatial variability of the soil-to-grain transfer within the cultivation area of each cultivar. This 'intra-cultivar' variability was investigated in 2001 and 2002 for 137Cs and 90Sr using three winter wheat cultivars with four replicates for each cultivar at three different sites in Bavaria, Germany. The intra-cultivar variability proved to be in the same range as the inter-cultivar variability which was determined earlier at the same sites for both radionuclides. An ANOVA of the 137Cs data set revealed that the variability of the 137Cs soil-to-grain transfer was caused by the soil and climate (year) at the field sites and the interaction of cultivar and field. A significant contribution of the factor 'cultivar' alone to the variability could not be detected. This may be due to the complex environmental conditions to which plants are exposed in field experiments. To find wheat cultivars with minimal uptake of fallout radionuclides it may be better to examine the molecular mechanisms of their root uptake in order to identify targets for breeding "safer" plants.     

A pilot study on the transfer of 137Cs and 90Sr to horse milk and meat

The radiological assessment of the impact of nuclear weapon's testing on the Semipalatinsk Test Site (STS) on the local population requires comprehensive site-specific information on radionuclide behaviour in the environment. However, information on radionuclide behaviour in the conditions of the STS is rather sparse and, in particular, there are no data in the literature on parameters of radionuclide transfer from feed to horse products proofed to be important contributors to the internal dose to the local population. The transfer of 137Cs and 90Sr to horse milk and meat was studied under laboratory and field conditions: in controlled experiment with three lactating horses maintained in the Kazakh Agricultural Research Institute, and in field measurements of horse products taken from horses grazing at the Semipalatinsk Test Site. The equilibrium transfer factors from feed to horse milk and meat were estimated to be 0.012 dl(-1) and 0.035 dkg(-1) for (137)Cs and 0.0022 dl(-1) and 0.003 dkg(-1) for (90)Sr, respectively. The biological half-lives were approximated by a sum of two exponentials amounting to 3 (85%) and 15 (15%) days for 137Cs and 3.5 (70%) and 100 (30%) days for 90Sr. The highest 137Cs transfer has been found to be to spleen, followed by lung, heart, muscles, kidneys, intestine, and finally skin and bones. For90Sr, the maximum activity concentration was observed in bones; contamination of other tissues is rather uniform except for liver and intestine with a factor of about 2 higher than muscles.     

Distribution of 90Sr and 137Cs in Arctic soil profiles polluted by heavy metals

Effects of industrial pollution on the behaviour of radionuclides in spruce forest ecosystems were studied along a gradient from of a copper-nickel smelter in Monchegorsk, NW Russia. A reference site was situated in Lapland, Finland, 152 km west of Monchegorsk. Most of the total 137Cs activity in soil was in mineral (E and B) horizons, except at the reference site where the major part was still in the organic surface layer. Most of the total 90Sr activity still remaining in the soil profile was found in the surface layer, but the relative amount decreased with increasing level of industrial pollution. Pollutants from the smelter clearly affected the chemical speciation of radionuclides. Smaller amounts of exchangeable radionuclides were present in the organic surface layer at the most polluted sites. The decline of 137Cs with decreasing distance from the smelter correlated strongly with a similar depletion in exchangeable K and Mg. Total concentrations of 137Cs and 90Sr showed high correlations with exchangeable cations, particularly in the E and upper B horizon. A sudden change in behaviour of 137Cs in the lower B horizon may be associated with changes in clay mineralogy along the soil profile caused by weathering.     

Transfer factors of 137Cs and 90Sr from soil to trees in arid regions

Transfer factors of (137)Cs and (90)Sr from contaminated soil (Aridisol) to olive, apricot trees and grape vines were determined under irrigated field conditions for four successive years. The transfer factors (calculated as Bqkg(-1) dry plant material per Bqkg(-1) dry soil) of both radionuclides varied among tree parts and were highest in olive and apricot fruits. However, the values for (90)Sr were much higher than those for (137)Cs in all plant parts. The geometric mean of the transfer factors in olives, apricots and grapes were 0.007, 0.095 and 0.0023 for (137)Cs and 0.093, 0.13 and 0.08 for (90)Sr, respectively, and were negligible in olive oil for both radionuclides. The transfer factors of both radionuclides were similar to, or in the lower limits of, those obtained in other areas of the world. This could be attributed to differences in soil characteristics: higher pH, lower organic matter, high clay content, and higher exchangeable potassium and calcium.     

A comparison of 90Sr and 137Cs uptake in plants via three pathways at two Chernobyl-contaminated sites

Foliar absorption of resuspended 90Sr, root uptake and contamination adhering to leaf surfaces (i.e. soil loading) were compared at two Chernobyl-contaminated sites, Chistogalovka and Polesskoye. Although foliar absorption of resuspended 90Sr was quantifiable, its contribution amounted to less than 10% of the plants' total, above-ground contamination. Root uptake was 200 times greater than foliar absorption at the near-field site of Chistogalovka and eight times greater at Polesskoye, where the fallout consisted of the more soluble condensation-type, rather than fuel particles. Strontium's bioavailability exceeded that of 137Cs (analyzed in the same plants) by orders of magnitude when compared using concentration ratios. Simplistic, cumulative effective dose calculations for humans ingesting 90Sr- and 137Cs-contaminated plants revealed that the dose at Chistogalovka was greater from 90Sr (185 mSv vs. 3 mSv from 137Cs), while at Polesskoye the dose from 137Cs (66 mSv) was 30 times greater than from 90Sr (2 mSv).     

239+240Pu, 90Sr and 137Cs inventories in surface soils of Vietnam

Fallout 239+240Pu, 238Pu, 90Sr and 137Cs inventories in surface soils were measured for 20 locations in northern Vietnam yielding the mean values (+/- standard error) of 26.5+/-3.8 Bq m(-2) for 239+240Pu, 1048+/-143 Bq m(-2) for 137Cs and 212+/-28 Bq m(-2) for 90Sr. The concentrations of 137Cs and plutonium isotopes strongly correlate with each other resulting in a stable 239+240Pu/137Cs inventory ratio of 0.025+/-0.002. Among soil parameters, organic matter and fulvic acids strongly correlate with caesium and plutonium isotopes, especially in the 0-10 cm layer. 137Cs and 239+240Pu are distributed rather similarly over the 0-10 cm and 10-20 cm layers. At locations with high contents of sand (82-93%) along the South China Sea coast, the downward percolation by rainwater results in a higher accumulation of 239+240Pu and 137Cs in the 10-20 cm layer. The mean 137Cs/ 90Sr inventory ratio is 9.3+/-2.2, and the correlation is weak between these isotopes.     

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.     

Discharge of 137Cs and 90Sr by Finnish rivers to the Baltic Sea in 1986-1996

The total amounts of 137Cs and 90Sr transported from Finland by rivers into the Gulf of Finland, Gulf of Bothnia and Archipelago Sea since 1986 were estimated. The estimates were based on long-term monitoring of 137Cs and 90Sr in river and other surface waters and on the statistics of water discharges from Finnish rivers to the above sub-areas of the Baltic Sea. The total amounts of 137Cs and 90Sr removed from Finland into the Baltic Sea during 1986-1996 were estimated to be 65 and 10 TBq, respectively. The results show that, although the deposition of 137Cs was much higher than that of 90Sr after the Chernobyl accident, the amount of 137Cs removed from Finland is only six times as high as that of 90Sr. This emphasizes the importance of 90Sr while considering radiation doses from surface waters and 137Cs while estimating doses via pathways from catchment soil, lake sediments and biota after a fallout situation.     

Contamination of the southern Baltic Sea with 137Cs and 90Sr over the period 2000-2004

Changes of the (137)Cs activity concentrations in the southern Baltic Sea waters were investigated over the period 2000-2004 and distribution of the (90)Sr concentrations was determined in 2004. In the discriminated period further decrease of (137)Cs concentrations was observed. The average activity concentration of (137)Cs declined from 59.4Bq/m(3) in 2000 to 45.1Bq/m(3) in 2004. The greatest changes of (137)Cs activities occurred in 2003 as a consequence of the medium-size inflow of a saline waters from the North Sea. This inflow affected (137)Cs activities as well as its distribution in the Baltic Sea. Changes in (90)Sr activity concentrations proceeded at much slower rate. The average activity concentration of (90)Sr was equal to 8.7Bq/m(3) in 2004. The annual fluvial (137)Cs fluxes from the Vistula river were also estimated. In 2000, the (137)Cs load from Vistula was of an order of 0.15TBq/year, and in 2004 0.05TBq/year.     

Current contamination by 137Cs and 90Sr of the inhabited part of the Techa river basin in the Urals

Previous discharges of radioactivity from the Mayak Production Association plant in the Urals have resulted in considerable radionuclide contamination of the Techa River, and consequent high radiation doses during the late 1940s and 1950s to residents of villages along the Techa river. The most contaminated villages close to the site were evacuated in the period 1954-1962. The objective of this recent study was to conduct a preliminary assessment of the current radioactive contamination of soil, vegetation and foodstuffs in the two remaining villages closest to the Mayak site, Muslyumovo and Brodokalmak. The highest contamination levels in soil were found in the floodplain at 5.5 MBq m(-2) for 137Cs and 1.0 MBq m(-2) for 90Sr. Radionuclide contamination in soil of the villages was much lower, but exceeded that expected from global fallout. Data from 1207 measurements of 137Cs in milk and 1180 for 90Sr in milk for the period 1992-1999 were collated. There was no change with time in the 90Sr or 137Cs activity concentration in milk over the measured period. There were significantly higher 137Cs activity concentrations in milk sampled during the housed winter period in Muslyumovo compared with the grazing summer period, but compared to that for Brodokalmak or for either settlement for 90Sr. The highest measured activity concentrations in food products of 137Cs and 90Sr were found in river fish, waterfowl, poultry and milk. The measured activity concentrations of 137Cs and 90Sr in some animal products were higher than that expected from soil and vegetation from fields and pasture in the villages (not including the floodplain) confirming that the highly contaminated floodplains are contributing to contamination of some animal products.     

(137)Cs and (90)Sr uptake by sunflower cultivated under hydroponic conditions

The (90)Sr and (137)Cs uptake by the plant Helianthus annuus L. was studied during cultivation in a hydroponic medium. The accumulation of radioactivity in plants was measured after 2, 4, 8, 16 and 32 days of cultivation. About 12% of (137)Cs and 20% of (90)Sr accumulated during the experiments. We did not find any differences between the uptake of radioactive and stable caesium and strontium isotopes. Radioactivity distribution within the plant was determined by autoradiography. (137)Cs was present mainly in nodal segments, leaf veins and young leaves. High activity of (90)Sr was localized in leaf veins, stem, central root and stomata. The influence of stable elements or analogues on the transfer behaviour was investigated. The percentage of non-active caesium and strontium concentration in plants decreased with the increasing initial concentration of Cs or Sr in the medium. The percentage of (90)Sr activity in plants decreased with increasing initial activity of the nuclide in the medium, but the activity of (137)Cs in plants increased. The influence of K(+) and NH(4)(+) on the uptake of (137)Cs and the influence of Ca(2+) on the uptake of (90)Sr was tested. The highest accumulation of (137)Cs (24-27% of the initial activity of (137)Cs) was found in the presence of 10 mM potassium and 12 mM ammonium ions. Accumulation of about 22% of initial activity of (90)Sr was determined in plants grown on the medium with 8 mM calcium ions.     

Radioactivity concentrations of 40K, 134Cs, 137Cs, 90Sr, 241Am, 238Pu and 239+240Pu radionuclides in Jordanian soil samples

In November 2000, surface and core soil samples were collected from different regions of Jordan. The samples were analyzed by direct gamma spectrometry and combined radiochemical separation procedure to quantify (40)K, (134)Cs, (137)Cs, (90)Sr, (241)Am, (238)Pu and (239+240)Pu radioactivity. Concentrations (Bq.kg(-1) dry weight) have been observed to vary in the range 1.5-2.6 for (134)Cs, 2.8-11.4 for (90)Sr, and 0.13-0.48 for (241)Am, 0.016-0.062 for (238)Pu, 0.28-1.01 for (239+240)Pu and 155-543 for (40)K. The typical concentration of (137)Cs found in topsoils (0-2 cm) ranged in 7.5-576 Bq.kg(-1), dry weight. These values were greater than those observed in samples taken at greater depths (up to 32 cm). Activity ratios of (134)Cs/(137)Cs, (90)Sr/(137)Cs, (239+240)Pu/(137)Cs, (238)Pu/(137)Cs, (241)Am/(137)Cs, (239+240)Pu/(238)Pu and (241)Am /(238)Pu have mean values of 0.0049 (R=1), 0.29 (R=0.76), 0.41 (R=0.90), 0.39 (R=0.85), 0.41 (R=0.88), 7.72 (R=0.97) and 16.66 (R=0.98), respectively. The underlying concentrations were correlated and relatively higher than those reported in neighboring countries. One moss sample, as a biomonitor indicator, was measured and evaluated along with the soil samples. Its data showed higher concentrations of all measured radionuclides due to accumulations over years. The depth distribution of the fission product (137)Cs and the total deposition (Bq.m(-2)) were also studied in selected samples. Estimations of the annual effective dose equivalent due to (137)Cs-soil contamination showed values up to more than 200 microSv.     

Chemical availability of 137Cs and 90Sr in undisturbed lysimeter soils maintained under controlled and close-to-real conditions

Chemical availability of 137Cs and 90Sr was determined in four undisturbed soils in a lysimeter study three and four years after deposition to the soil surface. The study was part of a larger project on radionuclide soil-plant interactions under well-defined conditions. The soil types were loam, silt loam, sandy loam and loamy sand, and were representatives of important European soil and climatic conditions. The lysimeters were installed in greenhouses with climatic and hydrological control, and were contaminated with 137Cs and 90Sr in an aerosol mixture simulating fallout from a nuclear accident. Soil samples were taken from several depths in each soil in 1997 and 1998 and the samples were sequentially extracted with H2O, NH4Ac, NH2OH.HCl, H2O2 and HNO3. Extractability of 137Cs decreased in the order: HNO3 > R-esidual > or = NH4Ac > H2O2 > or = NH2OH.HCl > or = H2O. More than 80% was found in the acid digestible or residual fractions, and 11-17% in labile fractions. Soil type differences were small. Extractability of 90Sr decreased in the order: NH4Ac > NH2OH.HCl > HNO3 > H2O2 approximately H2O. 31-58% was found in easily available fractions. Differences between soil types were quite small. The results suggest that availability of 137Cs for plant uptake and migration is low, whereas availability of 90Sr is rather high.