Distribution of fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) in soils of Taiwan

Depth profiles and cumulative deposition of four fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) were determined in presumably undisturbed soils in Taiwan. Inventories of these radionuclides in different areas correlate significantly with each other (except 7Be) and with mean annual rainfall, providing a necessary condition for the development of soil erosion studies in Taiwan. However, the data show very large spatial variability between and within landscape units, reflecting the steep topographic and meteorological gradients in the island. Thus, the application of fallout radionuclides to study soil conservation in Taiwan is expected to be a demanding task; it will call for dense sampling even at undisturbed reference sites.     

Comparative advantages and limitations of the fallout radionuclides (137)Cs, (210)Pb(ex) and (7)Be for assessing soil erosion and sedimentation

The fallout radionuclides (FRNs) (137)Cs, (210)Pb(ex) and (7)Be are increasingly being used as a means of obtaining quantitative information on soil erosion and sediment redistribution rates within agricultural landscapes, over a range of different timescales, and they are frequently seen to represent a valuable complement to conventional measurement techniques. The recent development of the (7)Be method has greatly extended the timescale over which FRNs can be used, by permitting assessment of short-term soil erosion linked to individual events and changing soil management practices. This paper aims to review the advantages and limitations of each of the three FRNs and to identify key knowledge gaps linked to their use. In addition, guidelines for selecting the most appropriate FRN and associated approach, in order to deal with a range of spatial and temporal scales and to investigate specific sets of agro-environmental problems, are provided. Key requirements for future work, related to the application of FRNs in soil erosion investigations, are also identified. These include the upscaling of the approach to the catchment scale and a shift from use of the approach as a research tool to a decision support tool.     

Global fallout (137)Cs accumulation and vertical migration in selected soils from South Patagonia

The spatial distribution and vertical migration of global fallout (137)Cs were studied in soils from South Patagonia at the austral region of South America in semi-natural and natural environments located between 50-54 degrees S and 68-74 degrees W. The (137)Cs areal activity density varied from 222 to 858 Bq m(-2), and was found to be significantly positively correlated (p<0.001) with the mean annual precipitation rate. The fraction of the total activity density observed in steppe grass varied from <0.03% to 0.12% (median <0.07%) and is considerably lower than the results obtained at the South Shetland Islands (median 8%) and in other temperate environments in south-central Chile (median 0.2%). The median of the convection velocity v(s) of (137)Cs in the soil in such polar isotundra climate has been determined to be 0.056 cm y(-1). This value is higher than v(s) determined under polar climate (-0.012 cm y(-1)) and is near to the upper limit of v(s)-values determined in temperate environments from Chile (0.019 cm y(-1)). The median value of the diffusion coefficient D(s) (0.048 cm(2) y(-1)) is similar to D(s) observed in an Antarctic region (0.043 cm(2) y(-1)) and lower than D(s) in temperate regions of Chile (1.24 cm(2) y(-1)). About 35 years after the highest depositions, (137)Cs had penetrated to a depth of 6-14 cm in the Patagonian soils and can be expected to remain in the rooting zone of grass for many decades. Nevertheless, because of its low transfer to steppe grass observed at this region, the radioecological sensitivity of this ecosystem with respect to fallout radiocesium seems to be lower than in other polar regions.     

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

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

Concentration and specific activity of fallout 137Cs in extracted and particle-size fractions of cultivated soils

Fallout (137)Cs and stable Cs in soils were separated with two extractants (1M CH(3)COONH(4) solution and 0.8M CH(3)COONH(4) in 5% HNO(3) solution after H(2)O(2) oxidization). The residue remaining after removal of the oxidizable organic-bound fraction was separated into the particle-size fractions including clay, silt, fine sand and coarse sand with a sieving and sedimentation method. Then, the concentrations of (137)Cs and stable Cs in the extracted fractions and the particle-size fractions were determined. The (137)Cs contents in the exchangeable and organic-bound fractions in the soil were approximately 10 and 20%, respectively. The (137)Cs content in the strongly bound fraction was about 70%, and the concentration of (137)Cs in the clay was the richest among the particle-size fractions. The specific activity of (137)Cs (concentration ratio of fallout (137)Cs/stable Cs) decreased in the order exchangeable, organic-bound and strongly bound fractions. The data suggest that equilibrium between (137)Cs and stable Cs was not reached among those fractions, even though most of the (137)Cs that had been deposited on the soil was derived from fallout weapons tests that occurred several decades ago. The concentration of (137)Cs among the particle-size fractions in each soil was different, whereas the specific activity of (137)Cs in the particle-size fractions had a relatively similar value.     

Geochronology of Pb and Hg pollution in a coastal marine environment using global fallout 137Cs

Global fallout 137Cs was used for dating sediment cores and estimation of recent sedimentation rates (up to 1 cm/y) in the Thane Creek, which lies in the southern part of the Deccan belt of India. The residence time of 210Pb in the Thane Creek water was calculated to be 0.7 years. Further, the concentrations of Pb (up to 70 microg/g) and Hg (up to 10 microg/g) in sediment profiles were measured to assess the anthropogenic input of contaminants due to large-scale industrialization, which has taken place in this area over the last two decades. The depth-wise concentration profile of Hg shows positive evidence of continued fresh input into the Creek.     

Vertical distributions of 210Pb excess, 7Be and 137Cs in selected grass covered soils in Southeast Queensland, Australia

Net accumulated areal activity densities and profiles of (210)Pb(ex), (7)Be and (137)Cs in the surface 10 cm of the soil are reported for eight sites in Southeast Queensland, Australia. Areal activity densities of (210)Pb(ex) and (7)Be varied from 1,080 to 4,100 Bqm(-2) and from 176 to 778 Bqm(-2), respectively. A significant (p < 0.001) portion of the variance (R(2) > 0.99) in their vertical distributions was explained by depth in the profile using an exponential function. Around 85% of accumulated (210)Pb(ex) was present in the surface 10 cm of the soil. Beryllium-7 was mainly confined to the grass and surface 2 cm of the soil. Average penetration half-depths of 3.6 +/- 0.2 and 0.3 +/- 0.1cm were determined for (210)Pb(ex) and (7)Be, respectively. Areal activity densities of global fallout (137)Cs varied from 10 to 361 Bqm(-2). Its signal was well mixed within the surface 10 cm. Comparison of the measured (137)Cs values to the estimated input value for the region ( approximately 490 Bqm(-2)) and profiling of a 1m deep soil core suggests a vertical migration of (137)Cs over the past decades. The paleo-radon activity flux determined from the (210)Pb(ex) areal activity density (5.1 +/- 0.9 mBqm(-2) s(-1)) was not statistically different to that measured using activated charcoal cups (5.5 +/- 0.4 mBqm(-2) s(-1)), tending to suggest that Southeast Queensland is neither a net source nor a net sink of (210)Pb-bearing aerosols.     

Reinvestigation of airborne 210Pb, 137Cs and 207Bi in Vienna (Austria) after atmospheric nuclear weapons tests

Reconstruction of atmospheric 210Pb and 137Cs activity concentrations occurring in Vienna immediately after the atmospheric nuclear weapons tests shall answer the question, whether artificial 210Pb has been produced by fusion devices using lead materials. If so, 207Bi also can be expected. In 1962, weekly average values for 210Pb were between 0.08 +/- 0.02 and 1.31 +/- 0.30 mBq/m2, 137Cs amounts up to 5.1 +/- 0.6 mBq/m3. 207Bi remains below the detection limit, viz. < 0.5 mBq/m3. Bimonthly averages for the periods 1962-1964 and 1974-1975 show 137Cs activity concentrations with typical springtime maxima occurring together with low 210Pb values and 207Bi < 0.02 mBq/m3. Annual averages of 210Pb are varying between 0.27 and 0.53 mBq/m3, independent of whether atmospheric tests have been performed or not. Comparison of the activity ratios 207Bi/210Pb, 207Bi/137Cs and 210Pb/137Cs with published data, leads to the conclusion that no evidence exists for a significant production of 210Pb by nuclear explosions, neither after the Soviet tests in 1961-1962 nor after the Chinese tests in 1973-1976.     

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.     

Precipitation scavenging of 7Be and 137Cs radionuclides in air

Atmospheric depositional fluxes of the naturally occurring 7Be of cosmogenic origin and 137Cs from fallout of the Chernobyl accident were measured over a 6-year period (January 1987-December 1992) at Thessaloniki, Greece (40 degrees 38'N, 22 degrees 58'E). Total precipitation accumulation during 1987-1992 varied between 33.7 cm and 65.2 cm, reflecting a relatively dry (precipitation-free) climate. The activity concentrations of 7Be and 137Cs in rainwater depended on the precipitation rate, being higher for low precipitation rates and lesser for high precipitation rates. 137Cs was removed by rain and snow more efficiently than 7Be. Snowfall was more efficient than rainfall in removing the radionuclides from the atmosphere. The annual bulk depositional fluxes of 7Be varied between 477 and 1133 Bq m(-2) y(-1) and this variability was attributed to the amount of precipitation and the variations of the atmospheric concentrations of 7Be. The annual bulk depositional fluxes of 137Cs showed a significant decrease over time from 1987 to 1992, resulting in a removal half-life of 1.33 years. The presence of 137Cs in air, and therefore in rainwater and snow, long after the Chernobyl accident (26 April 1986) was mainly due to the resuspension process. The normalized depositional fluxes of both radionuclides showed maximal values during the spring season where the maximum amount of precipitation occurred. The relatively high positive correlation between 7Be and 137Cs normalized depositional fluxes indicates that the scavenging process of local precipitation controlled the fluxes of both radionuclides. The dry depositional flux of 7Be was less than 9.37% of total (wet and dry) depositional flux. The fraction of dry-to-total depositional flux of 137Cs was much higher than that of 7Be, due to the resuspended soil.     

137Cs and 210Po dose assessment from marine food in Cienfuegos Bay (Cuba)

One part of Radiological Monitoring Programme in central Cuba (1991-1995) was dedicated to study the background levels of natural and anthropogenic radioactivity in Cienfuegos Bay in the vicinity of the first Cuban nuclear power station under construction. 210Po and 137Cs concentrations in fish, molluscs and crustaceans collected in Cienfuegos Bay were determined and the committed effective doses (CED) were calculated for two population groups inhabiting this region. The highest values of 210Po concentrations were found in crustaceans, but significant accumulation was also observed in fish and molluscs. The mean 137Cs concentrations in organisms are several times lower with respect to 210Po, a situation that characterises the regions affected by the global fallout only. Values of CED from the consumption of crustaceans and molluscs are very low both from 210Po and 137Cs. The mean individual dose from 210Po in the seafood consumed varies from 39 microSv for general populations to 2802 microSv for the "critical group" consuming 320 kg of fish per year. The dose from 137Cs is negligible.     

Model testing using data on 137Cs from Chernobyl fallout in the Iput River catchment area of Russia

Data collected for 10 years following the Chernobyl accident in 1986 have provided a unique opportunity to test the reliability of computer models for contamination of terrestrial and aquatic environments. The Iput River scenario was used by the Dose Reconstruction Working Group of the BIOMASS (Biosphere Modelling and Assessment Methods) programme. The test area was one of the most highly contaminated areas in Russia following the accident, with an average contamination density of 137Cs of 800,000 Bq m-2 and localized contamination up to 1,500,000 Bq m-2, and a variety of countermeasures that were implemented in the test area had to be considered in the modelling exercise. Difficulties encountered during the exercise included averaging of data to account for uneven contamination of the test area, simulating the downward migration and changes in bioavailability of 137Cs in soil, and modelling the effectiveness of countermeasures. The accuracy of model predictions is dependent at least in part on the experience and judgment of the participant in interpretation of input information, selection of parameter values, and treatment of uncertainties.     

Comparative analysis of (239)Pu, (137)Cs, (210)Pb and (40)K spatial distributions in the top soil layer at the Baltic coast

This paper presents the results of an investigation into the spatial distribution of radionuclides of artificial ((239,240)Pu, (137)Cs) and natural ((210)Pb, (40)K) origins in the upper (0-5 cm) soil layers on the Baltic coastline of Lithuania ( approximately 5 km(2) area). The samples were analysed by gamma ray spectrometry and combined radiochemical procedures. The highest (210)Pb, (239,240)Pu and (137)Cs activity concentrations were determined in the forest samples, whereas (40)K activity was rather homogeneous across the study area. Relatively high (239,240)Pu and (40)K activity concentrations were determined along the surf zone. The (210)Pb and (137)Cs activity concentrations showed a gradual increase from the surf zone to the forest. The average activity concentrations of (239,240)Pu, (137)Cs, (210)Pb and (40)K in the beach and forest samples, respectively, were as follows: 0.32+/-0.08 and 0.74+/-0.14; 50+/-4 and 1190+/-50; 4.7+/-2.0 and 48+/-6; 186+/-15 and 216+/-17 Bq/kg.     

Natural radionuclides and (137)Cs distributions and their relationship with sedimentological processes in Patras Harbour, Greece

Surficial and subsurficial sediment samples derived from gravity cores, selected from the harbour of Patras, Greece, were analyzed for grain size, water content, bulk density, specific gravity, organic carbon content and specific activities of natural radionuclides and (137)Cs. The specific activities of (232)Th, (226)Ra, (40)K and (137)Cs were measured radiometrically. The radionuclides (238)U and (232)Th were also analyzed using the INAA. The differences found between the specific activities of the natural radionuclides measured by the two methods are of no statistical significance. The sediment cores selection was based on a detailed bathymetric and marine seismic survey. Through the study of the detailed bathymetric map and the seismic profiles it was shown that ship traffic is highly influential to the harbour bathymetry. The granulometric and geotechnical properties of the sediments and therefore the specific activities of the natural radionuclides and (137)Cs seem to be controlled by the ship traffic. Relationship between radionuclide activity concentrations and granulometric/geotechnical parameters was defined after the treatment of all the analyses using R-mode factor analysis. The natural radionuclide activities are related to the fine fraction and bulk density of the sediments, while (137)Cs is mainly influenced by the organic carbon content. In addition, (238)U and (226)Ra seem to be in close relation with the heavy minerals fraction in coarse-grained sediments with high specific gravity.     

Accumulation of (137)Cs in Brazilian soils and its transfer to plants under different climatic conditions

The spatial distribution and behaviour of the global fallout (137)Cs in the tropical, subtropical and equatorial soil-plant systems were investigated at several upland sites in Brazil selected according to their climate characteristics, and to the agricultural importance. To determine the (137)Cs deposition density, undisturbed soil profiles were taken from 23 environments situated between the latitudes of 02 degrees N and 30 degrees S. Sampling sites located along to the equator exhibited (137)Cs deposition densities with an average value of 219Bqm(-2). Extremely low deposition densities of 1.3Bqm(-2) were found in the Amazon region. In contrast, the southern part of Brazil, located between latitudes of 20 degrees S and 34 degrees S, exhibited considerably higher deposition densities ranging from 140Bqm(-2) to 1620Bqm(-2). To examine the (137)Cs soil-to-plant transfer in the Brazilian agricultural products, 29 mainly tropical plant species, and corresponding soil samples were collected at 43 sampling locations in nine federal states of Brazil. Values of the (137)Cs concentration factor plant/soil exhibited a large range from 0.020 (beans) to 6.2 (cassava). Samples of some plant species originated from different collecting areas showed different concentration factors. The (137)Cs content of some plants collected was not measurable due to a very low (137)Cs concentration level found in the upper layers of the incremental soils. Globally, the soil-to-plant transfer of (137)Cs can be described by a logarithmic normal distribution with a geometric mean of 0.3 and a geometric standard deviation of 3.9.     

Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland)

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.     

Qualitative estimates of soil disturbance in the vicinity of CANDU stations, utilizing measurements of 137Cs and 210Pb in soil cores

Anthropogenically derived 14C has been used to trace recent carbon input in a study of carbon accumulation and turnover in Canadian soils. In order to do so, documentation of the undisturbed nature of the soil horizons sampled was of prime concern. Although all the sites chosen for coring were currently uncultivated, detailed information on long-term land usage was not available. To overcome this problem, 137Cs profiles were measured in all the cores used in the study. 210Pb measurements were also made in cases where total 137Cs deposition was lower than predicted. For some sample sites, the data obtained showed correlated losses of both radionuclides, indicating that land disturbance and/or erosion had indeed occurred in these areas over the past 50 years, hence invalidating the use of those cores for carbon cycling studies. In a few cases a marked lack of correlation between these two radionuclides has made it necessary to hypothesize that chemical, rather than physical, processes have been partially responsible for the observed anomalies. Since results of this nature raise doubts about the reliability of the 137Cs method for identification of land disturbance, further investigation is warranted.     

(90)Sr, (210)Po and (210)Pb in lichen and reindeer in Norway

Concentrations of (90)Sr, (210)Po and (210)Pb in lichen and reindeer were studied in central (?stre Namdal) and southern Norway (V?g?) during 2000-2003. The study focussed on potential differences in concentrations of these nuclides in reindeer of different ages. Concentrations of (90)Sr in bones of approximately 10 year old adult females were about 40% higher than those in calves' antlers ((90)Sr concentrations in antlers and bones of calves are similar), while the available data from V?g? suggest that (90)Sr concentrations in reindeer calves decreased with an effective ecological half-time of 9.03+/-0.06 years during 1988-2002. Furthermore, (90)Sr concentrations were 50-80% higher in bone of reindeer of a similar age from V?g? compared to those from ?stre Namdal. Concentrations of (210)Po and (210)Pb in muscle and liver tissues were comparable to those reported for reindeer in other Nordic areas, with no significant difference in (210)Po and (210)Pb concentrations between adults and calves or between reindeer from the two different study areas.     

210Pb and 137Cs as chronometers for salt marsh accretion in the Venice Lagoon - links to flooding frequency and climate change

Five salt marsh sediment cores from different parts of the Venice Lagoon were studied to determine their depositional history and its relationship with the environmental changes occurred during the past approximately 100 years. X-radiographs of the cores show no disturbance related to particle mixing. Accretion rates were calculated using a constant flux model applied to excess (210)Pb distributions in the cores. The record of (137)Cs fluxes to the sites, determined from (137)Cs profiles and the (210)Pb chronologies, shows inputs from the global fallout of (137)Cs in the late 1950s to early 1960s and the Chernobyl accident in 1986. Average accretion rates in the cores are comparable to the long-term average rate of mean sea level rise in the Venice Lagoon ( approximately 0.25 cm y(-1)) except for a core collected in a marsh presumably affected by inputs from the Dese River. Short-term variations in accretion rate are correlated with the cumulative frequency of flooding, as determined by records of Acqua Alta, in four of the five cores, suggesting that variations in the phenomena causing flooding (such as wind patterns, storm frequency and NAO) are short-term driving forces for variations in marsh accretion rate.     

Use of 210Pb and 137Cs to simultaneously constrain ages and sources of post-dam sediments in the Cordeaux reservoir, Sydney, Australia

Environmental radionuclides can be employed as tracers of sediment movement and delivery to water bodies such as lakes and reservoirs. The chronologies of sediments that have accumulated in the Cordeaux reservoir in Sydney, Australia, were determined by the rate of change of (210)Pb(ex) with depth and indicate slow accretion in the reservoir. The ratio of enrichment of radionuclides in sediment cores to (210)Pb(ex) and (137)Cs concentrations in a reference soil sample within the Cordeaux catchment indicates that the dominant source of sediment in the Cordeaux reservoir is surface erosion (detachment and removal of sediment at depths less than 30 cm). However, in the Kembla Creek arm of the reservoir a mixture of sources was detected and includes sheet and rill erosion together with sub-soil contributions. Implications for the utility of these radionuclide sedimentation assessments, especially where samples are limited, are that well-constrained chronologies and sources of soil erosion are facilitated.