Levels of 137Cs in muddy sediments of the seabed of the Bay of Cadiz, Spain. Part I. Vertical and spatial distribution of activities

This is the first of a two-part paper. This first part describes a detailed study conducted of the spatial and vertical distribution of the concentration of the radionuclide (137)Cs, utilising columns of sediment extracted from the seabed of the Bay of Cadiz (Spain) as specimens. The activity concentrations have been measured by means of gamma spectrometry using a HPGe detector and (137)Cs is used as an indicator of the sedimentation and contamination processes in the zone. At the same time the relationship between the levels of activity found and other hydrodynamic and sedimentological variables characteristic of the zone have been studied. The experimental results obtained will also serve to develop a model of the distribution of (137)Cs, which will be presented in the second part of this paper.     

Modeling 137Cs migration processes in lake sediments

Lake sediments can be considered as the "diary" of the lake: new layers are continuously deposited on top of the sediments. The migration behavior of radionuclides, particularly of (137)Cs, can be analyzed by modeling the input into and the vertical distribution within the sediment. For this purpose, a model consisting of sedimentation-diffusion equations was developed. Solved with a finite element method, this model can cover the time period from the nuclear weapons testing to the present. It takes into account fixation and redissolution, compaction of sediments, and the influence of competing ions on the retarded diffusion within the sediments. The outcome of the model is compared to water and sediment measurements from Lago Maggiore. The results of an optimization process can produce the sedimentation rate and (137)Cs distribution coefficients which determine the uptake of activity into the sediment and also the retarded diffusion within the sediment.     

Accumulation of Chernobyl-derived 137Cs in bottom sediments of some Finnish lakes

The amount and vertical distribution of Chernobyl-derived 137Cs in the bottom sediments of some Finnish lakes were studied. Sediment and surface water samples were taken in 2000 and 2003 from 12 stations in nine lakes and the results were compared with those obtained in corresponding surveys carried out in 1969, 1978, 1988 and 1990. Each of the five deposition categories of Chernobyl fallout in Finland were represented. The depth profiles of 137Cs in the sediments showed considerable variety in the lakes studied. The peak values varied between 1.5 and 46 kBq kg(-1) dry wt. The size and shape of the peak did not always correlate with the amount of deposition in the area, but on the other hand, reflected differences in sedimentation processes in different lakes. In some of the lakes the peak still occurred in the uppermost (0-2 cm) sediment layer, but in an extreme case the peak occurred at a depth of 22-23 cm corresponding to a sedimentation rate of 16 mm year(-1) during the 14 years after the Chernobyl accident. The total amounts of 137Cs in sediments varied from 15 to 170 kBq m(-2) at the sampling stations studied. Since 1990, the amounts have continued to increase slightly in two lakes, but started to decrease in the other lakes. In most of the lakes, the total amounts of 137Cs in sediments were about 1.5-2 times higher than in local deposition. In two lakes, the ratio was below 1, but in one case 3.2. Compared with the total amounts of 137Cs at the same stations in the late 1960s and 1970s, the values were now at their highest, at about 60-fold. The most important factors affecting 137Cs values in sediments were the local amount of deposition and the type of the lake and the sediment, but in addition, there were a number of other factors to be considered.     

137Cs and excess 210Pb deposition patterns in estuarine and marine sediment in the central region of the Great Barrier Reef Lagoon, north-eastern Australia

This paper focuses on the distribution of 137Cs and 210Pb(xs) in 51 estuarine and marine sediment cores collected between the Upstart Bay and Rockingham Bay in the Great Barrier Reef Lagoon, north-eastern Australia. Historical records of 210Pb(xs) and 137Cs atmospheric deposition and present day terrestrial inventories in north-eastern Australia are presented. 210Pb(xs) and 137Cs fluxes measured on suspended sediments in the Burdekin River are considered to be a source of recent inputs of these nuclides to the nearshore region of this part of the Great Barrier Reef. Direct correlations between sediment nuclide inventories, maximum detectable depths, and sediment mass accumulation rates (MARs), calculated using both 137Cs and 210Pb(xs), are explored. In relation to inventories of 210Pb(xs), 60% of atmospheric fallout 137Cs appears to be missing from the sediments. The reasons for these differences in two tracers, primarily of atmospheric origin, are discussed in terms of the geochemical properties of these two nuclides. Evidence is presented to support the hypothesis that the 137Cs distribution in these cores can be a useful independent tracer which provides confirmation of MARs calculated from the decay of 210Pb(xs).     

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.     

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.     

137Cs in the Danish Wadden Sea: contrast between tidal flats and salt marshes

The 137Cs activity of salt marsh and tidal flat sediments of the northern part of the European Wadden Sea was studied based on a comprehensive dataset of 210Pb dated cores. The 137Cs inventory of salt marsh sediments shows a major peak corresponding to the Chernobyl accident in 1986, and a minor peak located in the late 1960s interpreted as the combined effect of atmospheric testing of nuclear weapons. Emissions from the nuclear reprocessing plant Sellafield are not reflected as peaks in 137Cs activity, but may contribute to the rising 137Cs activity in the years prior to 1986. The 137Cs activity of tidal flat sediments differs from salt marsh sediment in two respects. First, the activity is much lower and, second, the major peak in the 1980s is located in the beginning instead of in the middle of the decade. The differences in 137Cs inventory between the two environments are interpreted to result from repeated cycles of deposition/resuspension and mixing on tidal flats. A simple model illustrating the consequence of mixings returns an apparent shift of major peaks in 137Cs activities backwards in time corresponding to the mixing depth divided by the deposition rate.     

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.     

Sedimentology models from activity concentration measurements: application to the “Bay of Cadiz” Natural Park (SW Spain)

A previous study on seabed sediments of the Bay of Cadiz (SW of Spain) enabled us to identify several relations between sedimentological variables and activity concentrations of environmental radionuclides such as ¹³⁷Cs, ²²⁶Ra, ²³²Th and ⁴⁰K. In this paper the study has been extended to a large neighbouring inter-tidal area in order to establish if the above mentioned models can be generalized. As a result we have determined that the measured activity concentrations are closely to the values predicted by the theoretical models (correlation coefficient range = 0.85–0.93).     

Post-depositional redistribution and gradual accumulation of 137Cs in a riparian wetland ecosystem in Sweden

After the Chernobyl accident, high activity concentrations of (137)Cs (>1 MBq m(-2)) were detected in a riparian swamp in the central-eastern part of Sweden. The objective of this study was to clarify the redistribution processes behind the accumulation of (137)Cs in the wetland. A mass balance budget of (137)Cs was calculated based on soil and sediment samples and reports in the literature. Results showed that accumulation occurred over several years. Of all the (137)Cs activity discharged between 1986 and 2002 from the upstream lake, 29% was estimated to be retained in the wetland. In 2003, measurements showed that 17 kBq m(-2) sedimented on the stream banks of the wetland. Continuing overbank sedimentation by spring flooding prolongs the time that the wetland will contain high activity concentrations of (137)Cs. Consequently, organisms living in wetlands serving as sinks for (137)Cs may become exposed over long time periods to high activity concentrations.     

Fixation of Cs to marine sediments estimated by a stochastic modelling approach

Dumping of nuclear waste in the Kara Sea represents a potential source of radioactive contamination to the Arctic Seas in the future. The mobility of 137Cs ions leached from the waste will depend on the interactions with sediment particles. Whether sediments will act as a continuous permanent sink for released 137Cs, or contaminated sediments will serve as a diffuse source of 137Cs in the future, depends on the interaction kinetics and binding mechanisms involved. The main purpose of this paper is to study the performance of different stochastic models using kinetic information to estimate the time needed for Cs ions to become irreversibly fixed within the sediments. The kinetic information was obtained from 134Cs tracer sorption and desorption (sequential extractions) experiments, conducted over time, using sediments from the Stepovogo Fjord waste dumping site, on the east coast of Novaya Zemlya. Results show that 134Cs ions interact rapidly with the surfaces of the Stepovogo sediment, with an estimated distribution coefficient Kd(eq) of 300 ml/g (or 13m2/g), and the 134Cs ions are increasingly irreversibly fixed to the sediment over time. For the first time, stochastic theory has been utilised for sediment-seawater systems to estimate the mean residence times (MRTs) of Cs ions in operationally defined sediment phases described by compartment models. In the present work, two different stochastic models (i) a Markov process model (MP) being analogous to deterministic compartment models, and (ii) a semi-Markov process model (SMP) which should be physically more relevant for inhomogeneous systems, have been compared. As similar results were obtained using the two models, the less complicated MP model was utilised to predict the time needed for an average Cs ion to become irreversibly fixed in the Stepovogo sediments. According the model, approximately 1100 days of contact time between Cs ions and sediments is needed before 50% of the 134Cs ion becomes fixed in the irreversible sediment phase. while about 12.5 years are needed before 99.7% of the Cs ions are fixed. Thus, according to the model estimates the contact time between 137Cs ions leached from dumped waste and the Stepovogo Fjord sediment should be about 3 years before the sediment will act as an efficient permanent sink. Until then a significant fraction of 137Cs should be considered mobile. The stochastic modelling approach provides useful tools when assessing sediment-seawater interactions over time, and should be easily applicable to all sediment-seawater systems including a sink term.     

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.     

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

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

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.     

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.     

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.     

Depositional records of plutonium and (137)Cs released from Nagasaki atomic bomb in sediment of Nishiyama reservoir at Nagasaki

In a sediment core of Nishiyama reservoir at Nagasaki city, depth profiles of (240)Pu/(239)Pu isotopic ratio, (239+240)Pu and (137)Cs activities were determined. Sediments containing plutonium and (137)Cs, which were deposited immediately after a detonation of Nagasaki atomic bomb, were identified in the core. Observed below the sediments were macroscopic charcoals, providing evidence for initial deposit of the fallout of the Nagasaki atomic bomb. This is the first entire depositional records of plutonium and (137)Cs released from the Nagasaki atomic bomb together with those from atmospheric nuclear tests.     

Recent Cs deposition in sediments of Admiralty Bay, Antarctica

Cesium-137, radium-226 and lead-210 profiles of a 25 cm sediment core give an indication of recent changes in land-ocean interactions at a polar coastal environment (Admiralty Bay, King George Island, Antarctica). The linear sedimentation accumulation rate at the study site calculated from the unsupported ²¹⁰Pb profile was 6.7 mm/year from 1965 to 2005. A 3.5-fold increase in ¹³⁷Cs concentrations was observed in the top layer of this sediment core. This sharp increase seems to indicate a recent redistribution of fallout radionuclides previously deposited on soil, vegetation and snow. These results imply enhanced land-ocean interactions at this site likely as a result of climate change. Because our results are based on a single core, additional investigations are needed to confirm our observations.     

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.     

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

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