Reconstructing historical radionuclide concentrations along the east coast of Ireland using a compartmental model

A mathematical model is presented that simulates the annually averaged transport of radionuclides, originating from the BNFL reprocessing plant at Sellafield, throughout the Irish Sea. The model, CUMBRIA77, represents the processes of radionuclide transport and dispersion in the marine environment and allows predictions of radionuclide concentration in various environmental media, including biota, to be made throughout the whole of the Irish Sea. In this paper we describe the use of the model to reconstruct the historical activity concentrations of 137Cs and 239+240Pu in a variety of environmental media in the western Irish Sea and along the Irish east coast back to 1950. This reconstruction exercise is of interest because only limited measurements of 137Cs and 239+240Pu activity are available prior to the 1980s. The predictions were compared to the available measured data to validate their accuracy. The results of the reconstruction indicate that activity concentrations of 137Cs in the western Irish Sea follow a similar, though slightly delayed and smoothed, profile to the discharges from the Sellafield site, with concentrations at the time of peak discharge (the mid-1970s) being around an order of magnitude higher than those measured in the 1980s and 1990s. By contrast, the concentrations of 239+240Pu at the time of peak discharges were similar to those presently measured. These differences reflect the distinct marine chemistries of the two nuclides, in particular the higher propensity of plutonium to bind to sediments leading to extended transport times. Despite these differences in behaviour the doses to Irish seafood consumers from 137Cs remain significantly higher than those from 239+240Pu.     

Comparing in situ distribution coefficients and exchangeability of radiocaesium in freshwater sediments with laboratory predictions

Two short-term (24 h) laboratory procedures, based on measurement of the affinity and capacity of the specific binding sites for radiocaesium on illitic clay minerals, are used to predict the in situ 137Cs distribution coefficients (KD) in two Dutch freshwater sediments. Differences in the measured amount of specific binding sites between the sediments are shown to be related to differences in the particle size and illite content. A procedure based on measurement of the combined parameter KD[NH4+] predicts the measured in situ 137Cs distribution in both sediments very well. This is remarkable because the in situ data are based on 137Cs/sediment contact times of > 1 year, while previous experiments have shown that increasing contact times between Cs+ and sediments decreases the short-term exchangeability of caesium, as measured by extraction with a high ammonium concentration. The good predictions of the 37Cs solid/water distribution by short-term ion-exchange experiments, therefore, indicate that more 137Cs in the sediments is exchangeable than is measured by the commonly used extraction with high ammonium concentrations.     

Assessment of Committed Effective Dose due to consumption of Red Sea coral reef fishes collected from the local market (Sudan)

An assessment of Committed Effective Dose (CED) due to consumption of Red Sea fish containing (210)Po and (137)Cs was performed for 23 different marine fish samples collected from the local market at Port Sudan. The fish were classified according to their feeding habits into three categories: carnivores, herbivores, and omnivores. Measured activity concentrations of (210)Po were found in the ranges 0.25-6.42 (carnivores), 0.7-5 (omnivores) and 1.5-3.8 (herbivores) Bq/kg fresh weight. In the same study, activity concentrations of Cs-137 were determined to be in the ranges 0.1-0.46 (carnivores), 0.09-0.35 (omnivores) and 0.09-0.32 (herbivores) Bq/kg fresh weight, which were several times lower than those of (210)Po. Appropriate conversion factors were used to derive the CED, which was found to be 0.012, 0.01 and 0.01 (microSv/yr) in carnivores, omnivores and herbivores, respectively, for (137)Cs. This contributes about 0.4% of the total dose exclusively by ingestion of fish. For (210)Po, it was found to be 3.47, 4.81 and 4.14 (microSv/yr) in carnivores, omnivores and herbivores, respectively, which represents 99.6% of the total dose (exclusively by ingestion of fish). The results of CED calculations suggest that the dose received by the Sudanese population from the consumption of marine fish is rather small and that the contribution of (137)Cs is negligible compared to (210)Po.     

Efficiency of measures aimed at decreasing the contamination of agricultural products in areas contaminated by the Chernobyl NPP accident.

The sequence of agricultural countermeasures taken in the Polessye area of the Ukraine contaminated by radionuclides as a result of the Chernobyl NPP accident is discussed. The efficiency of these countermeasures has been analysed. The concentration of 137Cs in crops has been shown to vary 10-100-fold, depending on the biological features of the plant species and on soil properties. Liming and mineral fertilizing of meadows increase the yield of grass and reduce 137Cs transfer to cows' milk up to 3.5-fold.     

Radionuclides in fruit systems: model prediction-experimental data intercomparison study

This paper presents results from an international exercise undertaken to test model predictions against an independent data set for the transfer of radioactivity to fruit. Six models with various structures and complexity participated in this exercise. Predictions from these models were compared against independent experimental measurements on the transfer of 134Cs and 85Sr via leaf-to-fruit and soil-to-fruit in strawberry plants after an acute release. Foliar contamination was carried out through wet deposition on the plant at two different growing stages, anthesis and ripening, while soil contamination was effected at anthesis only. In the case of foliar contamination, predicted values are within the same order of magnitude as the measured values for both radionuclides, while in the case of soil contamination models tend to under-predict by up to three orders of magnitude for 134Cs, while differences for 85Sr are lower. Performance of models against experimental data is discussed together with the lessons learned from this exercise.     

Prediction of the effects of soil-based countermeasures on soil solution chemistry of soils contaminated with radiocesium using the hydrogeochemical code PHREEQC

For agriculturally used areas, which are contaminated by the debris from a nuclear accident, the use of chemical amendmends (e.g. potassium chloride and lime) is among the most common soil-based countermeasures. These countermeasures are intended to reduce the plant uptake of radionuclides (mainly 137Cs and 90Sr) by competitive inhibition by chemically similar ions. So far, the impacts of countermeasures on soil solution composition - and thus, their effectiveness - have almost exclusively been established experimentally, since they depend on mineral composition and chemical characteristics of the soil affected. In this study, which focuses on caesium contamination, the well-established code PHREEQC was used as a geochemical model to calculate the changes in the ionic compositions of soil solutions, which result from the application of potassium or ammonium in batch equilibrium experiments. The simple ion exchange model used by PHREEQC was improved by taking into account selective sorption of Cs+, NH4+ and K+ by clay minerals. Calculations were performed with three different initial soil solution compositions, corresponding to particular soil types (loam, sand, peat). For loamy and sandy soils, our calculational results agree well with experimental data reported by Nisbet (Effectiveness of soil-based countermeasures six months and one year after contamination of five diverse soil types with caesium-134 and strontium-90. Contract Report NRPB-M546, National Radiation Protection Board, Chilton, 1995.). For peat, discrepancies were found indicating that for organic soils a reliable set of exchange constants of the relevant cations still has to be determined experimentally. For cesium, however, these discrepancies almost disappeared if selective sites were assumed to be inaccessible. Additionally, results of sensitivity analyses are presented by which the influence of the main soil parameters on Cs+ concentrations in solution after soil treatment has been systematically studied. It is shown that calculating the impacts of soil-based chemical countermeasures on soil solution chemistry using geochemical codes such as PHREEQC offers an attractive alternative to establishing these impacts by often time-consuming and site-specific experiments.     

Deposition of atmospheric (137)Cs in Japan associated with the Asian dust event of March 2002

Considerable deposition of (137)Cs was observed in the northwestern coastal area of Japan in March 2002. Since there were no nuclear explosions or serious nuclear accidents in the early 2000s, transport of previously contaminated dust appears to be the only plausible explanation for this event. In March 2002, there was a massive sandstorm on the East Asian continent, and the dust raised by the storm was transported across the sea to Japan. This dust originated in Mongolia and northeastern China, in an area distant from the Chinese nuclear test site at Lop Nor or any other known possible sources of (137)Cs. Our radioactivity measurements showed (137)Cs enrichment in the surface layer of grassland soils in the area of the sandstorm, which we attributed to accumulation as a result of past nuclear testing. We suggest that the grassland is a potential source of (137)Cs-bearing soil particles. Since the late 1990s, this area has experienced drought conditions, resulting in a considerable reduction of vegetation cover. We attribute the prodigious release of (137)Cs-bearing soil particles into the atmosphere during the sandstorm and the subsequent deposition of (137)Cs in Japan to this change.     

Prediction of spatial variation in global fallout of 137Cs using precipitation

Deposition from atmospheric nuclear weapons tests (termed global fallout) has been shown to be proportional to the rate of precipitation. Here we describe methods for using precipitation and radionuclide deposition information for a reference site to estimate global fallout at other locations. These methods have been used to estimate global fallout in Iceland, identified during the Arctic Monitoring and Assessment Programme (AMAP) by Wright et al. [Wright, S.M., Howard, B.J., Strand, P., Nylén, T., Sickel, M.A.K., 1999. Prediction of 137Cs deposition from atmospheric nuclear weapons tests within the Arctic. Environ Pollut 104, 131-143.] as one of the Arctic areas which received the highest global fallout, but where measurements of contamination were sparse, and difficult to obtain due to the remote and inaccessible terrain of much of the country. Measurements of global fallout 137Cs deposition have been made in Iceland at sites close to meteorological stations to ensure that precipitation data were of high quality. The AMAP modeling approach, based on measured precipitation and radionuclide deposition data, was applied using a reference monitoring station located close to Reykjavik. The availability of good precipitation data and locally based estimates of time dependent ratios of 137Cs deposition to precipitation during the fallout period gave a better correlation between predicted and measured 137Cs global fallout (r2=0.96) than that achieved using the much more heterogeneous set of data collected by AMAP over the whole of the Arctic. Having obtained satisfactory results with the model for a number of calibration sites alongside meteorological stations we then produced a map of estimated 137Cs deposition based on a model of estimated precipitation. This deposition map was then successfully validated (r2=0.85) for sites where 137Cs deposition was measured; the associated uncertainty in predictions was also estimated.     

Model testing of radioactive contamination by Sr, Cs and Pu of water and bottom sediments in the Techa River (Southern Urals, Russia)

This paper presents results of testing models for the radioactive contamination of river water and bottom sediments by ⁹⁰Sr, ¹³⁷Cs and ^239,240Pu. The scenario for the model testing was based on data from the Techa River (Southern Urals, Russia), which was contaminated as a result of discharges of liquid radioactive waste into the river. The endpoints of the scenario were model predictions of the activity concentrations of ⁹⁰Sr, ¹³⁷Cs and ^239,240Pu in water and bottom sediments along the Techa River in 1996. Calculations for the Techa scenario were performed by six participant teams from France (model CASTEAUR), Italy (model MARTE), Russia (models TRANSFER-2, CASSANDRA, GIDRO-W) and Ukraine (model RIVTOX), all using different models. As a whole, the radionuclide predictions for ⁹⁰Sr in water for all considered models, ¹³⁷Cs for MARTE and TRANSFER-2, and ^239,240Pu for TRANSFER-2 and CASSANDRA can be considered sufficiently reliable, whereas the prediction for sediments should be considered cautiously. At the same time the CASTEAUR and RIVTOX models estimate the activity concentrations of ¹³⁷Cs and ^239,240Pu in water more reliably than in bottom sediments. The models MARTE (^239,240Pu) and CASSANDRA (¹³⁷Cs) evaluated the activity concentrations of radionuclides in sediments with about the same agreement with observations as for water. For ⁹⁰Sr and ¹³⁷Cs the agreement between empirical data and model predictions was good, but not for all the observations of ^239,240Pu in the river water-bottom sediment system. The modelling of ^239,240Pu distribution proved difficult because, in contrast to ¹³⁷Cs and ⁹⁰Sr, most of models have not been previously tested or validated for plutonium.     

Radiocaesium and natural gamma emitters in mushrooms collected in Spain

Mushrooms can accumulate heavy metals in general, including radionuclides found in the nature. However, little attention has been paid to the radioactive content of mushrooms collected in Spain and the dose for the population due to their ingestion. To address this, we analysed the contents of 137Cs, 40K, 226Ra and 7Be present in different species of mushrooms, according to their genus and nutritional mechanism. We observed that mycorrhizal mushrooms accumulate 137Cs more than saprophytes, and vice versa for 7Be. 40K and 226Ra are accumulated to the same degree by the two groups of mushrooms. We estimated the dose due to ingestion of mushrooms in Spain to be 2 microSv/year, and the contribution of 40K and 226Ra to be generally greater than that of 137Cs. The contribution of 137Cs to the dose was calculated by taking into account the results of an experiment carried out under the controlled laboratory conditions, which showed that approximately 98% of 134Cs was associated with the readily digestible fraction of the mushrooms.     

GIS supported calculations of (137)Cs deposition in Sweden based on precipitation data

It is of interest to know the spatial variation and the amount of (137)Cs e.g. in case of an accident with a radioactive discharge. In this study, the spatial distribution of the quarterly (137)Cs deposition over Sweden due to nuclear weapons fallout (NWF) during the period 1962-1966 was determined by relating the measured deposition density at a reference site to the amount of precipitation. Measured quarterly values of (137)Cs deposition density per unit precipitation at three reference sites and quarterly precipitation at 62 weather stations distributed over Sweden were used in the calculations. The reference sites were assumed to represent areas with different quarterly mean precipitation. The extent of these areas was determined from the distribution of the mean measured precipitation between 1961 and 1990 and varied according to seasonal variations in the mean precipitation pattern. Deposition maps were created by interpolation within a geographical information system (GIS). Both integrated (total) and cumulative (decay corrected) deposition densities were calculated. The lowest levels of NWF (137)Cs deposition density were noted in north-eastern and eastern parts of Sweden and the highest levels in the western parts of Sweden. Furthermore the deposition density of (137)Cs, resulting from the Chernobyl accident was determined for an area in western Sweden based on precipitation data. The highest levels of Chernobyl (137)Cs in western Sweden were found in the western parts of the area along the coast and the lowest in the east. The sum of the deposition densities from NWF and Chernobyl in western Sweden was then compared to the total activity measured in soil samples at 27 locations. Comparisons between the predicted values of this study show a good agreement with measured values and other studies.     

Measurement of radioactivity levels of the Sirt gulf,Libya

The paper presents the results of measurements on air and soil samples collected for their natural and artificial radioactivity content. The radionuclides studied under this programme are ⁷Be and ¹³⁷Cs. Average activity concentrations in surface air of ⁷Be and ¹³⁷Cs were found to be 1920 and 2.1 μBq m^‐3, respectively. ¹³⁷Cs activity concentration in surface soil is found to be 450m Bq kg^‐1. Estimated effective doses to adult from inhaled ⁷Be and ¹³⁷Cs were found to be 1 and 0.13 nSvy^‐1, respectively.

The average outdoors absorbed dose rate in air, 1 m above the ground level was found to be (48 ± 4.0 nGy h^‐1), based on the analysis of thermoluminescence dosimeters data collected.     

Application of potassium chloride to a Chernobyl-contaminated lake: modelling the dynamics of radiocaesium in an aquatic ecosystem and decontamination of fish

This study tests a whole-lake experiment to reduce the bioaccumulation of radiocaesium (137Cs) in fish in lakes contaminated by the Chernobyl accident. In many lakes in the Chernobyl contaminated areas, radiocaesium activity concentrations in fish are still significantly higher (up to 100 times in some species) than acceptable limits for human consumption. Estimates of the long-term rate of decline of 137Cs in fish in these regions, in the absence of countermeasures, show that radioactivity in fish in some lakes may remain above acceptable consumption limits for a further 50-100 years from the present date. In February 1998 we applied 15 t of potassium chloride to Lake Svyatoe, Kostiukovichy. The addition of potassium chloride fertilizer to the lake resulted in a decrease in activity concentration of 137Cs to approximately 40% of pre-countermeasure values in a number of different fish species. In contrast to Lake Svyatoe, 137Cs activity concentrations in fish from four control lakes showed no systematic decrease over the study period. Simplified models for transfers of 137Cs in lakes successfully 'blind' predicted the changes in 137Cs in water and fish resulting from this major alteration of the potassium concentration of the lake. The experiment represents the first test of a predictive model for the dynamics of radiocaesium in response to a major perturbation in potassium (its major competitor ion) in a whole lake ecosystem.     

Measurements of long-term external and internal radiation exposure of inhabitants of some villages of the Bryansk region of Russia after the Chernobyl accident

A Nordic-Soviet programme was initiated in 1990 to evaluate the external and internal radiation exposure of the inhabitants of several villages in the Bryansk region of Russia. This area was one of the number of areas particularly affected by the nuclear accident at the Chernobyl Nuclear Power Plant in 1986. Measurements were carried out yearly until 1998 and after that more irregularly; in 2000, 2006 and 2008 respectively. The effective dose estimates were based on individual thermoluminescent dosemeters and on in vivo measurements of the whole body content of ¹³⁷Cs (and ¹³⁴Cs during the first years of the programme). The decrease in total effective dose during the almost 2 decade follow-up was due to a continuous decrease in the dominating external exposure and a less decreasing but highly variable exposure from internal irradiation. In 2008, the observed average effective dose (i.e. the sum of external and internal exposure) from Chernobyl ¹³⁷Cs to the residents was estimated to be 0.3 mSv y⁻¹. This corresponds to 8% of the estimated annual dose in 1990 and to 1% of the estimated annual dose in 1986. As a mean for the population group and for the period of the present study (2006-2008), the average yearly effective dose from Chernobyl cesium was comparable to the absorbed dose obtained annually from external exposure to cosmic radiation plus internal exposure to naturally occurring radionuclides in the human body. Our data indicate that the effective dose from internal exposure is becoming increasingly important as the body burdens of Chernobyl ¹³⁷Cs are decreasing more slowly than the external exposure. However, over the years there have been large individual variations in both the external and internal effective doses, as well as differences between the villages investigated. These variations and differences are presented and discussed in this paper.     

Mapping of 137Cs deposition over eastern France 16 years after the Chernobyl accident

We observed the relationship between present-day 137Cs surface activity and the rainfall in May 1986 to establish a relevant map of 137Cs deposition over eastern France. This study was performed in an area of the lower Rh?ne valley where clayey soils are assumed to trap caesium efficiently. Based on the rainwater/airborne activity ratio deduced from this relationship, we verified that present-day activities, measured in clayey soils of this type, are relatively representative of the initial depositions. The interlocked contaminated areas of the resulting map can be related to rainfall occurrences, as is the case for all countries affected by the Chernobyl fallout. This map can be reasonably compared with those obtained for countries bordering France in terms of both activity levels and extent of homogeneous activity areas. Lastly, we demonstrate that it would not be possible to produce a coherent map of initial fallout by extending the campaign over the whole of the eastern territory based on present-day soil activity measurements alone. Hence, only the relationship between 137Cs deposition and the rainfall of the first week of May 1986 can be used to construct a map depicting the Chernobyl fallout over eastern France.     

Long-term trends in the uptake of radiocesium in Rozites caperatus

Measurements of (134)Cs and (137)Cs in Rozites caperatus from 1991 to 2001 showed differences in the uptake pattern of Chernobyl and fallout derived radiocesium over time. The effective half-life of Chernobyl derived (137)Cs was determined to 12.4 years, whereas fallout derived (137)Cs had an effective half-life of 9.8 years. However, the trend for Chernobyl derived (137)Cs was clearly not linear. An effective average half-life of 3.1 years was determined for Chernobyl derived (137)Cs in the period from 1991 to 1994. The corresponding ecological half-life was 3.4 years. In the period from 1994 to 2001 it is possible that the effective half-life was longer than the physical, which indicates that more Chernobyl cesium becomes available than disappears through radioactive decay. The difference may be due to depth distribution of radiocesium, i.e. fallout derived cesium have penetrated deeper than Chernobyl. The changes in the half-lives of Chernobyl derived radiocesium over time together with the half-life of the older fallout derived radiocesium may be valuable in predictions of future radiocesium concentrations in mushrooms and thereby of food chain transfer to man.     

Chernobyl fallout in the uppermost (0-3 cm) humus layer of forest soil in Finland, North East Russia and the Baltic countries in 2000--2003

The situation resulting from the Chernobyl fallout in 1987 was compared to that in 2000--2001 in Finland and NW Russia and that in 2003 in the Baltic countries. 786 humus (0-3 cm layer) samples were collected during 2000--2001 in the Barents Ecogeochemistry Project, and 177 samples in the Baltic countries in 2003. Nuclides emitting gamma-radiation in the 0-3 cm humus layer were measured by the Radiation and Nuclear Safety Authority-STUK in Finland. In 1987 the project area was classified by the European Commission into four different fallout classes. 137Cs inventory Bg/m2 levels measured in 2000--2003 were compared to the EU's class ranges. Fitting over the whole project area was implemented by generalizing the results for samples from the Baltic countries, for which Bq/m2 inventories could be calculated. A rough estimation was made by comparing the mass of organic matter and humus with 137Cs concentrations in these two areas. Changes in 137Cs concentration levels are illustrated in both thematic maps and tables. Radionuclide 137Cs concentrations (Bq/kg d.w.) were detected in the humus layer at all the 988 sampling sites. 134Cs was still present in 198 sites 15 years after the nuclear accident in Chernobyl. No other anthropogenic nuclides emitting gamma-radiation were detected, but low levels of 60Co, 125Sb and 154Eu isotopes were found in 14 sites. Fifteen years after the Chernobyl accident, the radioactive nuclide 137Cs was and still is the most significant fallout radionuclide in the environment and in food chains. The results show that the fallout can still be detected in the uppermost humus layer in North East Europe.     

137Cs loss via soil erosion from a mountainous headwater catchment in central Japan

Eroded sediment and coarse organic material were sampled for a year at the outlet of the study catchment in central Japan to investigate characteristics of 137Cs loss and to quantify erosional 137Cs loss in a forested headwater catchment. Results showed that loss of both eroded sediment and 137Cs varied markedly according to the magnitude of rainfall events. About 90% of the total sediment delivery and the total 137Cs loss was associated with only two storm rainfall events. The significant contribution of high-magnitude-low-frequency storm events to 137Cs loss from the catchment was emphasized. To quantify the contribution of erosional 137Cs loss to 137Cs cycling, the current mean 137Cs inventory of the study catchment was estimated from direct measurements of 137Cs in soil cores collected from 27 points. The input of 137Cs through litterfall to the soil was estimated from monitoring the annual litterfall of the study catchment. The present 137Cs fallout input was estimated from published 137Cs fallout data. Consequently, the loss of 137Cs associated with eroded sediment was estimated to represent 0.013% of the 137Cs inventory of the study catchment, which is comparable to the input through litterfall. The equivalent value for 137Cs runoff with coarse organic material was estimated as 0.0003%. Therefore, the effect of 137Cs loss in association with coarse organic material on estimates of erosion rate obtained by measuring 137Cs inventories in soil core samples was inferred to be negligible in Japanese cypress plantations. Results confirm the applicability of 137Cs measurements to estimate erosion rates in other relatively stable forested areas.     

Caesium-137 migration in Hungarian soils

Distribution of 137Cs activity concentration has been measured in soils from 19 Hungarian counties. The levels of soil contamination in Hungary after the Chernobyl fallout are sufficient to study the vertical distribution of the 137Cs under natural conditions. Samples were taken layer by layer on plain, grassy and uncultivated fields down to a depth of 20 cm. The results show that radiocaesium migrates very slowly in the soils investigated. The 137Cs concentration peaks in almost all of the soils remain in the top 5 cm layer, but the distribution patterns are different. Variations in diffusion, sorption-desorption, and complexing processes, plant uptake and plant- and animal-originated mechanical changes result in the formation of site-specific radionuclide distribution profiles. On the basis of the experimental data a model has been developed for the long-term prediction of the 137Cs migration. By application of an applied diffusion-convection model the results can be well fitted, the initial deposition can be calculated and the data can be used for the long-term prediction of the 137Cs distribution profile.