Modelling the transport of radionuclides from land to water

This paper addresses some fundamental problems related to the structure and function of catchment areas in general and for seasonal (weekly, monthly) mass balance calculations of radionuclides (and metals, organics and nutrients) in particular. A new catchment area model has been developed and critically tested. This modelling approach is based on mechanistic principles. The catchment area is differentiated into inflow ( approximately dry land) areas and outflow (=wetland) areas. The model also accounts for time-dependent fixation of substances in the catchment related to single-pulse fallouts. The model has a general structure. It is simple to use since there are only two soil type classes and three categories for the outflow areas. In critical tests, the model was put within a framework where it is intended, i.e., within a more comprehensive lake model. Radiocesium was used as a tracer in these tests. Modelled values were compared to empirical data from 23 lakes (351 data on (137)Cs in water, as well as in sediments, small fish and on suspended particles) covering a very wide limnological domain (latitudes from 42 to 61 degrees V, altitudes from 0 to 1090 m ASL, catchment areas from 0.17 to 114,700 km(2), precipitation from 430 to 1840 mm/year, lake areas from 0.042 to 1147 km(2), mean depths from 1.1 to 90 m, pH from 5.1 to 9 units, potassium concentrations from 0.23 to 27.5 mg/l, total P concentrations from 8.3 to 100 microg/l and theoretical water retention times from 0.02 to 137 years). When modelled values were compared to empirical data, the slope was almost perfect (0.99) as well as the coefficient of determination (r2 = 0.96).     

Modelling multiple dispersion of radionuclides through the environment

The migration of a contaminant through the environment is the result of the transport by a variety of biotic and abiotic carriers which move according to different dispersion mechanisms. Consequently, the patterns of the distribution of a pollutant in the environment cannot be ever explained on the basis of a single migration process or assuming that the concentrations of contaminant in the different kinds of carriers quickly reach the equilibrium condition. The present work discusses two examples (wash-off from catchments and transport through soils of radionuclides) that clearly demonstrate the inadequacy of “single dispersion” models to predict these patterns. On the contrary, models based on multiple dispersion can successfully simulate the particular features of the above mentioned processes. It was demonstrated that the time behaviour of radionuclide migration rates from catchment of different rivers vary within small ranges as a consequence of multiple dispersion. This result can be useful for the development of generic predictive models.     

Evaluation of a model for leaf to fruit transfer of radionuclides in processing tomato plants using an independent set of data

Because of their varied possibilities of consumption, tomatoes are an important component of the human diet. This paper presents results of the evaluation of a dynamic model (Ventomod) for the short-term behaviour of radionuclides deposited on tomato plants following a direct contamination event. To check its forecasting capability in assessing the risk of radionuclide contamination of the human diet, it has been tested with an independent dataset on the leaf to fruit transfer of 134Cs in a typical Hungarian tomato variety, "Dwarf of Kecskemet". Data obtained from this pot experiment were used to evaluate model behaviour. Model constants were varied according to the differences between the Hungarian dataset and the one used to calibrate it. Results show that the model output well reproduces the observed activity of fruits for various levels of contamination and at different contamination dates. The main part of this report summarises the experimental protocol, compares the experimental results with model predictions generated by Ventomod and makes recommendations for both updating model parameters and undertaking further experimental work.     

Quantifying the transfer of radionuclides to food products from domestic farm animals

Databases have been compiled to derive parameter values relevant to the transfer of radionuclides from feedstuffs to domestic animal products to provide a revision to the IAEA Handbook on transfer parameters TRS 364. Significant new data inputs have been incorporated into the databases from an extensive review of Russian language information and inclusion of data published since the early 1990s. Fractional gastrointestinal absorption in adult ruminants presented in the revised handbook are generally similar to those recommended for adult humans by the ICRP. Transfer coefficient values are presented in the handbook for a range of radionuclides to farm animal products. For most animal products, transfer coefficient values for elements additional to those in TRS 364 are provided although many data gaps remain. Transfer coefficients generally vary between species with larger species having lower values than smaller species. It has been suggested that the difference is partly due to the inclusion of dietary dry matter intake in the estimation of transfer coefficient and that whilst dietary intake increases with size nutrient concentrations do not. An alternative approach to quantifying transfer by using concentration ratios (CR), which do not consider dietary intake, has been evaluated. CR values compiled for the handbook vary considerably less between species than transfer coefficient values. The advantage of the CR approach is that values derived for one species could be applied to species for which there are no data. However, transfer coefficients will continue to be used as few studies currently report CR values or give data from which they can be estimated.     

The transfer of radionuclides from saltmarsh vegetation to sheep tissues and milk

Radionuclides released into the Irish Sea by the Sellafield reprocessing plant are deposited onto tide-washed pastures along the western coast of the United Kingdom. Many of these pastures are grazed by sheep or cattle. This paper describes a controlled feeding study, in which saltmarsh vegetation harvested from close to the Sellafield plant, was fed to lambs and adult female sheep for a period of 8 weeks. Activity concentrations of (60)Co, (95)Nb, (106)Ru, (134)Cs, (137)Cs, (238)Pu, (239,240)Pu and (241)Am were determined in edible tissues and transfer parameters estimated. The activity concentrations of some of the radionuclides will not have been in equilibrium with those in the diet. Nevertheless, the study was reasonably realistic in terms of agricultural management as the period of the study was similar to that for which lambs graze on the saltmarshes. A field study to determine the activity concentrations of (137)Cs and (239,240)Pu in the milk of ewes grazing a saltmarsh close to Sellafield is also described.     

Radionuclide transfer to fruit in the IAEA TRS 364 Revision

Information on the transfer of radionuclides to fruits was almost absent in the former TRS 364 “Handbook of parameter values for the prediction of radionuclide transfer in temperate environments”. The revision of the Handbook, carried out under the IAEA Programme on Environmental Modelling for RAdiation Safety (EMRAS), takes into account the information generated in the years following the Chernobyl accident and the knowledge produced under the IAEA BIOMASS (Biosphere Modelling and Assessment) Programme in the years 1997–2000. This paper describes the most important processes concerning the behaviour of radionuclides in fruits reported in the IAEA TRS 364 Revision and provides recommendations for research and modelling.     

A model testing study for the transfer of radioactivity to fruit

This paper compares predictions of the foodchain model SPADE with experimental data for the transfer of (134)Cs and (85)Sr to strawberry plants following acute foliar and soil contamination. The transfer pathways considered in this exercise included direct deposition to fruit, leaf-to-fruit, soil-to-leaf and soil-to-fruit transfers. Following foliar contamination, the difference between predicted and measured radionuclide activity values varied between a factor of 0.5-10 for fruit and 4.5-7 for leaf. Following soil contamination, the difference between predicted and measured values varied between a factor of 3-74 for fruit and 32-44 for leaf. In all cases the difference between measured and predicted values was smaller for (85)Sr than (134)Cs. Measured and predicted activities were higher for leaf than fruit. Both measured and predicted (134)Cs concentrations in fruit and leaf are higher when deposition occurs at ripening than at anthesis. These results confirm the need for more data on fruit, even for Cs and Sr, to support models in predicting the transfer of radionuclides to fruit crops. Ongoing research projects funded by the UK Food Standards Agency aim to provide some data on radionuclide transfer to herbaceous, shrub and tree fruits, which will help improve radiological assessment models in order to provide better protection for consumers.     

Modelling the reworking effects of bioturbation on the incorporation of radionuclides into the sediment column: implications for the fate of particle-reactive radionuclides in Irish Sea sediments

A microcosm laboratory experiment was conducted to determine the impact of biological reworking by the ragworm Nereis diversicolor on the redistribution of particle-bound radionuclides deposited at the sediment-water interface. Over the course of the 40-day experiment, as much as 35% of a ¹³⁷Cs-labelled particulate tracer deposited on the sediment surface was redistributed to depths of up to 11 cm by the polychaete. Three different reworking models were employed to model the profiles and quantify the biodiffusion and biotransport coefficients: a gallery-diffuser model, a continuous sub-surface egestion model and a biodiffusion model. Although the biodiffusion coefficients obtained for each model were quite similar, the continuous sub-surface egestion model provided the best fit to the data. The average biodiffusion coefficient, at 1.8 ± 0.9 cm² y⁻¹, is in good agreement with the values quoted by other workers on the bioturbation effects of this polychaete species. The corresponding value for the biotransport coefficient was found to be 0.9 ± 0.4 cm y⁻¹. The effects of non-local mixing were incorporated in a model to describe the temporal evolution of measured ⁹⁹Tc and ⁶⁰Co radionuclide sediment profiles in the eastern Irish Sea, influenced by radioactive waste discharged from the Sellafield reprocessing plant. Reworking conditions in the sediment column were simulated by considering an upper mixed layer, an exponentially decreasing diffusion coefficient, and appropriate biotransport coefficients to account for non-local mixing. The diffusion coefficients calculated from the ⁹⁹Tc and ⁶⁰Co cores were in the range 2-14 cm² y⁻¹, which are consistent with the values found by other workers in the same marine area, while the biotransport coefficients were similar to those obtained for a variety of macrobenthic organisms in controlled laboratories and field studies.     

Modelling of long-term behaviour of caesium and strontium radionuclides in the Arctic environment and human exposure

In this paper a compartment model of the highly vulnerable Arctic terrestrial food chain "lichen-reindeer-man" is outlined. Based upon an analysis of measured (137)Cs and (90)Sr contents in lichen and reindeer meat from 1961 up to 2001, site specific model parameters for two regions in north-western Arctic Russia and for Kautokeino municipality in Arctic Norway have been determined. The dynamics of radionuclide activity concentrations in the "lichen-reindeer-man" food chain for all areas was satisfactorily described by a double exponential function with short-term and long-term effective ecological half-lives between 1-2 and 10-12 years, respectively, for both (137)Cs and (90)Sr. Using parameter values derived from the model, life-time internal effective doses due to consumption of reindeer meat by reindeer-breeders after an assumed single pulse deposit of 1 kBq m(-2) of (137)Cs were estimated to be 11.4 mSv (Kola Peninsula), 5 mSv (Nenets Autonomous Area), and 2 mSv (Kautokeino, Norway). Differences in vulnerability to radiocaesium deposition were due to differences in transfer between lichen and reindeer and in diet between the three regions.     

Ventomod: a dynamic model for leaf to fruit transfer of radionuclides in processing tomato plants (Lycopersicon esculentum Mill.) following a direct contamination event

This paper presents results on the calibration and validation of a model (Ventomod) for leaf to fruit transfer of (134)Cs, (85)Sr and (65)Zn in processing tomato plants after leaf contamination. Several models (e.g. FARMLAND) that deal specifically with the transfer of radionuclides to fruits are adaptations of models that were developed for agricultural crops such as leafy green vegetables. "Ventomod" represents a dynamic evaluation model exclusively built for the short-term behaviour of radionuclide depositions. It forecasts the level of radionuclide contamination in ripe processing tomato fruits following an accidental radionuclide release into the atmosphere. A validation of the developed model by data sets from an independent experiment showed that the model successfully reproduced the observed radionuclide distribution and dynamics in tomato fruits. The level of uncertainty was within the normal range of similar assessment models. For a more general use of this model further testing with independent data sets from experiments obtained under different environmental conditions and data from other horticulturally important plant species would be desirable.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part II: aerial modelling and radiological assessment

Modelling calculations have been performed to predict the radiological impact of the sea to land transfer pathway to members of the public in North Wales from 1952 to 2004. The radionuclides of interest were (99)Tc, (137)Cs, (239,240)Pu and (241)Am and the exposure routes considered were food consumption, external and inhalation. The consumption of locally grown terrestrial food in the early to mid 1980s was the most significant source of exposure to all of the groups considered, with (239,240)Pu being the radionuclide contributing most to the dose. A maximum dose of 1.46muSvy(-1) was calculated for adult members of the critical consumption group in 1985, with doses for 2004 reducing to 0.59muSvy(-1). Despite the conservative approach of the dose calculations, the dose rate values are very low, less than 0.15% of the annual limit of 1000muSvy(-1) for the UK public from controlled radiation sources (excluding medical).     

Modelling radiocaesium transfer and long-term changes in reindeer

A dynamic model on (137)Cs in reindeer is presented, taking into consideration short- and long-term mechanisms, including the effect of ground deposition, transfer to vegetation, reindeer diet, feed intake, absorption and depletion of radiocaesium in the reindeer body. The model was optimised to fit measured activity concentrations in Swedish reindeer after the Chernobyl fallout. For comparison, regression analyses were made and aggregated transfer factors and effective ecological half-lives were estimated. The fit of the simulated model to observed activity concentrations was slightly better than the fit obtained by linear regressions. Improved knowledge about radiocaesium in vegetation would make the model more accurate for predictive purposes. Presently, the use of Tag and T(eff) is probably better for predictions, provided that their temporal and geographical limitations are taken into consideration. The dynamic model describes mechanisms better and may explain how changes in the system influence on activity concentrations of radiocaesium in the animal.     

Predicting soil-to-plant transfer of radionuclides with a mechanistic model (BioRUR)

BioRUR model has been developed for the simulation of radionuclide (RN) transfer through physical and biological compartments, based on the available information on the transfer of their nutrient analogues. The model assumes that radionuclides are transferred from soil to plant through the same pathways as their nutrient analogues, where K and Ca are the analogues of Cs and Sr, respectively. Basically, the transfer of radionuclide between two compartments is calculated as the transfer of nutrient multiplied by the ratio of concentrations of RN to nutrient, corrected by a selectivity coefficient. Hydroponic experiments showed the validity of this assumption for root uptake of Cs and Sr and reported a selectivity coefficient around 1.0 for both. However, the application of this approach to soil-to-plant transfer raises some questions on which are the effective concentrations of RN and nutrient detected by the plant uptake mechanism. This paper describes the evaluation of two configurations of BioRUR, one which simplifies the soil as an homogeneous pool, and the other which considers that some concentration gradients develop around roots and therefore ion concentrations at the root surface are different from those of the bulk soil. The results show a good fit between the observed Sr transfer and the mechanistic simulations, even when a homogeneous soil is considered. On the other hand, Cs transfer is overestimated by two orders of magnitude if the development of a decreasing K profile around roots is not taken into account.     

Soil-to-plant transfer factors for natural radionuclides and stable elements in a Mediterranean area

The transfer factors (TF) for natural uranium isotopes (238U and 234U), thorium isotopes (232Th, 230Th and 228Th), and 226Ra were obtained in plant samples (grass-pasture) growing in granitic and alluvial soils around a disused uranium mine located in the Extremadura region in the south-west of Spain. Affected and non-affected areas of the mine presented large differences in the activity concentrations of radionuclides of the uranium series. We also determined transfer factors for several stable elements (essential and non-essential). A set of statistical tests were applied to validate the data. The results showed that the transfer factors for both the natural radionuclides and the stable elements are independent of the two substrate types involved and also of the two areas considered in the study.     

Modelling 3H and 14C transfer to farm animals and their products under steady state conditions

The radionuclides (14)C and (3)H may both be released from nuclear facilities. These radionuclides are unusual, in that they are isotopes of macro-elements which form the basis of animal tissues, feed and, in the case of (3)H, water. There are few published values describing the transfer of (3)H and (14)C from feed to animal derived food products under steady state conditions. Approaches are described which enable the prediction of (14)C and (3)H transfer parameter values from readily available information on the stable H or C concentration of animal feeds, tissues and milk, water turnover rates, and feed intakes and digestibilities. We recommend that the concentration ratio between feed and animal product activity concentrations be used as it is less variable than the transfer coefficient (ratio between radionuclide activity concentration in animal milk or tissue to the daily intake of a radionuclide).     

Anthropogenic radionuclides in sediment in the Japan Sea: distribution and transport processes of particulate radionuclides

Distributions of anthropogenic radionuclides ((90)Sr, (137)Cs and (239+240)Pu) in seabed sediment in the Japan Sea were collected during the period 1998-2002. Concentration of (90)Sr, (137)Cs and (239+240)Pu in seabed sediment was 0.07-1.6 Bq kg(-1), 0.4-9.1 Bq kg(-1) and 0.002-1.9 Bq kg(-1), respectively. In the northern basin of the sea (Japan Basin), (239+240)Pu/(137)Cs ratios in seabed sediment were higher and their variation was smaller compared to that in the southeastern regions of the sea. The higher (239+240)Pu/(137)Cs ratios throughout the Japan Basin were considered to reflect production of Pu-enriched particles in the surface layer and substantial sinking of particulate materials in this region. In the southern regions of the Japan Sea (<38 degrees N), both inventories and (239+240)Pu/(137)Cs ratios in sediment were larger than those in the other regions. In the southern Japan Sea, observations suggested that supply of particulate radionuclides by the Tsushima Warm Current mainly enhanced accumulation of the radionuclides in this region.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part I: external gamma radiation and radionuclide concentrations in intertidal sediments, soil and air

Previous projects specifically aimed at performing radiological assessments in the vicinity of North Wales, investigating the presence and transfer of radionuclides from sea to land, were in 1986 and 1989. Since then, changes have occurred in the radioactive discharges from the British Nuclear Group Sellafield site. Annual discharges of (137)Cs, (238)Pu, (239,340)Pu and (241)Am have decreased markedly whereas, up until recent years, discharges of (99)Tc have increased. It is therefore desirable to quantify current transfer processes of radionuclides in the North Wales region and thus provide an update on 15-year-old studies. A field campaign was conducted collecting soil samples from 10 inland transects and air particulates on air filters from three High Volume Air Samplers, along the northern coast of Wales at Amlwch, Bangor Pier and Flint. Complementary field data relating to external gamma dose rates were collected at the soil sites. The field data generated for (137)Cs, (238)Pu, (239,340)Pu and (241)Am were consistent with what had been reported 15 years previously. Therefore, there has been no increase in the supply of these Sellafield-derived radionuclides to the terrestrial environment of the North Wales coast. The (99)Tc data in sediments were consistent with reported values within annual monitoring programmes, however, a relatively high activity concentration was measured in one sediment sample. This site was further investigated to determine the reason why such a high value was found. At present there is no clear evidence as to why this elevated concentration should be present, but the role of seaweed and its capacity in accumulating (99)Tc and transferring it to sediment is of interest. The analysis of the field samples for (99)Tc, (137)Cs, (238)Pu, (239,240)Pu and (241)Am has provided a data set that can be used for the modelling of the transfer of anthropogenic radionuclides from sea to land and its subsequent radiological implications and is reported in an accompanying paper.     

Soil-fungi transfer coefficients: Importance of the location of mycelium in soil and of the differential availability of radionuclides in soil fractions

Soil-fungus transfer coefficients are usually defined as the ratio between the content of the fruiting bodies and that of the soil. Since, however, the methodology of how to determine the soil content is not firmly established, there exist a variety of definitions in the literature. We analyzed the 137Cs, 90Sr, 40K, and 226Ra content of mushroom and soil samples from two pine-wood ecosystems in Spain. The location of the mycelium in the soil profiles of these ecosystems was determined by means of the ergosterol concentration. The results showed the mycelium to generally be localized in the surface layer of soil (0-5 cm). We also carried out a speciation procedure for this layer of soil to determine the different degrees of association of the radionuclides in the soil. The results led us to propose some variations to the traditional definition used in quantifying radionuclide transfer. With these modifications, we were able to analyze Cs-K competition in several species of mycorrhizal and saprophytic fungi.     

Natural radionuclides in Brazilian mineral water and consequent doses to the population

Based on production data published by the Brazilian Mineral Water Producers Association, bottled mineral waters were bought at the market, covering, at least, 50% of the annual production of each Brazilian geographical region. 228Ra, 226Ra and 210Pb were analyzed and the weighted mean values obtained for Brazilian mineral waters were 0.097, 0.027 and 0.066 Bq l-1 respectively. Individual effective dose rate estimates due to ingestion of mineral water in Brazil were of the order of 10-100 microSv yr-1, depending on the geographical region. Based on the available data, it was also possible to evaluate the per caput effective dose rate and the highest value obtained was 4.3 microSv yr-1 for the northern region.