Review and assessment of models used to predict the fate of radionuclides in lakes

A variety of models for predicting the behaviour of radionuclides in fresh water ecosystems have been developed and tested during recent decades within the framework of many international research projects. These models have been implemented in Computerised Decision Support Systems (CDSS) for assisting the appropriate management of fresh water bodies contaminated by radionuclides. The assessment of the state-of-the-art and the consolidation of these CDSSs has been envisaged, by the scientific community, as a primary necessity for the rationalisation of the sector. The classification of the approaches of the various models, the determination of their essential features, the identification of similarities and differences among them and the definition of their application domains are all essential for the harmonisation of the existing CDSSs and for the possible development and improvement of reference models that can be widely applied in different environmental conditions. The present paper summarises the results of the assessment and evaluation of models for predicting the behaviour of radionuclides in lacustrine ecosystems. Such models were developed and tested within major projects financed by the European Commission during its 4th Framework Programme (1994-1998). The work done during the recent decades by many modellers at an international level has produced some consolidated results that are widely accepted by most experts. Nevertheless, some new results have arisen from recent studies and certain model improvements are still necessary.     

Estimation of animal transfer factors for radioactive isotopes of iodine,technetium, selenium and uranium

In post-closure radiological safety assessments of repositories for solid radioactive wastes, transfers of radionuclides to animal products are typically characterised using Transfer Factors (TFs), defined as the ratio of the concentration of the radionuclide in the animal product of interest to the rate of intake in diet. Such transfer factors can be measured directly in experimental studies, but they can also be estimated by use of biokinetic models for uptake and retention of radionuclides in animals. Based on a review of the literature, biokinetic models have been developed for the uptake and retention of iodine, technetium, selenium and uranium. These biokinetic models allow TF values to be estimated for different types of animals and for different animal lifetimes.For each radionuclide considered, reference values and ranges of TF values are estimated. These are summarised in Table 1.     

Probabilistic biokinetic modelling of radiocaesium uptake in Arctic seal species: verification of modelled data with empirical observations

The necessity to provide information about radionuclide concentrations in Arctic marine species has been heightened in recent years due to a number of accidents in Arctic regions involving nuclear vessels and the presence of a large number of potential radioactive contamination sources. The provision for such information is largely dependent on the use of radionuclide uptake and transfer models. The uptake of radionuclides in Arctic seal species in this study has been modelled using a probabilistic biokinetic approach. In this paper, model results are compared with empirical data from relevant samples taken within the Arctic region. Results indicate that the model performs well when estimating concentrations of (137)Cs in two seal species for both median values and reproduction of the distribution of data values, but not as well for a third seal species. Likely factors affecting the results are the probability density functions used for the input parameters.     

An overview of BORIS: Bioavailability of Radionuclides in Soils

The ability to predict the consequences of an accidental release of radionuclides relies mainly on the level of understanding of the mechanisms involved in radionuclide interactions with different components of agricultural and natural ecosystems and their formalisation into predictive models. Numerous studies and databases on contaminated agricultural and natural areas have been obtained, but their use to enhance our prediction ability has been largely limited by their unresolved variability. Such variability seems to stem from incomplete knowledge about radionuclide interactions with the soil matrix, soil moisture, and biological elements in the soil and additional pollutants, which may be found in such soils. In the 5th European Framework Programme entitled Bioavailability of Radionuclides in Soils (BORIS), we investigated the role of the abiotic (soil components and soil structure) and biological elements (organic compounds, plants, mycorrhiza, and microbes) in radionuclide sorption/desorption in soils and radionuclide uptake/release by plants. Because of the importance of their radioisotopes, the bioavailability of three elements, caesium, strontium, and technetium has been followed. The role of one additional non-radioactive pollutant (copper) has been scrutinised in some cases. Role of microorganisms (e.g., K(d) for caesium and strontium in organic soils is much greater in the presence of microorganisms than in their absence), plant physiology (e.g., changes in plant physiology affect radionuclide uptake by plants), and the presence of mycorrhizal fungi (e.g., interferes with the uptake of radionuclides by plants) have been demonstrated. Knowledge acquired from these experiments has been incorporated into two mechanistic models CHEMFAST and BIORUR, specifically modelling radionuclide sorption/desorption from soil matrices and radionuclide uptake by/release from plants. These mechanistic models have been incorporated into an assessment model to enhance its prediction ability by introducing the concept of bioavailability factor for radionuclides.     

Deposition of gaseous radionuclides to fruit

14C, 35S and 3H are released to the environment during the operation of gas-cooled reactors and were identified as radionuclides of interest by the BIOMASS Fruits Working Group. This paper provides a review of the deposition, uptake, allocation and loss of these radionuclides with respect to fruit and conceptual models for gaseous radionuclides. It is concluded that the mechanisms for the uptake of CO35S, HTO and 14CO2 are well understood and that their deposition velocities have been quantified. There is also a reasonable body of work on the translocation of 14C once in the crop, but much less for 35S and 3H, which are considered to follow source-sink relationships. The loss rates of the three radionuclides show large differences, with tritium lost rapidly in the form of HTO but retained longer when converted to OBT. The losses of 14C are less and those of sulphur are minimal post fixation. When fruit crops alone are considered, the quantity of information is further reduced but predictions on possible behaviour of these radionuclide species can be made from the current knowledge.     

Radioecological consequences of a potential accident during transport of spent nuclear fuel along an Arctic coastline

This article presents results pertaining to a risk assessment of the potential consequences of a hypothetical accident occurring during the transportation by ship of spent nuclear fuel (SNF) along an Arctic coastline. The findings are based on modelling of potential releases of radionuclides, radionuclide transport and uptake in the marine environment. Modelling work has been done using a revised box model developed at the Norwegian Radiation Protection Authority. Evaluation of the radioecological consequences of a potential accident in the southern part of the Norwegian Current has been made on the basis of calculated collective dose to man, individual doses for the critical group, concentrations of radionuclides in seafood and doses to marine organisms. The results of the calculations indicate a large variability in the investigated parameters above mentioned. On the basis of the calculated parameters the maximum total activity (“accepted accident activity”) in the ship, when the parameters that describe the consequences after the examined potential accident are still in agreement with the recommendations and criterions for protection of the human population and the environment, has been evaluated.     

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.     

On the sensitivity of a marine dispersion model to parameters describing the transfers of radionuclides between the liquid and solid phases

The sensitivity of a marine dispersion model for non-conservative radionuclides, previously developed and validated for the English Channel, to parameters describing the exchanges between the liquid and solid phases (suspended matter and bottom sediments) has been studied using a Monte Carlo method. A probability distribution is assigned to each parameter. They are sampled to obtain a set of model parameters and a model run is carried out. This process is repeated to obtain a distribution of model outputs. Partial correlation coefficients are calculated to assess the relative influence of each parameter on model output. Errors are also assigned to model results. Three situations are studied: an instantaneous release of radionuclides, a continuous release and the case of a contaminated sediment behaving as a long-term source of radionuclides. Calculations have also been carried out for two radionuclides with different geochemical behaviour: (137)Cs and (239,240)Pu. The results indicate that all parameters are relevant, depending on the phase we are interested in obtaining the result and on the source term (instantaneous, continuous or due to sediments). However, parameters that are, in general, more influential are kinetic rates, mixing depth in the sediment and mean radius of suspended and sediment particles. This suggests that including several particle sizes in future radionuclide dispersion models could lead to an improvement in model results. Differences have also been found with respect to the relevance of some parameters depending on the geochemical behaviour of the radionuclide.     

The significance of agricultural vs. natural ecosystem pathways in temperate climates in assessments of long-term radiological impact

Recent developments in performance assessment biosphere models have begun to emphasise the importance of natural accumulation pathways. In contrast to the agricultural pathways, the database for natural ecosystem pathways is less well developed, leading to a mismatch in quality of representations of the two types of system. At issue is the lack of reliable soil-plant and animal ingestion transfer factors for key radionuclides in natural ecosystems. The relative importance of the agricultural vs. natural ecosystem pathways is investigated here, in the context of a temperate site in present day, Eastern France. The BIOMASS Candidate Critical Group (CCG) methodology has been applied to map a set of eight candidate critical groups derived from the present-day societal context onto physical locations within a simple model of a river catchment system. The overall assessment model has been implemented using the Aquabios code. Annual individual dose to each of the CCGs has been calculated for each of the key radionuclides (79Se, 94Nb, 99Tc, 129I, 135Cs and 237Np) released to the valley aquifer and river. In addition to the traditional agricultural pathways, lifestyle groups exploiting natural habitats are explicitly addressed. Results show the susceptibility of different candidate critical groups to different radionuclides. A reference database typical of those employed in long-term performance assessment models is employed. Doses from external exposure (94Nb) and dust inhalation (237Np) are shown to dominate agricultural food consumption by factors of more than six, but, with the reference data set, foodstuffs obtained from natural ecosystems do not contribute significantly to critical group dose and, at most, show similar exposures to the agricultural pathways. This may lead to the conclusion that natural food can be ruled out of consideration in performance assessment models. However, systematic parametric sensitivity studies carried out on soil-plant and animal ingestion transfer factors restrict the validity of this observation and demonstrate the limitations of existing databases. Remaining uncertainties can be reduced by improving structural models for performance assessment and by better characterisation of sources of locally obtained foods. Improved characterisation of radionuclide accumulation in natural ecosystems in temperate as well as alternative future climate states should complement the modelling approach.     

Transport and fate of radionuclides in aquatic environments--the use of ecosystem modelling for exposure assessments of nuclear facilities

In safety assessments of nuclear facilities, a wide range of radioactive isotopes and their potential hazard to a large assortment of organisms and ecosystem types over long time scales need to be considered. Models used for these purposes have typically employed approaches based on generic reference organisms, stylised environments and transfer functions for biological uptake exclusively based on bioconcentration factors (BCFs). These models are of non-mechanistic nature and involve no understanding of uptake and transport processes in the environment, which is a severe limitation when assessing real ecosystems. In this paper, ecosystem models are suggested as a method to include site-specific data and to facilitate the modelling of dynamic systems. An aquatic ecosystem model for the environmental transport of radionuclides is presented and discussed. With this model, driven and constrained by site-specific carbon dynamics and three radionuclide specific mechanisms: (i) radionuclide uptake by plants, (ii) excretion by animals, and (iii) adsorption to organic surfaces, it was possible to estimate the radionuclide concentrations in all components of the modelled ecosystem with only two radionuclide specific input parameters (BCF for plants and Kd). The importance of radionuclide specific mechanisms for the exposure to organisms was examined, and probabilistic and sensitivity analyses to assess the uncertainties related to ecosystem input parameters were performed. Verification of the model suggests that this model produces analogous results to empirically derived data for more than 20 different radionuclides.     

Review and assessment of models for predicting the migration of radionuclides through rivers

The present paper summarises the results of the review and assessment of state-of-the-art models developed for predicting the migration of radionuclides through rivers. The different approaches of the models to predict the behaviour of radionuclides in lotic ecosystems are presented and compared. The models were classified and evaluated according to their main methodological approaches. The results of an exercise of model application to specific contamination scenarios aimed at assessing and comparing the model performances were described. A critical evaluation and analysis of the uncertainty of the models was carried out. The main factors influencing the inherent uncertainty of the models, such as the incompleteness of the actual knowledge and the intrinsic environmental and biological variability of the processes controlling the behaviour of radionuclides in rivers, are analysed.     

Transfer of radium-228, thorium-228 and radium-226 from forage to cattle and reindeer

Concentrations of radium-228, thorium-228 and radium-226 were measured in different natural forage materials and in feed supplements. The activity concentrations of these nuclides were then determined in the bones of domestic farm animals, with emphasis on their distributions within the skeleton and humerus. Feeds added in recent years to the forage of domestic animals alter the concentrations of the naturally occurring radionuclides. The modified daily radium uptakes associated with the various feeds are reflected in the radium concentrations observed in the different layers of the humerus. Radium uptake and retention are highly dependent on calcium metabolism.We propose a method for calculation of nuclide retention coefficients via an approach which simplifies theis assesssment and provides important information on radium metabolism. The data obtained here are of value in dosimetric assessments related to these natural radionuclides.     

The influence of the development of temperate fruit tree species on the potential for their uptake of radionuclides

This paper reviews the published literature that describes the phenological development of above and below ground organs of temperate fruit trees (top fruit), particularly with respect to apple (Malus domestica). Critical information is presented which is considered appropriate in developing an understanding of the potential for top fruit species to take up radionuclide contaminants from the atmosphere and the soil. Information is cited on how climatic and edaphic factors influence the growth and development of temperate fruit trees, the phenological production of their leaf area and the development and growth of their fruit and hence the potential for foliar and fruit uptake of radionuclides from the atmosphere. The study also reports on the importance of the distribution and phenological development of roots in the soil and the potential for their uptake of radionuclides from the soil. The effects of above and below ground management procedures, within temperate fruit orchards, on potential radionuclide uptake are also considered. It is concluded that the potential for the uptake of radionuclides by temperate fruit tree species will depend on a number of phenological and physiological factors. For uptake from the soil these factors include; root distribution and density in the soil profile, seasonal changes in the production and distribution of roots, and the presence and amount of water in the soil. These factors are themselves influenced by rootstock type and its growth vigour, scion type and its growth vigour, tree age, spacing of trees in the orchard, orchard management practices (presence or absence of weeds or grass under the trees) and soil type and depth. Direct uptake by the shoot, however, will be influenced by the climatic conditions at the time of exposure and the presence of foliage. Deposition and uptake are likely to change with leaf area development and the ability of radionuclides to penetrate the cuticle of the leaf changes with seasonal development. Transport of radionuclides to the fruit may also depend on the time of season, as the importance of the xylem and phloem transport routes can change with the growth and development of the fruit.     

Modified approach to modelling radiological consequences from releases into the marine environment

One of the general assumptions for box modelling of the dispersion of radionuclides in marine systems relates to instantaneous mixing in each box which, in turn, results in practical calculations involving instantaneous mixing in the whole of oceanic space. A new approach to box modelling, which includes dispersion of radionuclides as a function of time, was therefore developed in order to provide a better and more realistic/physical approximation to reality relative to traditional box modelling. The novel and significant practical features of the approach are discussed. Calculations of concentrations of radionuclides in the marine environment and doses to man for some scenarios indicate differences of up to orders of magnitude between the traditional and new approaches to box modelling.     

A probabilistic approach to obtaining limiting estimates of radionuclide concentration in biota

The US Department of Energy has developed a graded approach for evaluating radiation doses to biota. Limiting concentrations of radionuclides in water, soil, and sediment were derived for twenty-three radionuclides. Four organism types (aquatic animals, riparian animals, terrestrial animals, and terrestrial plants) were selected as the basis for method development. While environmental transfer data needed for deriving biota tissue concentrations are available for aquatic animals and terrestrial plants, less information is available for terrestrial and riparian organisms. Two methods were applied and examined for their ability to provide estimates of organism:soil or organism:water concentration factors in lieu of measured data. The kinetic/allometric approach combined with a parameter uncertainty analysis provides a needed method to estimate concentration factors across multiple species with limited input data.     

The influence of hot particle contamination on Sr and Cs transfers to milk and on time-integrated ingestion doses

Most models for transfers of radionuclides through the food chain typically assume that the radioactivity is initially deposited in chemically available forms. It is known, however, that releases of radionuclides in the form of hot particles may significantly influence their environmental transfers and uptake to the food chain. This study presents models for time changes in ⁹⁰Sr and ¹³⁷Cs in milk which incorporate hot particle contamination using observed rates of hot particle dissolution following the Chernobyl accident. A general equation is presented for the influence of hot particles on overall ingestion doses. As expected from previous work, fallout of hot particles significantly influences time changes in radionuclide activity concentrations in foodstuffs. It is also shown that incorporation of radionuclides in hot particles influences time-integrated ingestion doses. For a situation in which a large proportion (90–100%) of fallout is in slowly dissolving hot particles, time-integrated ingestion doses from ⁹⁰Sr and ¹³⁷Cs are reduced by a factor of approximately two compared to the case where all radioactivity is deposited in bioavailable forms. However, the influence of rapidly dissolving hot particles on time-integrated ingestion doses is relatively minor. Remaining significant uncertainties in dose estimates are discussed.     

Mycorrhizal association of maritime pine, Pinus pinaster, with Rhizopogon roseolus has contrasting effects on the uptake from soil and root-to-shoot transfer of 137Cs, 85Sr and 95mTc

The beneficial role of mycorrhizal association on plant nutrition and water supply is well-known, however, very little information exists with respect to the availability of radionuclides. We have measured the effect of controlled mycorrhizal association on the root uptake from soil and accumulation in leaves of three radionuclides. The radionuclides have contrasting chemical and biological properties: Cs is strongly adsorbed on soil, has no biological role and is a close analogue of potassium; Sr is less strongly adsorbed on soil and behaves very similarly to calcium; and Tc is very mobile in soil as pertechnetate, but immobilised when reduced to Tc(IV), it is also considered to be easily assimilated by biological systems. We found that mycorrhizal association had no effect on root-to-needle transfer of Cs, but increased root uptake and that this increase could not be explained by improved potassium nutrition. In contrast, the symbiotic relation decreased Tc soil-to-needle transfer, but this resulted from complex dynamics of root uptake and rapid immobilisation of Tc in soil. No effect of mycorrhizal association on Sr, like its stable analogue Ca, was observed. The addition of a phytotoxic metal, Cu, inhibited mycorrhizal association, thus eliminating the effects observed for non-contaminated plant-fungus couples, but had no additional effect on radionuclide dynamics.     

Some physical and chemical features of the variability of kd distribution coefficients for radionuclides

k_d distribution coefficients are widely used as a first approach to the understanding and determination of the eventual fate of metals and radionuclides released into the aquatic environment. For some radionuclides, k_d varies within a range of more than two orders of magnitude. Based on some physical and chemical aspects of the interactions between the dissolved and the particulate phases, some mathematical equations have been developed to explain some features of the observed k_d variability quantitatively. Thus, we have studied the decrease in particle size of k_d in the case of man-made radionuclides interacting with natural particles, and its increase in the case of naturally occurring radionuclides. For the latter, the dependence of k_d on the instantaneous water state has also been investigated. The study also shows the competition effects, particularly the dependence of k_d on pH and salinity. Finally, the effects produced by the size distribution of a given population of particles or the mixture of different populations, are also included. The present work provides for each situation, experimental support from literature data and/or modelling exercises.