Geochemical evaluation of different groundwater–host rock systems for radioactive waste disposal

The geochemical suitability of a deep bedrock repository for radioactive waste disposal is determined by the composition of geomatrix and groundwater. Both influence radionuclide solubility, chemical buffer capacity and radionuclide retention. They also determine the chemical compatibility of waste forms, containers and backfill materials. Evaluation of different groundwater–host rock systems is performed by modeling the geochemical environments and the resulting radionuclide concentrations. In order to demonstrate the evaluation method, model calculations are applied to data sets available for various geological formations such as granite, clay and rocksalt.The saturation state of the groundwater–geomatrix system is found to be fundamental for the evaluation process. Hence, calculations are performed to determine if groundwater is in equilibrium with mineral phases of the geological formation. In addition, corrosion of waste forms in different groundwater is examined by means of reaction path modeling. The corrosion reactions change the solution compositions and pH, resulting in significant changes of radionuclide solubilities. The results demonstrate that geochemical modeling of saturation state and compatibility of the host formation environment with the radioactive waste proves to be a feasible tool for evaluation of various sites considered as deep underground repositories.     

Regional-scale application of the decision support system MOIRA-PLUS: an example of assessment of the radiological impact of the Chernobyl accident on the fresh water ecosystem in Italy

The present work illustrates the customisation and application of the decision support system MOIRA-PLUS (a MOdel-based computerised system for management support to Identify optimal remedial strategies for Restoring radionuclide contaminated Aquatic ecosystems and drainage areas) to the fresh water environment in Italy. MOIRA-PLUS is aimed at evaluating the behaviour of radiocaesium and radiostrontium in fresh water ecosystems and at assessing the appropriateness of suitable strategies for the management of contaminated water bodies by the application of multi-attribute analysis techniques. MOIRA-PLUS can be applied to complex networks of lakes, rivers and tributaries and can be straightforwardly customised utilising data and information from readily accessible sources such as official websites provided by scientific or government organisations. The present work shows an application of the decision system to 10 lakes and 18 rivers in Italy contaminated with ¹³⁷Cs of Chernobyl origin. Site-specific values of some aggregated transfer parameters were estimated for the most important Italian lakes. Although high values of fish and water consumptions were hypothesised, very low doses to public from the fresh water pathway following the accident were calculated.     

Watershed wash-off of atmospherically deposited radionuclides: a review of normalized entrainment coefficients

Radionuclide wash-off is the transport of activity by flowing water over the soil surface (runoff). To complete existing reviews on long-term removal rates, this paper focuses on short-term wash-off fluxes, quantified in the literature by soil-runoff transfer factors called normalized liquid and solid entrainment coefficients (noted K(l)(*), K(s)(*)). Compiled data concerned essentially (137)Cs and (90)Sr wash-off measured under simulated rainfalls on small experimental plots after Chernobyl fallout in the exclusion zone. K(l)(*) and K(s)(*) values span approximately one order of magnitude. Their validity is limited to a season, and their representativeness is limited by restricted studied situations, notably dominant unsoluble forms in fallout, light soils and intense rainfalls. Formulas based on a simplified representation of the soil-runoff system were proposed to generalize the existing values for other conditions. However, their implementation requires a more systematic compilation of the available information, including decisive influence factors such as the fraction of exchangeable form, distribution coefficient, suspended matter enrichment ratio. Entrainment coefficients K(l)(*) and K(s)(*) were mathematically related to the transfer function approach. The proposed relationships proved their complementarity in terms of time support and captured fluctuations. Both approaches should be used in assessments to estimate average fluxes and their variability.     

The role of physical processes controlling the behaviour of radionuclide contaminants in the aquatic environment: a review of state-of-the-art modelling approaches

This paper is aimed at presenting and discussing the methodologies implemented in state-of-the-art models for predicting the physical processes of radionuclide migration through the aquatic environment, including transport due to water currents, diffusion, settling and re-suspension. Models are briefly described, model parameter values reviewed and values recommended. The different modelling approaches are briefly classified and the advantages and disadvantages of the various model approaches and methodologies are assessed.     

Transfer parameter values in temperate forest ecosystems: a review

Compared to agricultural lands, forests are complex ecosystems as they can involve diverse plant species associations, several vegetative strata (overstorey, shrubs, herbaceous and other annual plant layer) and multi-layered soil profiles (forest floor, hemi-organic and mineral layers). A high degree of variability is thus generally observed in radionuclide transfers and redistribution patterns in contaminated forests. In the long term, the soil compartment represents the major reservoir of radionuclides which can give rise to long-term plant and hence food contamination. For practical reasons, the contamination of various specific forest products has commonly been quantified using the aggregated transfer factor (T_ag in m² kg⁻¹) which integrates various environmental parameters including soil and plant type, root distribution as well as nature and vertical distribution of the deposits. Long lasting availability of some radionuclides was shown to be the source of much higher transfer in forest ecosystems than in agricultural lands. This study aimed at reviewing the most relevant quantitative information on radionuclide transfers to forest biota including trees, understorey vegetation, mushrooms, berries and game animals. For both radiocaesium and radiostrontium in trees, the order of magnitude of mean T_ag values was 10⁻³ m² kg⁻¹ (dry weight). Tree foliage was usually 2–12 times more contaminated than trunk wood. Maximum contamination of tree components with radiocaesium was associated with (semi-)hydromorphic areas with thick humus layers. The transfer of radionuclides to mushrooms and berries is high, in comparison with foodstuffs grown in agricultural systems. Concerning caesium uptake by mushrooms, the transfer is characterized by a very large variability of T_ag, from 10⁻³ to 10¹ m² kg⁻¹ (dry weight). For berries, typical values are around 0.01–0.1 m² kg⁻¹ (dry weight). Transfer of radioactive caesium to game animals and reindeer and the rate of activity reduction, quantified as an ecological half-life, reflect the soil and pasture conditions at individual locations. Forests in temperate and boreal regions differ with respect to soil type and vegetation, and a faster decline of muscle activity concentrations in deer occurs in the temperate zone. However, in wild boar the caesium activity concentration shows no decline because of its special feeding habits. In the late phase, i.e. at least a few months since the external radionuclide contamination on feed plants has been removed, a T_ag value of 0.01 m² kg⁻¹ (fresh weight) is common for ¹³⁷Cs in the muscles of adult moose and terrestrial birds living in boreal forests, and 0.03 m² kg⁻¹ (fresh weight) for arctic hare. Radiocaesium concentrations in reindeer muscle in winter may exceed the summer content by a factor of more than two, the mean T_ag values for winter ranging from 0.02 to 0.8 m² kg⁻¹ (fresh weight), and in summer from 0.04 to 0.4 m² kg⁻¹. The highest values are found in the year of initial contamination, followed by a gradual reduction. In waterfowl a relatively fast decline in uptake of ¹³⁷Cs has been found, with T_ag values changing from 0.01 to 0.002 m² kg⁻¹ (fresh weight) in the three years after the contaminating event, the rate being determined by the dynamics of ¹³⁷Cs in aquatic ecosystems.     

Radionuclide transfer to freshwater biota species: review of Russian language studies

Around 130 publications reporting studies on radionuclide transfer to freshwater biota species conducted in the former USSR were reviewed to provide the concentration ratio values. None of these studies were available up to now in the English language reviews or publications. The values derived have been compared with the CR values used for freshwater systems in the International reviews. For some radionuclides reviewed in this paper, the data are in good agreement with the mean CR values presented earlier, however for some of them, in particular, for ²⁴¹Am (bivalve molluscs, gastropods and pelagic fish), ⁶⁰Co (gastropods, benthic fish and insect larvae), ⁹⁰Sr and ¹³⁷Cs (benthic fish and zooplankton), the mean values given here are substantially different from those presented earlier. The data reported in this paper for thirty five radionuclides and eleven groups of freshwater species markedly improve the extent of available data for evaluation of radiation impact on freshwater species.     

The influence of colloid formation in a granite groundwater bentonite porewater mixing zone on radionuclide speciation

In the context of deep geological storage of high level nuclear waste the repository will be designed as multiple barrier system including bentonite as buffer/backfill material and the host rock formation as geological barrier. The engineered barrier (bentonite) will be in contact with the host rock formation and consequently it can be expected that bentonite porewater will mix with formation groundwater. We simulate in this study the mixing of Grimsel groundwater (glacial melt water) with synthetic Febex porewater (assuming already saturated state) in a batch-type study and investigate the formation of colloids by laser-induced breakdown detection (LIBD) and SEM-EDX as well as the changes in radionuclide (U, Th, Eu) speciation via ultrafiltration or via time-resolved laser fluorescence spectroscopy (TRLFS) analysis in the case of Cm(III). Based on PHREEQC saturation index (SI) calculations a precipitation of calcite might be expected at low Febex porewater (FPW) content (< 20%), fluorite precipitation at FPW contents < 60% and gibbsite precipitation at FPW contents above 10%. The colloids generated in the mixing zone aggregate when the synthetic FPW content exceeds 10%. LIBD analysis of the time-dependent colloid generation/aggregation revealed a low concentration of colloids to be stable with an estimated plateau value around 100–200 ppt and an average colloid diameter around 30 nm after 140 days reaction time at FPW admixture > 10%. SEM/EDX mostly identifies Al/Si containing colloidal phases and some sulfates could be found under certain admixture ratios. TRLFS studies show that the Cm speciation is strongly influenced by colloid formation in all solutions. In the Febex pore water/GGW mixing zone with high groundwater contents (> 80%) colloids are newly formed and Cm is almost quantitatively associated with most likely polysilicilic acid colloids.     

Characterization of ²⁴¹ Am and ¹³⁴Cs bioaccumulation in the king scallop Pecten maximus: investigation via three exposure pathways

In order to understand the bioaccumulation of ²⁴¹Am and ¹³⁴Cs in scallops living in sediments, the uptake and depuration kinetics of these two elements were investigated in the king scallop Pecten maximus exposed via seawater, food, or sediment under laboratory conditions. Generally, ²⁴¹Am accumulation was higher and its retention was stronger than ¹³⁴Cs. This was especially obvious when considering whole animals exposed through seawater with whole-body concentration factors (CF_7d) of 62 vs. 1, absorption efficiencies (A_0l) of 78 vs. 45 for seawater and biological half-lives (T_b½l) of 892 d vs. 22 d for ²⁴¹Am and ¹³⁴Cs, respectively. In contrast, following a single feeding with radiolabelled phytoplankton, the assimilation efficiency (AE) and T_b½l of ¹³⁴Cs were higher than those of ²⁴¹Am (AE: 28% vs. 20%; T_b½l: 14 d vs. 9 d). Among scallop tissues, the shells always contained the higher proportion of the total body burden of ²⁴¹Am whatever the exposure pathway. In contrast, the whole soft parts presented the major fraction of whole-body burden of ¹³⁴Cs, which was generally associated with muscular tissues. Our results showed that the two radionuclides have contrasting behaviors in scallops, in relation to their physico-chemical properties.     

Laboratory migration experiments with radionuclides and natural colloids in a granite fracture

Natural colloids in groundwater could facilitate radionuclide transport, provided the colloids are mobile, are present in sufficient concentrations and can adsorb radionuclides. This paper describes the results of a laboratory migration study carried out with combinations of radionuclides and natural colloids within a fracture in a large granite block to experimentally determine the impact of colloids on radionuclide transport. The 85Sr used in this study is an example of a moderately sorbing radionuclide, while the 241Am is typical of a strongly sorbed radionuclide with very low solubility. The natural colloids used in this study were isolated from granite groundwater from Atomic Energy of Canada (AECL) Underground Research Laboratory (URL), and consisted of mostly 1-10 nm organic colloids, along with lesser amounts of 10-450 nm colloids (organics and aluminosilicates). The measured coefficients for radionuclide sorption onto these colloids were between 3 x 10(2) and 1 x 10(3) ml/g for 85Sr, and between 7 x 10(4) and 7 x 10(5) mg/l for 241Am. The 85Sr sorption on the natural colloids appeared to be reversible. Migration experiments in the granite block were carried out by establishing a flow field between two boreholes (out of a total of nine) intersecting a main horizontal fracture. These experiments showed that dissolved 85Sr behaved as a moderately sorbing tracer, while dissolved 241Am was completely adsorbed by the fracture surfaces and showed no evidence of transport. However, when natural colloids were injected together with dissolved 241Am, a small amount of 241Am transport was observed, demonstrating the ability of natural colloids to facilitate the transport of radionuclides with low solubility. Natural colloids had only a minor effect on the transport of 85Sr. In a separate experiment to test the effect of higher colloid concentrations on 85Sr migration, synthetic colloids were produced from Avonlea bentonite. The introduction of a relatively high concentration of bentonite colloids actually reduced 85Sr transport because, compared to natural colloids, the bentonite colloids were less mobile and they sorbed 85Sr more strongly.