Radioactive Waste Repository Research Articles

Review of secondary phases formed under natural alkaline conditions at low temperatures and implications for cement–bentonite interactions in radioactive waste repositories

Abstract The alteration of bentonite under alkaline conditions and the subsequent changes in properties such as permeability and self-sealing ability should be evaluated for the performance assessment of radioactive waste repositories. As the period of evaluation for alterations is extremely long, natural analog (NA) studies that can observe long-term phenomena similar to the system of radioactive waste repositories have significant advantages. However, locations that can be set up as NA study sites with significant similarity are limited and should be pursued by localizing analog systems. This literature review summarized studies reporting secondary phases formed at low temperatures (<100°C) under a broader range of natural sites which are chemically similar to the alkaline conditions expected at bentonite in radioactive waste repositories, including near pyrometamorphic rocks, near ophiolites, and in alkaline saline lakes. This review provides insights into the species, formation conditions, and stability of secondary phases that could be formed during cement–bentonite interactions and the timescale for mineralogical transitions from a metastable to a stable phase. The findings could be useful for selecting secondary phases to be considered in reactive transport modeling for predicting cement–bentonite interactions in radioactive waste repositories.

Radioactive waste Repository in Italy and annexed Technology Park

Radioactive waste is produced, in advanced industrial countries, by many activities, including medical, industrial and research fields. In Italy such waste, increasing year after year, has to be added to those deriving from nuclear activities. Italy operated Nuclear Power Plants (NPPs) until 1987, when they were shutdown after a referendum. After a ten year stand-by, in 1999 the Italian Government created SOGIN, a public company charged for NPPs decommissioning and for the safe and responsible management of the Italian radioactive waste, acting as a Waste Management Organisation (WMO). Such management, following international guidelines and best-practice, is framed and implemented in a holistic approach, Radioactive Waste Management (RWM), that aims to guarantee safety “from cradle to grave”, from the moment when a radioactive waste is produced to the moment when it can be disposed of accordingly to safety standards, that include a classification of radioactive waste, assigning specifical requirements for disposal of each category of waste. The overall amount of radioactive waste is described and analysed, in each country, in a National Inventory. The Italian National Inventory is composed of many and different waste streams. This situation was originated from a pioneering nuclear programme started in the early ’60s, from a spread and diversified industrial installations, and from publicly enhanced research and medical activities. Following international best practices, Italy has adopted and is implementing a National Programme for RWM, that provides the disposal of some 78 000 m3 of radioactive waste in a near-surface repository, the National Repository (NR). A smaller amount of radioactive waste, some 17 000 m3, will be hosted in the NR for a long-term interim storage (50 to 100 years), waiting for its final disposal in a Geological Disposal Facility (GDF), that is required to be built deeply underground. The siting procedure for the NR is designed following a “mixed-mode approach”, that combines technical and engineering criteria with others referred to societal and economic aspects, in order to draw a National Map of Potentially Suitable Areas. SOGIN drafted this Map in 2014, and held a Public Consultation and a National Workshop (2021) to discuss, with a wide range of stakeholders, modifications to be applied in a National Map of Suitable Areas, that is currently waiting for green light from the government for its publication. After the publication of the National Map of Suitable Areas, Regions and local communities concerned will be asked to issue an expression of interest, aimed to start consultation with SOGIN (Project’s Implementer) to define an agreement that includes the research of a suitable site in the territory to host the NR. Together with the NR, a Technology Park will be built to carry out activities related to the NR operations, and other activities to be developed in various branches, from radiological and environmental protection to research laboratories. The choice of activities to be developed will be agreed with hosting communities.

GIS-based multi-criteria assessment of areas suitable for the construction of a repository for low and intermediate level radioactive waste in Slovenia

GIS-based multi-criteria assessment of areas suitable for the construction of a repository for low and intermediate level radioactive waste in Slovenia

Uncertainties and robustness with regard to the safety of a repository for high-level radioactive waste: introduction of a research initiative

The Federal Company for Radioactive Waste Disposal (BGE mbH) is tasked with the selection of a site for a high-level radioactive waste repository in Germany in accordance with the Repository Site Selection Act. In September 2020, 90 areas with favorable geological conditions were identified as part of step 1 in phase 1 of the Site Selection Act. Representative preliminary safety analyses are to be carried out next to support decisions on the question, which siting regions should undergo surface-based exploration. These safety analyses are supported by numerical simulations building on geoscientific and technical data. The models that are taken into account are associated with various sources of uncertainties. Addressing these uncertainties and the robustness of the decisions pertaining to sites and design choices is a central component of the site selection process. In that context, important research objectives are associated with the question of how uncertainty should be treated through the various data collection, modeling and decision-making processes of the site selection procedure, and how the robustness of the repository system should be improved. BGE, therefore, established an interdisciplinary research cluster to identify open questions and to address the gaps in knowledge in six complementary research projects. In this paper, we introduce the overall purpose and the five thematic groups that constitute this research cluster. We discuss the specific questions addressed as well as the proposed methodologies in the context of the challenges of the site selection process in Germany. Finally, some conclusions are drawn on the potential benefits of a large method-centered research cluster in terms of simulation data management.

Рецензия на горно-геологическую часть обоснования строительства подземного хранилища радиоактивных отходов

The city district “Closed Administrative-territorial formation of the city of Zheleznogorsk” has appointed and organized public discussions on the materials of the justification of the license (including environmental impact assessment materials) for activities in the field of nuclear energy use “Creation of a second-class RW storage facility at FSUE GCK”. The mining and geological materials on the construction site of an underground repository of radioactive waste (RW) of the second hazard class in Zheleznogorsk of the Krasnoyarsk Territory are considered. The purpose of the construction of the storage facility is to ensure the storage of second-class radioactive waste at the site of the mining and chemical plant in volumes that meet the needs of the enterprise until the national operator is ready to handle radioactive waste. The review is a response to an offer to discuss supposedly public materials of open access. The subject of public discussions was conducted in the form of a survey. It is proposed to carry out the initial stage of the justification of the object on the basis of the Law “On Subsoil”. The following conclusion is made: the target horizon after the conservation of the object is likely to be flooded, primarily along vertical collector trunks; heterogeneous backfilling of the internal free space of trunks and horizontal workings with finished concrete lining with crushed/granular natural bentonite will not help; in reality, the volume of water in the burial zone will significantly determine the characteristics and the inexhaustible resource of the overlying water supply layers of rocks, rather than rocks of the target range, and even without recharge from other sources, the flooded PGZRO will quickly turn into a supplier of hot water and radiolytic gases. The opinion is expressed that it is unacceptable to turn a temporary storage facility into a permanent disposal site for radioactive waste.

Pore‐Scale Modeling of Water and Ion Diffusion in Partially Saturated Clays

AbstractAn accurate mechanistic understanding of solute diffusion in partially saturated clays is critical for assessing the safety of deep geological repositories for radioactive waste. In this study, a pore‐scale numerical framework is developed to simulate water and ion diffusion in partially saturated clays. First, the two‐phase Shan‐Chen Lattice Boltzmann method is employed to establish the liquid‐gas distribution in a reconstructed three‐dimensional pore geometry of a clay. An equivalent solute method is also developed and validated to improve the numerical stability of the solution at the liquid/gas interface corresponding to steep variations of the concentration and diffusion coefficient of the water tracer. By using a mobility‐distance relationship from molecular simulations, Fick's law is numerically solved to simulate water diffusion in nanopores, while the coupled Poisson‐Boltzmann‐Nernst‐Planck equations are solved to simulate ion diffusion under the influence of the electrical double layer (EDL). Our model reveals that the decrease of relative effective diffusion coefficients during the desaturation is more pronounced for ions than for water, due to the additional transport pathway of water tracers in the gas phase. The obtained effective diffusion coefficients of tritiated water and ions agree well with reported data from compacted sedimentary rocks. By comparing the local electric potential and the distribution of ion concentrations in single pores, the simulation results suggest that the EDL in unsaturated clays has a more complex influence on ion distribution than under fully water‐saturated conditions. This study provides critical insights into the coupled transport processes of solutes in partially saturated clays.

Modelling of preferential gas flow in saturated bentonite using a bimodal, strain-dependent pore model

This paper presents a novel strain-dependent water retention model for improved predictive modelling of localized gas flow in bentonite. The proposed model uses fundamental material properties such as dry density and montmorillonite content to generate improved predictions of water retention under different strain conditions. The model was validated with the use of laboratory measurements of capillary pressure in MX-80 bentonite at different dry densities. An additional phenomenological test simulated microfracture induced gas flow in FEBEX bentonite, which showed strong local desaturation due to developing microfractures and a resulting decreasing gas entry pressure. The application of the approach provided first good results that can be relevant for modelling radioactive waste repositories.

Water-rock interactions of uranium deposits: A field investigation and laboratory batch experiment

Interactions between bedrock and groundwater in the far-field of a deep geological repository (DGR) for high-level radioactive waste significantly affect the transport of uranium, which is the major radionuclide in a DGR. Therefore, the present study evaluated the geochemical behavior of uranium by assessing the hydrogeochemical characteristics of groundwater, surface water, mine water, and quarry runoff water in the Okcheon metamorphic belt, which represents a natural analogue study site in Korea. A batch experiment was also conducted to further elucidate the interactions between the uranium-containing rock and groundwater in the study area. The results of the field investigation indicated that uranium in groundwater formed aqueous complexes in the form of calcium uranyl tricarbonate. The concentrations of uranium in groundwater were low, at less than 1 μg L−1, which seems to be attributable to the dissolutions of uraninite, coffinite, UO2(am), and U4O9(c) under the moderately reduced condition and subsequent control by co-precipitation with iron (hydr)oxides. The results of the batch experiment showed that uranium concentrations may be controlled by adsorption or surface complexation with iron oxides. The field study demonstrates the equilibrium state maintained in the current geochemical conditions at the study site, while the batch experiment provides implications regarding the reaction processes over time. Overall, this study showed that uranium forms complexes with carbonate and sulfate under the geochemical conditions of the study site, and that its mobility could be restricted through co-precipitation or adsorption/surface complexation. This study is expected to contribute to a comprehensive understanding of how the behavior of uranium is affected by the evolution of geochemical conditions around the DGR.

Design-of-Experiment (DoE) based history matching for probabilistic integrity analysis—A case study of the FE-experiment at Mont Terri

We present an application of design-of-experiment (DoE) based history matching as an approach to reduce and investigate parameter uncertainties in finite-element models for repositories of high-level radioactive waste. We combine experimental data from the FE-experiment at the Mont Terri underground research laboratory in Switzerland with thermo-hydro-mechanical modeling using the open-source package OpenGeoSys. Uncertainties were reduced by an initial parameter screening to find heavy hitters and an experiment-matching procedure using Monte-Carlo sampling on a Gaussian proxy model to fit the error between modeling response and the experiment. Furthermore, we performed a global sensitivity analysis based on the proxy model, demonstrating the spatial impact of parameter sensitivities. Very good agreement between the experimental data and the model was found for the temperature response, whereas the pressure match hints at a significant remaining gap in the physical models and/or structure. This gap could not be filled within the scope of our contribution and needs further investigation.

Effect of drying cracks on swelling and self-healing of bentonite-sand blocks used as engineered barriers for radioactive waste disposal

Experiments were conducted to evaluate the healing of drying cracks in air-dried bentonite-sand blocks after hydration and swelling in groundwater, providing justifications to simplify the protection of blocks prior to installation in a high-level radioactive waste repository. Synthetic groundwater was prepared to represent the geochemistry of Beishan groundwater, and was used to hydrate the blocks during the swelling pressure and swelling strain measurements, as Beishan is the most promising site for China's repository. Healing of the surface cracks was recorded by photography, and healing of the internal cracks was visualized by CT images and hydraulic conductivity of air-dried blocks. The results indicate that the maximum swelling pressure and swelling strain are primarily affected by the geochemistry of Beishan groundwater, but not affected by the drying cracks. The maximum swelling pressure and swelling strain of air-dried blocks are comparable to or even higher than the pressure and strain of fresh blocks. The maximum swelling pressure measured in strong (i.e. high ion strength) Beishan groundwater was 44% of the pressure measured in deionized (DI) water, and the maximum swelling strain was reduced to 23% of the strain measured in DI water. Nevertheless, the remained swelling of the blocks hydrated in strong Beishan groundwater was sufficient to heal the surface and internal drying cracks, as demonstrated by the pictures of surface cracks and CT images. The hydraulic conductivity of the air-dried block permeated with strong groundwater was comparable (3.7× higher) to the hydraulic conductivity of the fresh block, indicating the self-healing of drying cracks after hydration and swelling in groundwater. A simplified method of protecting the block with plastic wraps before installation is recommended, since the remained swelling of the block hydrated in Beishan groundwater is sufficient to heal the drying cracks.

Free swelling behavior of MX80 bentonite under elevated temperatures up to 200 °C

This paper focuses on understanding trends in the swelling potential of MX80 bentonite under temperatures up to 200 °C using a high-pressure cell. The free swelling behavior of expansive clays under high temperature and high fluid pressure conditions that may be encountered in geological repositories for high-level radioactive waste is important as the swelling potential is closely linked with key transition points on the physical and chemical properties of these clays. Free swell tests performed at temperatures ranging from 22 to 200 °C under sufficient pressure to ensure that the pore water remains as a superheated liquid were performed to assess whether the swell index of bentonite follows similar non-monotonic trends with temperature as observed in the literature for the cation exchange capacity. The measured swell indices follow an increasing-decreasing trend with a transition close to 100 °C. The experimental results can be used to guide parameter selection in long-term simulations on the buffer behavior of the buffer material, which requires an understanding of temperature effects on the coupled thermal-hydraulic-mechanical properties governing these processes.

Sorption Behavior of Radionuclides on Engineered and Natural Barriers and Prediction of Sorption Distribution Coefficients Using Support Vector Regression

A low- and intermediate-level radioactive waste repository contains various types of radionuclides and organic complexing agents. Their chemical interaction within the repository can lead to the formation of radionuclide-ligand complexes, influencing the limited retention behaviors of radionuclides. This study focuses on the sorption behavior of radionuclides on both engineered (concrete) and natural barriers (sedimentary rock and granite), as well as the prediction of sorption distribution coefficients (Kd) using support vector regression. Batch studies were conducted to determine the K d values for three radionuclides (99Tc, 137Cs, and 238U) under different conditions, including pH, temperature, and the presence of organic ligands (such as ethylenediaminetetraacetic acid, nitrilotriacetic acid, and isosaccharinic acid). The K d values for 238U exhibited a sharp decrease with increasing concentrations of organic ligands. In contrast, the K d values for 99Tc showed only a slight reduction at higher organic ligand concentrations. Meanwhile, the K d values for 137Cs remained relatively unchanged, regardless of the type and initial concentration of organic ligands. This suggests a high level of retention for 137Cs in the rock samples. The support vector regression model with a radial basis kernel function proved effective in predicting the K d values under different experimental conditions. This enhancement in predicting accuracy contributes valuable insights into understanding the sorption processes involved in radionuclide behavior. Overall, this study advances our knowledge of radionuclide behavior on both engineered and natural barriers while providing a reliable prediction tool for estimating sorption distribution coefficients.

Effect of fracture characteristics on groundwater flow adjacent to high-level radioactive waste repository

In the study, a 2-D numerical model-delineating the high-level radioactive waste repository surrounded by hosting granite-rock was designed to evaluate pressure build-up, elevated temperature, and fracture flow caused by heat generation at the repository. During the early stage (0.1 years), build-up pressure at the repository induced radial groundwater flow. On the other hand, buoyancy-driven vertical flow was dominant during the late stage (2,000 years). The pressure build-up and elevated temperature varied significantly in bentonite, excavation-damaged zone and granite, resulting in different groundwater velocity. Fracture flow in both single and intersecting fractures were also influenced by the pressure and temperature, but their impact varied depending on the geometrical properties (e.g. orientation, elevation, lateral position) of the fracture. In complex discrete fracture network models, build-up pressure in the early stage mainly generated preferential fracture flow through few pathways, while in the late stage, convection-circulating flow induced by the buoyancy was distinct. In the early stage, higher density and connectivity of fracture network did not lead to an increase in average fracture flow, whereas the circulating flow in the late stage became more frequent and larger. Especially, long fractures served as both preferential flow pathways in the early stage and conduits for circulating flow in the late stage. The circulating flow was highly dependent on the spatial distribution of the long fractures, causing a significant uncertainty of average fracture flow in the late stage. The low angle of intersection between fractures resulted in low connectivity that decelerated the average fracture flow in both stages.

Modelling the thermo-mechanical behaviour of a rock joint

The CNSC, the Canadian regulator for the nuclear industry, participated in DECOVALEX-2023 Task G that focuses on the thermo (T) - hydro (H)- mechanical (M) behaviour of rock joints. Joints are omnipresent in rock masses and are planes of weakness in the host rock. When deep geological repositories (DGRs) for radioactive waste are being considered in areas where rock joints are present, the joints could be preferential pathways for radionuclide migration. Therefore, their THM behaviour must be better understood to assess the safety of the DGR. Under different possible internal and external perturbations, a joint can move by shear and dilation. If the joint crosses the emplacement area of a waste container, the heat generated from the waste can itself induce shearing of the joint. Excessive shear movement can in turn lead to failure of the container, resulting in earlier release of radionuclides. Furthermore, dilation that might accompany shear, results in an increase in the joint aperture creating a faster flow path for radionuclide transport. Mathematical models are important tools that need to be developed and employed, in order to assess joint shear and dilation under different loading conditions, such as the heat generated from the emplaced waste. The authors have developed such a mathematical model based on a macroscopic formulation within the framework of elasto-plasticity. It is verified against analytical solutions and validated against shear under constant normal load tests and thermal shearing tests of joints in granite.

Swiss deep drilling campaign 2019–2022: Geological overview and rock properties with focus on porosity and pore-space architecture

A recently completed deep drilling campaign, comprising 9 deep boreholes penetrating the Mesozoic sedimentary sequence of northern Switzerland, yielded >6 km of drillcore. One of the main objectives was to characterise the low-permeability sequence with the lower Jurassic Opalinus Clay in its centre, motivated by the site selection for a deep geological repository for radioactive waste. In this context, the chemical and isotopic composition of the porewater, as well as the mineralogical and petrophysical properties of the rocks, were among the main study targets. In this paper, the main objective was the characterisation of the lithologically diverse Jurassic rock sequence with focus on mineralogy, porosity and pore-space architecture. Given the large amount of data, a well constrained relationship between clay content (relating to fine-grained sheet-silicate minerals) and porosity could be established. Porosity increases with clay content along a concave curve, but in detail minor formation-specific differences of the positions relative to the best-fit curve were identified. These are attributed to the highly variable deposition rates that resulted in different times available for early diagenesis to alter the rock fabric by mineral dissolution and cementation, thereby affecting the compaction behaviour. Pore-size distributions were obtained from N2 ad-/desorption isotherms. A distinct peak at a radius of 3 nm can be clearly correlated with clay minerals, whereas limestones are dominated by pore sizes in the range of 40–100 nm, and marls show intermediate distributions. A conceptual framework is proposed distinguishing a nanometric porosity that is proportional to the clay content and a contribution of larger pores that are related to the geometric incompatibility between platy clay minerals and isometric calcite or quartz. The contribution of these larger pore is thought to explain the curvature of the clay content-porosity relationship and the more limited compaction of the clay in pressure shadows adjacent to the larger grains. A number of outliers towards high porosity at a given clay content were identified in oolites (most strongly in Fe-rich oolites), sandstones and a unit containing coral-reef material. All these units have in common the presence of competent calcite or quartz grains at the time of deposition, leading to grain-supported fabrics and therefore to a more limited compaction in the interstitial pore space.

Diffusion of HTO, 36Cl and 22Na in the Mesozoic rocks of northern Switzerland: I. Effective diffusion coefficients and capacity factors across the heterogeneous sediment sequences

Argillaceous rocks are currently being examined worldwide as potential host rocks for repositories for radioactive waste and spent fuel due to their favourable characteristics such as the self-sealing ability or limited diffusive transport of fluids, solutes or gases. In this study, through-diffusion experiments focused on rock samples with different mineralogical compositions taken from deep boreholes in the Mesozoic rock sequence of northern Switzerland, to determine diffusion parameters of HTO, 36Cl− and 22Na+ perpendicular to the bedding plane. Both effective diffusion coefficients and accessible porosities were calculated from the data obtained. In the Opalinus Clay, the primary selected host rock of the repository, the effective diffusion coefficients (De) and accessible porosity values (ε) of the neutral species HTO within and across all study areas are relatively consistent (De = 8.8 ± 1.9 × 10−12 m2 s−1; ε = 0.12 ± 0.02), indicating that the material can be considered homogeneous in terms of diffusion properties. Importantly, the chemical composition of the pore water has no effect on the values of the effective diffusion coefficients of HTO. On the other hand, the rocks above and below the Opalinus Clay, up to the next aquifer, consist of tight sedimentary units (carbonates, siliciclastics including argillaceous rocks) with a wider range of diffusion coefficients, indicating a higher level of heterogeneity. The diffusion coefficients of anions, such as 36Cl−, tend to be smaller due to anion exclusion effects, while those of cations, such as 22Na+, tend to be larger due to surface enhanced diffusion. The extent of these effects is largely determined by the composition of the pore water, and – in the case of cations – by the extent of sorption which depends also on the sorption capacity – indicated by the cation exchange capacity - of the solid. As a result, variations in the effective diffusion coefficient of 36Cl− and 22Na+ can be observed firstly between different rock types (i.e. composition, fabric), and secondly between the different study areas due to differences in the chemical composition of the pore waters in contact with the solid phase.Based on the analysis of around 130 samples, it has been observed that the diffusion coefficients of the Mesozoic units in northern Switzerland exhibit a significant correlation with the total clay content of the rocks. These findings pave the way for the establishment of a diffusion database for the relevant elements under consideration in the Swiss radioactive waste programme and the Safety Case.

Experimental study of water-extractable sulphate in Opalinus Clay and implications for deriving porewater concentrations

In northern Switzerland, the Opalinus Clay, a Jurassic claystone formation, is foreseen as host rock for a deep geological repository for radioactive waste. Characterizing its porewater is of particular importance for assessing the mobility of radionuclides and the stability of the engineered barriers. Although the porewater composition of the Opalinus Clay is fairly well known, there is still controversy on the sources of sulphate obtained by different porewater characterization methods. A striking observation is that sulphate concentrations from aqueous extraction and recalculated to in-situ conditions are consistently much higher than sulphate concentrations measured in borehole waters, squeezed waters and advectively displaced waters (“excess sulphate”). Accordingly, the main objective of this study is to better investigate the processes affecting dissolved sulphate concentrations during aqueous extraction and, thus, to reduce uncertainties in predicting the concentrations of this compound in the Opalinus Clay porewater. To this end, a series of extraction experiments were conducted using variable solid/liquid ratios, extraction times and extract solutions. In order to suppress sulphide-mineral oxidation, all the experiments were performed in a glovebox under oxygen-free conditions (atmosphere and solutions). Measurements of the sulphur and oxygen isotope composition of the dissolved sulphate in aqueous extracts are aimed to further constrain the source of the “excess sulphate”. Finally, the plausibility of the SO4 data from extraction experiments in terms of their representativeness for in-situ conditions was evaluated by simple geochemical modelling. The modelling shows that SO4 concentrations from aqueous extracts recalculated to in-situ conditions imply dissolved and exchangeable cation concentrations which are not consistent with measured data, thus, attesting non-conservative behaviour for sulphate during aqueous extraction. However, the various extraction experiments showed that pyrite oxidation was successfully suppressed during the experiments and neither contributions from e.g. organic material, congruent calcite dissolution and/or sulphate mineral dissolution provide enough SO4 to explain the “excess sulphate”. Ultimately, the various extraction experiments failed to definitely identify the source of the “excess sulphate” in aqueous extracts. However, the good agreement found between the δ18O and δ34S values of dissolved SO4 in aqueous extracts and those of borehole waters suggest that the “excess sulphate” might be weakly bound to mineral surfaces.

Impact of a Biological Chelator, Lanmodulin, on Minor Actinide Aqueous Speciation and Transport in the Environment.

Minor actinides are major contributors to the long-term radiotoxicity of nuclear fuels and other radioactive wastes. In this context, understanding their interactions with natural chelators and minerals is key to evaluating their transport behavior in the environment. The lanmodulin family of metalloproteins is produced by ubiquitous bacteria and Methylorubrum extorquens lanmodulin (LanM) was recently identified as one of nature's most selective chelators for trivalent f-elements. Herein, we investigated the behavior of neptunium, americium, and curium in the presence of LanM, carbonate ions, and common minerals (calcite, montmorillonite, quartz, and kaolinite). We show that LanM's aqueous complexes with Am(III) and Cm(III) remain stable in carbonate-bicarbonate solutions. Furthermore, the sorption of Am(III) to these minerals is strongly impacted by LanM, while Np(V) sorption is not. With calcite, even a submicromolar concentration of LanM leads to a significant reduction in the Am(III) distribution coefficient (Kd, from >104 to ∼102 mL/g at pH 8.5), rendering it even more mobile than Np(V). Thus, LanM-type chelators can potentially increase the mobility of trivalent actinides and lanthanide fission products under environmentally relevant conditions. Monitoring biological chelators, including metalloproteins, and their biogenerators should therefore be considered during the evaluation of radioactive waste repository sites and the risk assessment of contaminated sites.

Assessment of canister degradation for the encapsulation of spent nuclear fuel: Key research issues encountered in recent regulatory reviews and government decision making in Sweden

Abstract. Regulatory review of a licence application for construction and operation of a geological repository for radioactive waste should not only be based on information provided by the applicant but also on viewpoints brought up by stakeholders and decision makers. In the Swedish Radiation Safety Authority's (SSM) licensing review of a spent fuel repository at the Forsmark site, the main concerns brought up in court hearings, from national consultations and by the Swedish government were focused around the long-term protective capacity of the copper canisters with cast iron inserts. The most debated canister degradation mechanisms were anoxic corrosion of copper (in oxygen gas free water), localised sulphide corrosion (pitting corrosion and stress corrosion cracking), the influence of gamma radiation, and strain hardening of the canister cast iron insert. The main question addressed by SSM is not whether such effects can be ruled out altogether, but rather their potential extent and influence on canister integrity during a sufficiently long period in the repository environment. Constraints are mainly based on rock properties and associated hydrological and geochemical factors known from site investigation and knowledge about the protective capability of the buffer barrier. The key factors are in general well characterised and cover for instance sulphide availability, groundwater flow, mass transfer rates and expected mechanical loading on canisters in the repository environment. The canister corrosion/degradation mechanisms reviewed in this paper are judged by SSM to have a small or limited importance for demonstration of regulatory compliance, taking into account the characteristics of the site, the function of the buffer, and the margins provided by the significant thickness and mechanical strength of the proposed canister.

Investigating the role of Na-bentonite colloids in facilitating Sr transport in granite minerals through column experiments and modeling

Colloids play a crucial role in influencing the mobility of radionuclides in high-level radioactive waste repositories. However, the co-transport behavior of radionuclides and colloids in geological media remains insufficiently understood. This study investigated the transport of Strontium (Sr) in four types of granite minerals (quartz, biotite, K-feldspar, and plagioclase) in the presence and absence of Na-bentonite colloids (Na-BC) using column experiments. Employing a stepwise modeling strategy, this study first determined the basic flow and transport parameters through breakthrough curve analysis of the conservative tracer (Br). Then, the experimental data of Sr in the colloid-free Sr transport experiments and Na-BC in the Sr-colloid co-transport experiments were quantitatively explained using a two-site sorption model and a two kinetic sites model, respectively. Finally, the co-transport behavior of Sr and Na-BC was fitted using the colloid-facilitated solute transport model. The stepwise modeling allowed quantification of the kinetics of Sr sorption onto mobile and immobile Na-BC and highlighted the role of straining in Na-BC retention. In the absence of Na-BC, Sr transport experienced the greatest retardation in biotite, followed by plagioclase, K-feldspar, and quartz, respectively, which positively correlated with the specific surface area of the minerals. Moreover, Na-BC enhanced Sr transport with the same retardation order in all tested minerals, with recovery rate increments of 68.61%, 19.21%, 6.67%, and 4.33%, respectively. The transport of Sr in K-feldspar was found to be less affected by Na-BC compared to the other tested minerals, likely due to the strong cation exchange capacity of K+ among the cation components of minerals, making hydrated K+ more likely to exchange with Sr2+ on K-feldspar surfaces. These findings hold significant implications for assessing the risks associated with the transport of radionuclides in deep geological repositories.