Search Results (13)

Because of its swelling capacity, compacted bentonite clay is a suitable buffer material in deep geological repositories for high-level nuclear waste. However, this only applies if the swelling capacity is maintained. Accordingly, bentonites have to be stable to changing temperature, humidity, infiltrating fluids or microbial activity. In batch experiments, we investigated combined microbial and thermo-hydro-geochemical effects on the swelling capacity of uncompacted bentonite MX-80. Bentonite was exposed to fluids of different ionic strength and the bacterium Stenotrophomonas bentonitica. Bacterial growth was monitored by counting colony-forming units while the swelling capacity of bentonite was evaluated using in situ XRD at varied temperatures and humidity. The presence of bentonite prolonged the survival of S. bentonitica. However, electron microscopy, XRD and ICP-OES analyses showed neither an interaction of S. bentonitica with bentonite, nor significant changes in the swelling capacity or element composition. The swelling capacity and diffraction peak intensity were, however, strongly reduced by the ionic strength of the fluid and the exposure time. The study highlights that bentonite is affected by thermo-hydro-geochemical and microbial processes to different degrees and that the complexity of different co-occurring factors in potential nuclear waste repositories is important to consider in safety assessments. Full article

This study investigates the performance of two bentonite materials, specifically MX-80 (Na-bentonite) and FEBEX (Ca-Mg-Na-bentonite), employed as engineered barriers in deep geological disposal facilities for the isolation of high-level radioactive waste, contained in metallic canisters. Experiments conducted at the laboratory scale focused on the interaction of these bentonites with FeCl₂ powder, used as a soluble iron source, to observe enhanced alteration of the bentonite. The experiments were carried out under a hydrothermal gradient. A dominant Na-Cl-SO₄ saline solution was put in contact with the compacted bentonites from the top, while a constant temperature of 100 °C was maintained at the bottom using a heater in contact with the layer of FeCl₂. The experimental cells were examined after six months of interaction. Various changes in the physical and chemical properties of the bentonites were observed. An increase in the water content, a reduction in the specific surface area and cation exchange capacity, changes in the distribution of aqueous species, and the formation of secondary minerals were observed. Reaction products formed at the bentonite interface with FeCl₂, primarily comprising akaganeite, goethite, and hematite. The smectites showed evident structural modifications, with an enrichment in iron content, and a shift in the exchangeable ion distribution in the case of MX-80 bentonite. This work provides valuable insights into the complex interactions between bentonite barriers and materials that dissolve iron, serving as proxies for deep geological disposal environments and indicating the potential long-term behavior, taking into account higher concentrations of dissolved iron than those expected in a real repository. Full article

In a deep geological disposal system, bentonite buffer material is an important barrier used to protect the disposal canister from the inflow of groundwater and prevent the outflow of radionuclides. This study aimed to characterize the mineralogical and chemical reactions of bentonite caused by copper corrosion of the canister in a radioactive waste repository. We investigated the d-spacings of montmorillonite in Gyeongju bentonite (Ca-type, KJ-I) under groundwater-saturated conditions over 10 years and compared their characteristics with those of Wyoming bentonite (Na-type, MX-80) in the Korea Atomic Energy Research Institute Underground Research Tunnel. Mineralogical investigations using X-ray diffraction and focused ion beam energy-dispersive spectroscopy indicated that no transformation of smectite or neo-formed clay phases occurred. In the Ca-type bentonite (KJ-I), the swelling was observed when it was in contact with rolled plate (RP) and cold-spray-coated (CSC) copper, with d-spacing expansions of 2.9% and 3.8%, respectively. In contrast, the Na-type bentonite (MX-80) showed d-spacing expansions of 17.6% and 19.6% when it was in contact with the RP and CSC Cu, respectively. The Cu concentration and distribution indicated that the corrosion products dissolved and then diffused into the surrounding bentonite, with maximum penetration depths of 2.0 and 0.5 mm over 10 years, respectively. Full article

The Alternative Buffer Material ABM5 experiment is an in situ medium-scale experiment performed at Äspö Hard Rock Laboratory (HRL) conducted by SKB in Sweden with the aim of analysing the long-term stability of bentonites used as an engineering barrier for a high-level radioactive waste repository (HLWR). In this work, four different ring-shaped Ca- and Na-bentonite blocks, which were piled around a carbon steel cylindrical heater, subjected to a maximum temperature of 250 °C and hydrated with saline Na-Ca-Cl Äspö groundwater (0.91 ionic strength), were characterized after dismantling. This work allowed us to identify the main geochemical processes involved, as well as the modifications in the physico-chemical properties and pore water composition after 4.4 years of treatment. No significant modifications in mineralogy were observed in samples close to the heater contact, except an increase in Fe content due to C-steel corrosion, carbonate dissolution/precipitation (mainly calcite and siderite) and Mg increase. No magnetite and a low amount of Fe(II) inside the clay mineral structure were detected. No modifications were observed in the smectite structure, except a slight increase in total and tetrahedral charge. A decrease in external surface area and cation exchange capacity (CEC) was found in all samples, with lower values being detected at the heater contact. As a consequence of the diffusion of the infiltrating groundwater, a modification of the composition at clay mineral exchange sites occurred. Ca-bentonites increased their Na content at exchange sites, whereas Na-bentonite increased their Ca content. Exchangeable Mg content decreased in all bentonites, except in MX-80 located at the bottom part of the package. A salinity gradient is observed through the bentonite blocks from the granite to the heater contact due to anions are controlled by diffusion and anion exclusion. The pore water chemistry of bentonites evolved as a function of the diffusion transport of the groundwater, the chemical equilibrium of cations at exchange sites and mineral dissolution/precipitation processes. These reactions are in turn dependent on temperature and water vapor fluxes. Full article

Radioactive waste disposal, as the final step of the open nuclear fuel cycle, is an important process to protect humans and the environment from harmful effects of ionising radiation. Approaching the construction of the geological repository, the understanding and predictability of the behavior of engineered barrier material becomes more important than ever. Therefore, a number of research studies are being focused on the experimental and numerical analysis of the engineered barrier material state and behavior under repository conditions. Engineered barrier material will be in contact with the host rock and waste packages, and its properties and behavior will be governed by complex and coupled thermo-hydro-mechanical processes. This paper presents the modeling activities of the Lithuanian Energy Institute, performed in the framework of the H2020 project BEACON (Bentonite Mechanical Evolution). The numerical model, developed in COMSOL Multiphysics (Burlington, MA 01803, USA), was applied for the modeling of experiments, performed by Ecole Polytechnique Federale de Lausanne (EPFL, Switzerland), on granular MX-80 bentonite in the odeometer cell. The hydromechanical behavior of a compacted bentonite sample was analyzed under different conditions: hydration with groundwater under confined volume conditions and hydration under free swelling conditions and subsequent mechanical loading. Model outcomes (swelling pressure, saturation, dry density, and void ratio) were compared to the available experimental data. The modeling results were in line with the analyzed experimental data. Full article

Compacted bentonite is envisaged as engineering buffer/backfill material in geological disposal for high-level radioactive waste. In particular, Na-bentonite is characterised by lower hydraulic conductivity and higher swelling competence and cation exchange capacity, compared with other clays. A solid understanding of the hydraulic behaviour of compacted bentonite remains challenging because of the microstructure expansion of the pore system over the confined wetting path. This work proposed a novel theoretical method of pore system evolution of compacted bentonite based on its stacked microstructure, including the dynamic transfer from micro to macro porosity. Furthermore, the Kozeny–Carman equation was revised to evaluate the saturated hydraulic conductivity of compacted bentonite, taking into account microstructure effects on key hydraulic parameters such as porosity, specific surface area and tortuosity. The results show that the prediction of the revised Kozeny–Carman model falls within the acceptable range of experimental saturated hydraulic conductivity. A new constitutive relationship of relative hydraulic conductivity was also developed by considering both the pore network evolution and suction. The proposed constitutive relationship well reveals that unsaturated hydraulic conductivity undergoes a decrease controlled by microstructure evolution before an increase dominated by dropping gradient of suction during the wetting path, leading to a U-shaped relationship. The predictive outcomes of the new constitutive relationship show an excellent match with laboratory observation of unsaturated hydraulic conductivity for GMZ and MX80 bentonite over the entire wetting path, while the traditional approach overestimates the hydraulic conductivity without consideration of the microstructure effect. Full article

The geological disposal in deep bedrock repositories is the preferred option for the management of high-level radioactive waste (HLW). In some of these concepts, carbon steel is considered as a potential canister material and bentonites are planned as backfill material to protect metallic waste containers. Therefore, a 1D radial reactive transport model has been developed in order to better understand the processes occurring during the long-term iron-bentonite interaction. The numerical model accounts for diffusion, aqueous complexation reactions, mineral dissolution/precipitation and cation exchange at a constant temperature of 25$°\mathrm{C}$ under anoxic conditions. Our results suggest that Fe is sorbed at the montmorillonite surface via cation exchange in the short-term, and it is consumed by formation of the secondary phases in the long-term. The numerical model predicts precipitation of nontronite, magnetite and greenalite as corrosion products. Calcite precipitates due to cation exchange in the short-term and due to montmorillonite dissolution in the long-term. Results further reveal a significant increase in pH in the long-term, while dissolution/precipitation reactions result in limited variations of the porosity. A sensitivity analysis has also been performed to test the effect of selected parameters, such as corrosion rate, diffusion coefficient and composition of the bentonite porewater, on the corrosion processes. Overall, outcomes suggest that the predicted main corrosion products in the long-term are Fe-silicate minerals, such phases thus should deserve further attention as a chemical barrier in the diffusion of radionuclides to the repository far field. Full article

Various numerical methods have been being extensively used to estimate the diffusion parameters of pertechnetate (⁹⁹TcO_4⁻) in compacted MX80 bentonite clay using through-diffusion (TD) techniques. In this study, an improved TD column test was applied, and the diffusion fluxes of tritium (HTO) as a non-reactive radionuclide, and ⁹⁹TcO_4⁻ with various dry densities, were compared under the same experimental conditions. Similar results were obtained for the apparent diffusion coefficients of HTO and ⁹⁹TcO_4⁻ using three estimation methods: a graphical method applying the asymptote calculation, an analytical solution using Lsqcurvefit installed in MATLAB, and the Marquardt–Levenberg optimization algorithm in the HYDRUS-1D inverse method. The statistical analysis showed that the densities using a one-way analysis of variance (ANOVA) for the three estimation methods ranged from 1200 to 2000 kg/m³, which indicated that there were no obvious differences between HTO and ⁹⁹TcO_4⁻. In general, the diffusion parameters of ⁹⁹TcO_4⁻ were lower than those for HTO due to anion exclusion effects and lower accessible porosity. Full article

The cement–clay interaction (CI) experiment was carried out at the Mont Terri rock laboratory to complement the current knowledge on the influence that cementitious materials have on Opalinus Clay (OPA) and bentonite (MX). Drill cores including the interface of OPA, concrete (LAC = low-alkali binder, and OPC = ordinary Portland cement), and MX, which interacted for 4.9 and 10 years, were successfully retrieved after drilling, and detailed analyses were performed to evaluate potential mineralogical changes. The saturated compacted bentonites in core samples were divided into ten slices, profiling bentonite in the direction towards the interface, to evaluate the extent and spatial variation of the mineralogical alteration of bentonite. Regarding the mineral compositions of bentonite, cristobalite was dissolved within a range of 10 mm from the interface in both LAC-MX and OPC-MX, while calcite precipitated near the interface for OPC-MX. In LAC-MX and OPC-MX, secondary products containing Mg (e.g., M-S-H) also precipitated within 20 mm of the interface. These alterations of bentonite developed during the first 4.9 years, with very limited progress observed for the subsequent 5 years. Detectable changes in the mineralogical nature of montmorillonite (i.e., the formation of illite or beidellite, increase in layer charge) did not occur during the 10 years of interaction. Full article

The removal of potentially harmful radioactive waste from the anthroposphere will require disposal in geological repositories, the designs of which often favour the inclusion of a clay backfill or engineered barrier around the waste. Bentonite is often proposed as this engineered barrier and understanding its long-term performance and behaviour is vital in establishing the safety case for its usage. There are many different compositions of bentonite that exist and much research has focussed on the properties and behaviour of both sodium (Na) and calcium (Ca) bentonites. This study focusses on the results of a swelling test on Bulgarian Ca bentonite that showed an unusual gel formation at the expanding front, unobserved in previous tests of this type using the sodium bentonite MX80. The Bulgarian Ca bentonite was able to swell to completely fill an internal void space over the duration of the test, with a thin gel layer present on one end of the sample. The properties of the gel, along with the rest of the bulk sample, have been investigated using ESEM, EXDA and XRD analyses and the formation mechanism has been attributed to the migration of nanoparticulate smectite through a more silica-rich matrix of the bentonite substrate. The migration of smectite clay out of the bulk of the sample has important implications for bentonite erosion where this engineered barrier interacts with flowing groundwater in repository host rocks. Full article

Engineered barrier system (EBS) has been proposed for the disposal of high-level waste (HLW). An EBS is composed of a disposal canister with spent fuel, a buffer material, backfill material, and a near field rock mass. The buffer material is especially essential to guarantee the safe disposal of HLW, and plays the very important role of protecting the waste and canister against any external mechanical impact. The buffer material should also possess high thermal conductivity, to release as much decay heat as possible from the spent fuel. Its thermal conductivity is a crucial property since it determines the temperature retained from the decay heat of the spent fuel. Many studies have investigated the thermal conductivity of bentonite buffer materials and many types of soils. However, there has been little research or overall evaluation of the thermal conductivity of Korean Ca-type bentonite buffer materials. This paper investigated and analyzed the thermal conductivity of Korean Ca-type bentonite buffer materials produced in Gyeongju, and compared the results with various characteristics of Na-type bentonites, such as MX80 and Kunigel. Additionally, this paper suggests various predictive models to predict the thermal conductivity of Korean bentonite buffer materials considering various influential independent variables, and compared these with results for MX80 and Kunigel. Full article

The study investigated the basic geomechanical and mineralogical evolution of the bentonite barrier under various experimental boundary conditions which replicated the near-field Thermo-Hydro-Chemico (THC) conditions in a repository. The relationships between the physicochemical alterations and changes in the geotechnical properties have seldom been studied, especially on a consistent dataset. This paper attempts to link the physicochemical properties of Na-bentonite (MX-80) to the macro-scale engineering functionality of the bentonite post THC exposure. Experiments investigated the impact of THC variables on the engineering and physicochemical functionality of the bentonite with respect to its application within a High-Level Waste (HLW) engineered barrier system. Intrinsic alterations to the MX-80 bentonite under relatively short-term exposure to hydrothermal and chemical conditions were measured. Additionally, two long-term tests were conducted under ambient conditions to consider the impact of exposure duration. The intrinsic measurements were then related to the overall performance of the bentonite as a candidate barrier material for application in a UK geological disposal facility. Findings indicate that exposure to thermo-saline-corrosion conditions (i.e., corrosion products derived from structural grade 275 carbon steel) inhibits the free swell capacity and plasticity of the bentonite. However, the measured values remained above the design limits set out for the Swedish multi-barrier concept, from which the UK concept may take a lead. Corrosion alone does not appear to significantly affect the geotechnical measurements compared with the influence of thermal loading and high saline pore water after relatively short-term exposure. Thermal and corrosion exposure displayed no impact on the intrinsic swelling of the smectite component, indicating that no significant structural alteration had occurred. However, when exploring more complex saline solutions i.e., mixed Na, K and Ca, rather than the reference NaCl, divalent cation replacement was observed within the interlayer exchange site. This was accelerated in higher thermal loading conditions. Full article

The final disposal of high-level nuclear waste in many countries is preferred to be in deep geological repositories. Compacted bentonites are proposed for use as the buffer surrounding the waste canisters which may be subjected to both thermal and hydraulic loadings. A significant increase in the temperature is anticipated within the buffer, particularly during the early phase of the repository lifetime. In this study, several non-isothermal and non-isothermal hydraulic tests were carried on compacted MX80 bentonite. Compacted bentonite specimens (water content = 15.2%, dry density = 1.65 Mg/m³) were subjected to a temperature of either 85 or 150 °C at one end, whereas the temperature at the opposite end was maintained at 25 °C. During the non-isothermal hydraulic tests, water was supplied from the opposite end of the heat source. The temperature and relative humidity were monitored along predetermined depths of the specimens. The profiles of water content, dry density, and degree of saturation were established after termination of the tests. The test results showed that thermal gradients caused redistribution of the water content, whereas thermo-hydraulic gradients caused both redistribution and an increase in the water content within compacted bentonites, both leading to development of axial stress of various magnitudes. The applied water injection pressures (5 and 600 kPa) and temperature gradients appeared to have very minimal impact on the magnitude of axial stress developed. The thickness of thermal insulation layer surrounding the testing devices was found to influence the temperature and relative humidity profiles thereby impacting the redistribution of water content within compacted bentonites. Under the influence of both the applied thermal and thermo-hydraulic gradients, the dry density of the bentonite specimens increased near the heat source, whereas it decreased at the opposite end. The test results emphasized the influence of elevated temperatures (up to 150 °C) on the thermo-hydro-mechanical response of compacted bentonites in the nuclear waste repository settings. Full article