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Hydration and Dehydration of Montmorillonite With Saline Fluids Under P-T-X Conditions Relevant to the Deep Geological Repository Environment
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Bentonite, primarily composed of montmorillonite, plays a crucial role as one of the engineering barrier materials in a deep geological repository (DGR). The advantageous properties of montmorillonite, such as its swelling capacity, low permeability, and low thermal conductivity, make it a key component as a buffer material for isolating high-level radioactive waste from the surrounding natural environment. It has been known that the stability of montmorillonite is influenced by a wide range of pressure-temperature-composition (P-T-X) conditions relevant to the DGR environment. When considering potential geological events, of notable concerns are its interactions with groundwater or seawater at elevated temperatures, leading to safety hazards within the system. In this study, therefore, we investigated the hydration and dehydration reactions of Ca-montmorillonite with saline fluids such as NaCl and KCl solutions at elevated pressures and temperatures by conducting in-situ X-ray diffraction experiments using both a capillary sample heating cell and a resistive-heated diamond anvil cell. As a result, we observed different hydration states of montmorillonite depending on the chemical composition of fluids, i.e., tri-hydrated layers in NaCl and bi-hydrated layers in KCl solutions, respectively. Furthermore, we identified that montmorillonite undergoes distinct stepwise dehydration with increasing temperature, and the dehydration temperature of montmorillonite significantly increases with increasing water pressure. Consequently, this study would provide insights into the stability of hydrated montmorillonite in a seawater-dominated fluid environment and its implications for the long-term safety of the disposal system.
