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Bateman, K.*; 村山 翔太*; 花町 優次*; Wilson, J.*; 瀬田 孝将*; 天野 由記; 久保田 満*; 大内 祐司*; 舘 幸男
Minerals (Internet), 12(7), p.883_1 - 883_20, 2022/07
被引用回数:1 パーセンタイル:0.02(Geochemistry & Geophysics)The construction of a repository for geological disposal of radioactive waste will include the use of cement-based materials. Following closure, groundwater will saturate the repository and the extensive use of cement will result in the development of a highly alkaline porewater, pH 12.5; this fluid will migrate into and react with the host rock. The chemistry of the fluid will evolve over time, initially high [Na] and [K], evolving to a Ca-rich fluid, and finally returning to the groundwater composition. This evolving chemistry will affect the long-term performance of the repository, altering the physical and chemical properties, including radionuclide behaviour. Understanding these changes forms the basis for predicting the long-term evolution of the repository. This study focused on the determination of the nature and extent of the chemical reaction, as well as the formation and persistence of secondary mineral phases within a granite, comparing data from sequential flow experiments with the results of reactive transport modelling. The reaction of the granite with the cement leachates resulted in small changes in pH and the precipitation of calcium aluminum silicate hydrate (C-(A-)S-H) phases of varying compositions, of greatest abundance with the Ca-rich fluid. As the system evolved, secondary C-(A-)S-H phases re-dissolved, partly replaced by zeolites. This general sequence was successfully simulated using reactive transport modelling.
Bateman, K.; 村山 翔太*; 花町 優次*; Wilson, J.*; 瀬田 孝将*; 天野 由記; 久保田 満*; 大内 祐司*; 舘 幸男
Minerals (Internet), 11(9), p.1026_1 - 1026_23, 2021/09
被引用回数:2 パーセンタイル:22.02(Geochemistry & Geophysics)The construction of a repository for geological disposal of radioactive waste will include the use of cement-based materials. Following closure, groundwater will saturate the repository and the extensive use of cement will result in the development of a highly alkaline porewater, pH 12.5. This fluid will migrate into and react with the host rock. The chemistry of the fluid will evolve over time, initially high [Na] and [K], evolving to a Ca-rich fluid and finally returning to the groundwater composition. This evolving chemistry will affect the long-term performance of the repository altering the physical and chemical properties, including radionuclide behaviour. Understanding these changes forms the basis for predicting the long-term evolution of the repository. This study focused on the determination of the nature and extent of the chemical reaction; the formation and persistence of secondary mineral phases within an argillaceous mudstone, comparing both data from sequential flow experiments with the results of reactive transport modeling. The reaction of the mudstone with the cement leachates resulted in small changes in pH but the precipitation of calcium aluminium silicate hydrate (C-A-S-H) phases of varying compositions. With the change to the groundwater secondary C-(A-)S-H phases re-dissolved being replaced by secondary carbonates. This general sequence was successfully simulated by the reactive transport model simulations.
Bateman, K.; 天野 由記; 舘 幸男
no journal, ,
The use of cement for geological disposal repository will result in the development of a highly alkaline porewater, pH 12.5 in the case of Ordinary Portland cement (OPC). The fluid will migrate into and react with the host rock. The chemistry of the migrating fluid will evolve over time, initially being high in Na and K, evolving to a Ca rich fluid and finally returning to the groundwater composition. This evolving fluid chemistry will affect the long-term performance of the repository altering the physical and chemical properties of the host rock. This study focused on the alteration due to OPC-type leachates on mudstone from the Horonobe URL, Hokkaido, Japan, by coupling the sequential flow tests and the reactive transport modelling. The reaction of the mudstone with the successive OPC leachates demonstrated its chemical buffering capacity, leading to a reduction in pH, the dissolution of primary minerals with Ca and Si concentrations being controlled by C-S-H phase precipitation. However, when the fluid returns to the natural background groundwater composition the C-S-H phases re-dissolve, which would potentially release any sorbed radionuclides. The experimental data was used to validate a reactive transport model generating increased confidence in its predictive capabilities.