The release of anionic nuclides such as 129I from underground nuclear waste disposals is of great environmental concern due to its long half-life and high mobility in alkaline environments. The leachability of iodide is largely dependent on the sorption capacity of various Ca-bearing minerals such as ettringite, hydrocalumite, and calcium silicate hydrate (C-S-H) which are common hydration products of cement materials. Moreover, the pore water chemistry of cement materials is dominated by Si, Al, and Ca during the initial stage of weathering, and the ratios of the ions present vary much depending on the source materials. Examining the mineral phases generated in Si–Al–Ca systems with respect to different ratios of Si, Al, and Ca and their interaction with iodide is important to better understand the sorption behavior of iodide in nuclear waste disposal facilities. In this study, the mineral synthesis in Si–Al–Ca systems was conducted under alkaline conditions at ambient temperature, and the sorption behavior of iodide with the mineral phases was investigated during and after the mineral formation. The results showed that portlandite, C-S-H, stratlingite (CASH), hydrocalumite, gibbsite, and amorphous compounds were precipitated from the systems, depending on the Si, Al, and Ca ratios. The Kd values of iodide were greatly affected by the Ca content and relatively high Ca-containing phases such as hydrocalumite, C-S-H, CASH, and portlandite showed high iodide retention capacity. Hence, ensuring the formation of these secondary minerals by modification of the chemical composition of cement materials could assist in safety design of nuclear waste disposals.
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