Arguably the most fundamental chemical reaction involving mineral surfaces in Earth-surface environments is their interaction with aqueous solutions (Stumm et al., 1987; Brown, 2001). Even in air, metal-(oxyhydr)oxide surfaces are likely to have multiple monolayers (ML) of sorbed water. For example, α-Al2O3 surfaces have been shown by thermo-gravimetric analysis to have the equivalent of one monolayer of water at a relative humidity (RH) of ∼35% and the equivalent of more than 20 ML at 95% RH (Yan et al., 1987). In the case of high surface area silica, Miyata (1968)...

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