Evidence for auto-catalytic mineral dissolution from surface-specific vibrational spectroscopy

The dissolution of minerals in water is typically studied on macroscopic length- and time-scales, by detecting dissolution products in bulk solution and deducing reaction rates from model assumptions. Here, we report a direct, real-time measurement of silica dissolution, by monitoring how dissolution changes the first few interfacial layers of water in contact with silica, using surface-specific spectroscopy. We obtain direct information on the dissolution kinetics of this geochemically relevant mineral. The interfacial concentration of dissolution products saturates at the level of the solubility limit of silica (similar to millimolar) on the surprisingly short timescale of tens of hours. The observed kinetics reveal that the dissolution rate increases substantially with progressing dissolution, suggesting that dissolution is an autocatalytic process.