Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 46, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202207017
Keywords
Adsorption; Flow; Mineral-Water Interface; Non-Linear Spectroscopy; Vibrational Spectroscopy
Categories
Funding
- Max Planck Graduate Center
- Johannes Gutenberg University Mainz (MPGC)
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The dissolution of minerals in water is important in geochemistry, but studying the interfacial chemistry at the molecular level is challenging. By using surface-specific vibrational sum frequency generation spectroscopy, this study investigates the chemical reaction at the fluorite-water interface and resolves the controversy regarding the role of fluoride and calcium ions in surface charge.
The dissolution of minerals in contact with water plays a crucial role in geochemistry. However, obtaining molecular insight into interfacial chemistry is challenging. Dissolution typically involves the release of ions from the surface, giving rise to a charged mineral surface. This charge affects the interfacial water arrangement, which can be investigated by surface-specific vibrational Sum Frequency Generation (v-SFG) spectroscopy. For the fluorite-water interface, recent spectroscopic studies concluded that fluoride adsorption/desorption determines the surface charge, which contrasts zeta potential measurements assigning this role to the calcium ion. By combining v-SFG spectroscopy and flow experiments with systematically suppressed dissolution, we uncover the interplay of dominant fluoride and weak calcium adsorption/desorption, resolving the controversy in the literature. We infer the calcium contribution to be orders of magnitude smaller, emphasizing the sensitivity of our approach.
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