Article Dans Une Revue Nature Chemistry Année : 2024

Unconventional structural evolution of an oxide surface in water unveiled by in situ sum-frequency spectroscopy

Résumé

Oxide–water interfaces host a wide range of important reactions in nature and modern industrial applications; however, accurate knowledge about these interfaces is still lacking at the molecular level owing to difficulties in accessing buried oxide surfaces. Here we report an experimental scheme enabling in situ sum-frequency vibrational spectroscopy of oxide surfaces in liquid water. Application to the silica–water interface revealed the emergence of unexpected surface reaction pathways with water. With ab initio molecular dynamics and metadynamics simulations, we uncovered a surface reconstruction, triggered by deprotonation of surface hydroxylated groups, that led to unconventional five-coordinated silicon species. The results help demystify the multimodal chemistry of aqueous silica discovered decades ago, bringing in fresh information that modifies the current understanding. Our study will provide new opportunities for future in-depth physical and chemical characterizations of other oxide–water interfaces.

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Dates et versions

hal-04829586 , version 1 (10-12-2024)

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Xiaoqun Li, Flavio Brigiano, Simone Pezzotti, Xinyi Liu, Wanlin Chen, et al.. Unconventional structural evolution of an oxide surface in water unveiled by in situ sum-frequency spectroscopy. Nature Chemistry, 2024, ⟨10.1038/s41557-024-01658-y⟩. ⟨hal-04829586⟩
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