Ab initio molecular dynamics investigation of the Pt(111)-water interface structure in an alkaline environment with high surface OH-coverages

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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

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en

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11

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Physical Chemistry Chemical Physics, Volume 26, issue 26, pp. 18233-18243

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In this study, we investigate the structure of the Pt(111)-water interface in an alkaline environment with large OH coverages of 1/3, 2/3 and 1 monolayer using a large well-equilibrated system. We observe that the OH coverage influences both the orientational distribution of the water molecules and their density, with more structure associated with higher coverage. At the same time, there is evidence of a highly dynamic hydrogen bond network on the lower coverage systems with substantial exchange of water between the surface and the solvent. In addition to OH and H2O species, which are preferentially located at the top sites, the 1/3 and 2/3 monolayer surfaces also contain O atoms, which are relatively stable and prefer the hollow sites. In contrast, the 1 monolayer surface shows none of these dynamics, and is unlikely to be active. The dynamic coexistence of O, OH and H2O on Pt(111) electrodes in alkaline conditions necessitates the investigation of several possible reaction paths for processess like ORR and water splitting. Finally, the exchange processes observed between the solvent and the interface underscore the need to explicitly include liquid water in simulations of systems similar to Pt(111).

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Publisher Copyright: © 2024 The Royal Society of Chemistry.

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Partanen, L & Laasonen, K 2024, 'Ab initio molecular dynamics investigation of the Pt(111)-water interface structure in an alkaline environment with high surface OH-coverages', Physical Chemistry Chemical Physics, vol. 26, no. 26, pp. 18233-18243. https://doi.org/10.1039/d4cp01100g