Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias
File(s)
Published version
Author(s)
Raffone, Federico
Khatib, Remi
Sulpizi, Marialore
Cucinotta, Clotilde
Type
Journal Article
Abstract
While electrified interfaces are crucial for electrocatalysis and corrosion, their molecular morphology remains largely unknown. Through highly realistic ab initio molecular dynamics simulations of the Pt(111)-water solution interface in reducing conditions, we reveal a deep interconnection among electrode coverage, wettability, capacitive response, and catalytic activity. We identify computationally the experimentally hypothesised states for adsorbed hydrogen on Pt, HUPD and HOPD, revealing their role in governing interfacial water reorientation and hydrogen evolution. The transition between these two H states with increasing potential, induces a shift from a hydrophobic to a hydrophilic interface and correlates with a change in the primary electrode screening mechanism. This results in a slope change in differential capacitance, marking the onset of the experimentally observed peak around the potential of zero charge. Our work produces crucial insights for advancing electrocatalytic energy conversion, developing deep understanding of electrified interfaces.
Date Issued
2025-02-24
Date Acceptance
2025-02-04
Citation
Communications Chemistry, 2025, 8 (2)
ISSN
2399-3669
Publisher
Nature Portfolio
Journal / Book Title
Communications Chemistry
Volume
8
Issue
2
Copyright Statement
© The Author(s) 2025. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
License URL
Identifier
10.1038/s42004-025-01446-w
Publication Status
Published
Article Number
ARTN 58