Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias
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...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-02-01
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| Series: | Communications Chemistry |
| Online Access: | https://doi.org/10.1038/s42004-025-01446-w |
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| author | Federico Raffone Rémi Khatib Marialore Sulpizi Clotilde Cucinotta |
| author_facet | Federico Raffone Rémi Khatib Marialore Sulpizi Clotilde Cucinotta |
| author_sort | Federico Raffone |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-b6099b008d244f8dad1d2cd4e9d5f218 |
| institution | DOAJ |
| issn | 2399-3669 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Communications Chemistry |
| spelling | doaj-art-b6099b008d244f8dad1d2cd4e9d5f2182025-08-20T03:03:57ZengNature PortfolioCommunications Chemistry2399-36692025-02-018111210.1038/s42004-025-01446-wRevealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under biasFederico Raffone0Rémi Khatib1Marialore Sulpizi2Clotilde Cucinotta3Department of Chemistry and Thomas Young Centre, Imperial College LondonDepartment of Physics, Johannes Gutenberg UniversityDepartment of Physics, Ruhr-University BochumDepartment of Chemistry and Thomas Young Centre, Imperial College LondonAbstract 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.https://doi.org/10.1038/s42004-025-01446-w |
| spellingShingle | Federico Raffone Rémi Khatib Marialore Sulpizi Clotilde Cucinotta Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias Communications Chemistry |
| title | Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias |
| title_full | Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias |
| title_fullStr | Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias |
| title_full_unstemmed | Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias |
| title_short | Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias |
| title_sort | revealing the molecular interplay of coverage wettability and capacitive response at the pt 111 water solution interface under bias |
| url | https://doi.org/10.1038/s42004-025-01446-w |
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