Molecular-scale insights into the electrical double layer at oxide-electrolyte interfaces
Abstract The electrical double layer (EDL) at metal oxide-electrolyte interfaces critically affects fundamental processes in water splitting, batteries, and corrosion. However, limitations in the microscopic-level understanding of the EDL have been a major bottleneck in controlling these interfacial...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-54631-1 |
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| author | Chunyi Zhang Marcos F. Calegari Andrade Zachary K. Goldsmith Abhinav S. Raman Yifan Li Pablo M. Piaggi Xifan Wu Roberto Car Annabella Selloni |
| author_facet | Chunyi Zhang Marcos F. Calegari Andrade Zachary K. Goldsmith Abhinav S. Raman Yifan Li Pablo M. Piaggi Xifan Wu Roberto Car Annabella Selloni |
| author_sort | Chunyi Zhang |
| collection | DOAJ |
| description | Abstract The electrical double layer (EDL) at metal oxide-electrolyte interfaces critically affects fundamental processes in water splitting, batteries, and corrosion. However, limitations in the microscopic-level understanding of the EDL have been a major bottleneck in controlling these interfacial processes. Herein, we use ab initio-based machine learning potential simulations incorporating long-range electrostatics to unravel the molecular-scale picture of the EDL at the prototypical anatase TiO2-electrolyte interface under various pH conditions. Our large-scale simulations, capable of capturing interfacial water dissociation/recombination reactions and electrolytic proton transport, provide unprecedented insights into the detailed structure of the EDL. Moreover, the larger capacitance of the EDL under basic relative to acidic conditions, originating from the higher affinity of the cations for the oxide surface, is found to give rise to distinct charging mechanisms on negative and positive surfaces. Our results are validated by the agreement between the computed EDL capacitance and experimental data. |
| format | Article |
| id | doaj-art-bf3583097d4e4bf98ace5c11b2a820c8 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-bf3583097d4e4bf98ace5c11b2a820c82024-12-01T12:34:27ZengNature PortfolioNature Communications2041-17232024-11-011511910.1038/s41467-024-54631-1Molecular-scale insights into the electrical double layer at oxide-electrolyte interfacesChunyi Zhang0Marcos F. Calegari Andrade1Zachary K. Goldsmith2Abhinav S. Raman3Yifan Li4Pablo M. Piaggi5Xifan Wu6Roberto Car7Annabella Selloni8Department of Chemistry, Princeton UniversityMaterials Science Division, Lawrence Livermore National LaboratoryDepartment of Chemistry, Princeton UniversityDepartment of Chemistry, Princeton UniversityDepartment of Chemistry, Princeton UniversityDepartment of Chemistry, Princeton UniversityDepartment of Physics, Temple UniversityDepartment of Chemistry, Princeton UniversityDepartment of Chemistry, Princeton UniversityAbstract The electrical double layer (EDL) at metal oxide-electrolyte interfaces critically affects fundamental processes in water splitting, batteries, and corrosion. However, limitations in the microscopic-level understanding of the EDL have been a major bottleneck in controlling these interfacial processes. Herein, we use ab initio-based machine learning potential simulations incorporating long-range electrostatics to unravel the molecular-scale picture of the EDL at the prototypical anatase TiO2-electrolyte interface under various pH conditions. Our large-scale simulations, capable of capturing interfacial water dissociation/recombination reactions and electrolytic proton transport, provide unprecedented insights into the detailed structure of the EDL. Moreover, the larger capacitance of the EDL under basic relative to acidic conditions, originating from the higher affinity of the cations for the oxide surface, is found to give rise to distinct charging mechanisms on negative and positive surfaces. Our results are validated by the agreement between the computed EDL capacitance and experimental data.https://doi.org/10.1038/s41467-024-54631-1 |
| spellingShingle | Chunyi Zhang Marcos F. Calegari Andrade Zachary K. Goldsmith Abhinav S. Raman Yifan Li Pablo M. Piaggi Xifan Wu Roberto Car Annabella Selloni Molecular-scale insights into the electrical double layer at oxide-electrolyte interfaces Nature Communications |
| title | Molecular-scale insights into the electrical double layer at oxide-electrolyte interfaces |
| title_full | Molecular-scale insights into the electrical double layer at oxide-electrolyte interfaces |
| title_fullStr | Molecular-scale insights into the electrical double layer at oxide-electrolyte interfaces |
| title_full_unstemmed | Molecular-scale insights into the electrical double layer at oxide-electrolyte interfaces |
| title_short | Molecular-scale insights into the electrical double layer at oxide-electrolyte interfaces |
| title_sort | molecular scale insights into the electrical double layer at oxide electrolyte interfaces |
| url | https://doi.org/10.1038/s41467-024-54631-1 |
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