Molecular-scale insights into the electrical double layer at oxide-electrolyte interfaces

Chunyi Zhang, Marcos F. Calegari Andrade, Zachary K. Goldsmith, Abhinav S. Raman, Yifan Li, Pablo M. Piaggi, Xifan Wu, Roberto Car () and Annabella Selloni ()
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Chunyi Zhang: Princeton University
Marcos F. Calegari Andrade: Lawrence Livermore National Laboratory
Zachary K. Goldsmith: Princeton University
Abhinav S. Raman: Princeton University
Yifan Li: Princeton University
Pablo M. Piaggi: Princeton University
Xifan Wu: Temple University
Roberto Car: Princeton University
Annabella Selloni: Princeton University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-54631-1

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