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Published July 15, 2023 | Published + Supplemental Material
Journal Article Open

Potential-dependent transition of reaction mechanisms for oxygen evolution on layered double hydroxides

  • 1. ROR icon California Institute of Technology


Oxygen evolution reaction (OER) is of crucial importance to sustainable energy and environmental engineering, and layered double hydroxides (LDHs) are among the most active catalysts for OER in alkaline conditions, but the reaction mechanism for OER on LDHs remains controversial. Distinctive types of reaction mechanisms have been proposed for the O-O coupling in OER, yet they compose a coupled reaction network with competing kinetics dependent on applied potentials. Herein, we combine grand-canonical methods and micro-kinetic modeling to unravel that the nature of dominant mechanism for OER on LDHs transitions among distinctive types as a function of applied potential, and this arises from the interplay among applied potential and competing kinetics in the coupled reaction network. The theory-predicted overpotentials, Tafel slopes, and findings are in agreement with the observations of experiments including isotope labelling. Thus, we establish a computational methodology to identify and elucidate the potential-dependent mechanisms for electrochemical reactions.

Additional Information

© The Author(s) 2023. 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 license, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons license 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 license, visit http://creativecommons.org/licenses/by/4.0/. This work was supported by National Natural Science Foundation of China (Nos. 22122304 and 92261111), Tsinghua University Dushi Program, National Key Research and Development Project (2022YFA1503000), and Tsinghua University Initiative Scientific Research Program (20221080065) all awarded to H.X. We are grateful to the Center of High-Performance Computing at Tsinghua University and Tsinghua Xuetang Talents Program for providing computational resources. Data availability: The data generated in this study are provided in the article and the Supplementary Information files. Contributions: H.X. conceived and designed the project. Z.W. conducted all the calculations. Z.W., W.A.G., and H.X. analyzed the results. Z.W. wrote the initial manuscript. Z.W., W.A.G., and H.X. revised the manuscript and approved the final version. The authors declare no competing interests.

Attached Files

Published - s41467-023-40011-8.pdf

Supplemental Material - 41467_2023_40011_MOESM1_ESM.pdf

Supplemental Material - 41467_2023_40011_MOESM3_ESM.pdf

Supplemental Material - 41467_2023_40011_MOESM4_ESM.zip


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August 22, 2023
November 21, 2023