Electrocatalytic water oxidation with manganese phosphates
Shujiao Yang,
Kaihang Yue,
Xiaohan Liu,
Sisi Li,
Haoquan Zheng,
Ya Yan (),
Rui Cao and
Wei Zhang ()
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Shujiao Yang: Shaanxi Normal University
Kaihang Yue: Chinese Academy of Sciences (SICCAS)
Xiaohan Liu: Shaanxi Normal University
Sisi Li: Shaanxi Normal University
Haoquan Zheng: Shaanxi Normal University
Ya Yan: Chinese Academy of Sciences (SICCAS)
Rui Cao: Shaanxi Normal University
Wei Zhang: Shaanxi Normal University
Nature Communications, 2024, vol. 15, issue 1, 1-13
Abstract:
Abstract As inspired by the Mn4CaO5 oxygen evolution center in nature, Mn-based electrocatalysts have received overwhelming attention for water oxidation. However, the understanding of the detailed reaction mechanism has been a long-standing problem. Herein, homologous KMnPO4 and KMnPO4•H2O with 4-coordinated and 6-coordinated Mn centers, respectively, are prepared. The two catalysts constitute an ideal platform to study the structure-performance correlation. The presence of Mn(III), Mn(IV), and Mn(V) intermediate species are identified during water oxidation. The Mn(V)=O species is demonstrated to be the substance for O−O bond formation. In KMnPO4•H2O, the Mn coordination structure did not change significantly during water oxidation. In KMnPO4, the Mn coordination structure changed from 4-coordinated [MnO4] to 5-coordinated [MnO5] motif, which displays a triangular biconical configuration. The structure flexibility of [MnO5] is thermodynamically favored in retaining Mn(III)−OH and generating Mn(V)=O. The Mn(V)=O species is at equilibrium with Mn(IV)=O, the concentration of which determines the intrinsic activity of water oxidation. This study provides a clear picture of water oxidation mechanism on Mn-based systems.
Date: 2024
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DOI: 10.1038/s41467-024-45705-1
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