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Electrocatalytic water oxidation with manganese phosphates

Author

Listed:
  • 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)

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.

Suggested Citation

  • Shujiao Yang & Kaihang Yue & Xiaohan Liu & Sisi Li & Haoquan Zheng & Ya Yan & Rui Cao & Wei Zhang, 2024. "Electrocatalytic water oxidation with manganese phosphates," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45705-1
    DOI: 10.1038/s41467-024-45705-1
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