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Voltage- and time-dependent valence state transition in cobalt oxide catalysts during the oxygen evolution reaction

Author

Listed:
  • Jing Zhou

    (Chinese Academy of Sciences)

  • Linjuan Zhang

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Yu-Cheng Huang

    (Tamkang University)

  • Chung-Li Dong

    (Tamkang University)

  • Hong-Ji Lin

    (National Synchrotron Radiation Research Center)

  • Chien-Te Chen

    (National Synchrotron Radiation Research Center)

  • L. H. Tjeng

    (Max Planck Institute for Chemical Physics of Solids)

  • Zhiwei Hu

    (Max Planck Institute for Chemical Physics of Solids)

Abstract

The ability to determine the electronic structure of catalysts during electrochemical reactions is highly important for identification of the active sites and the reaction mechanism. Here we successfully applied soft X-ray spectroscopy to follow in operando the valence and spin state of the Co ions in Li2Co2O4 under oxygen evolution reaction (OER) conditions. We have observed that a substantial fraction of the Co ions undergo a voltage-dependent and time-dependent valence state transition from Co3+ to Co4+ accompanied by spontaneous delithiation, whereas the edge-shared Co–O network and spin state of the Co ions remain unchanged. Density functional theory calculations indicate that the highly oxidized Co4+ site, rather than the Co3+ site or the oxygen vacancy site, is mainly responsible for the high OER activity.

Suggested Citation

  • Jing Zhou & Linjuan Zhang & Yu-Cheng Huang & Chung-Li Dong & Hong-Ji Lin & Chien-Te Chen & L. H. Tjeng & Zhiwei Hu, 2020. "Voltage- and time-dependent valence state transition in cobalt oxide catalysts during the oxygen evolution reaction," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-15925-2
    DOI: 10.1038/s41467-020-15925-2
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    Cited by:

    1. Chun-Kuo Peng & Yu-Chang Lin & Chao‐Lung Chiang & Zhengxin Qian & Yu-Cheng Huang & Chung-Li Dong & Jian‐Feng Li & Chien-Te Chen & Zhiwei Hu & San-Yuan Chen & Yan-Gu Lin, 2023. "Zhang-Rice singlets state formed by two-step oxidation for triggering water oxidation under operando conditions," Nature Communications, Nature, vol. 14(1), pages 1-9, December.

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