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Exchange coupling states of cobalt complexes to control proton-coupled electron transfer

Author

Listed:
  • Jueun Lee

    (Gwangju Institute of Science and Technology
    Gwangju Institute of Science and Technology)

  • Junseong Lee

    (Chonnam National University)

  • Junhyeok Seo

    (Gwangju Institute of Science and Technology
    Gwangju Institute of Science and Technology)

Abstract

The electrochemical proton reactivity of transition metal complexes receives significant attentions. A thorough understanding of proton-coupled electron transfer (PCET) pathways is essential for elucidating the mechanism behind a proton reduction reaction, and controlling the pathway is a key focus in the field of the catalyst development. Spin interactions within complexes, which arise during electron transfer, can affect significantly the PCET pathway. Herein, we explore the phenomenon of spin rearrangement during the electrochemical reorganization of high-spin cobalt complexes. Our findings reveal that opposing spin interactions, induced by different coordination environments, can alter the PCET pathway. Finally, detailed analysis of the PCET pathway allows us to propose mechanisms for proton reduction in high-spin cobalt complexes.

Suggested Citation

  • Jueun Lee & Junseong Lee & Junhyeok Seo, 2024. "Exchange coupling states of cobalt complexes to control proton-coupled electron transfer," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53099-3
    DOI: 10.1038/s41467-024-53099-3
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    References listed on IDEAS

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    1. Cameron W. Kellett & Wesley B. Swords & Michael D. Turlington & Gerald J. Meyer & Curtis P. Berlinguette, 2018. "Resolving orbital pathways for intermolecular electron transfer," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
    2. Sagnik Chakrabarti & Soumalya Sinha & Giang N. Tran & Hanah Na & Liviu M. Mirica, 2023. "Characterization of paramagnetic states in an organometallic nickel hydrogen evolution electrocatalyst," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Peng Zhou & Ishtiaque Ahmed Navid & Yongjin Ma & Yixin Xiao & Ping Wang & Zhengwei Ye & Baowen Zhou & Kai Sun & Zetian Mi, 2023. "Solar-to-hydrogen efficiency of more than 9% in photocatalytic water splitting," Nature, Nature, vol. 613(7942), pages 66-70, January.
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