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Stabilizing atomic Ru species in conjugated sp2 carbon-linked covalent organic framework for acidic water oxidation

Author

Listed:
  • Hongnan Jia

    (Wuhan University)

  • Na Yao

    (Wuhan Textile University)

  • Yiming Jin

    (Wuhan University)

  • Liqing Wu

    (Wuhan University)

  • Juan Zhu

    (Wuhan University)

  • Wei Luo

    (Wuhan University)

Abstract

Suppressing the kinetically favorable lattice oxygen oxidation mechanism pathway and triggering the adsorbate evolution mechanism pathway at the expense of activity are the state-of-the-art strategies for Ru-based electrocatalysts toward acidic water oxidation. Herein, atomically dispersed Ru species are anchored into an acidic stable vinyl-linked 2D covalent organic framework with unique crossed π-conjugation, termed as COF-205-Ru. The crossed π-conjugated structure of COF-205-Ru not only suppresses the dissolution of Ru through strong Ru-N motifs, but also reduces the oxidation state of Ru by multiple π-conjugations, thereby activating the oxygen coordinated to Ru and stabilizing the oxygen vacancies during oxygen evolution process. Experimental results including X-ray absorption spectroscopy, in situ Raman spectroscopy, in situ powder X-ray diffraction patterns, and theoretical calculations unveil the activated oxygen with elevated energy level of O 2p band, decreased oxygen vacancy formation energy, promoted electrochemical stability, and significantly reduced energy barrier of potential determining step for acidic water oxidation. Consequently, the obtained COF-205-Ru displays a high mass activity with 2659.3 A g−1, which is 32-fold higher than the commercial RuO2, and retains long-term durability of over 280 h. This work provides a strategy to simultaneously promote the stability and activity of Ru-based catalysts for acidic water oxidation.

Suggested Citation

  • Hongnan Jia & Na Yao & Yiming Jin & Liqing Wu & Juan Zhu & Wei Luo, 2024. "Stabilizing atomic Ru species in conjugated sp2 carbon-linked covalent organic framework for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49834-5
    DOI: 10.1038/s41467-024-49834-5
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