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

Hongnan Jia, Na Yao, Yiming Jin, Liqing Wu, Juan Zhu and Wei Luo ()
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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

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-49834-5

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