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- Title
Stabilizing atomic Ru species in conjugated sp<sup>2</sup> carbon-linked covalent organic framework for acidic water oxidation.
- Authors
Jia, Hongnan; Yao, Na; Jin, Yiming; Wu, Liqing; Zhu, Juan; Luo, Wei
- 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. Developing efficient and stable Ru-based catalysts for acidic water oxidation is highly desirable for proton exchange membrane electrolyzers. Here the authors report atomically anchoring Ru species on an acidic-stable π-conjugated covalent organic framework with robust sp2-carbon-linkage for stable and efficient water oxidation.
- Subjects
OXIDATION of water; ACTIVATION energy; ENERGY levels (Quantum mechanics); X-ray powder diffraction; DIFFRACTION patterns; OXIDATION; OXYGEN reduction
- Publication
Nature Communications, 2024, Vol 15, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-024-49834-5