Unraveling oxygen vacancy site mechanism of Rh-doped RuO2 catalyst for long-lasting acidic water oxidation

Yi Wang, Rong Yang, Yajun Ding, Bo Zhang, Hao Li, Bing Bai, Mingrun Li, Yi Cui, Jianping Xiao () and Zhong-Shuai Wu ()
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Yi Wang: Chinese Academy of Sciences
Rong Yang: Chinese Academy of Sciences
Yajun Ding: Chinese Academy of Sciences
Bo Zhang: Dalian Institute of Chemical Physics Chinese Academy of Sciences
Hao Li: Chinese Academy of Sciences
Bing Bai: Chinese Academy of Sciences
Mingrun Li: Chinese Academy of Sciences
Yi Cui: Chinese Academy of Sciences
Jianping Xiao: Chinese Academy of Sciences
Zhong-Shuai Wu: Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Exploring durable electrocatalysts with high activity for oxygen evolution reaction (OER) in acidic media is of paramount importance for H2 production via polymer electrolyte membrane electrolyzers, yet it remains urgently challenging. Herein, we report a synergistic strategy of Rh doping and surface oxygen vacancies to precisely regulate unconventional OER reaction path via the Ru–O–Rh active sites of Rh-RuO2, simultaneously boosting intrinsic activity and stability. The stabilized low-valent catalyst exhibits a remarkable performance, with an overpotential of 161 mV at 10 mA cm−2 and activity retention of 99.2% exceeding 700 h at 50 mA cm−2. Quasi in situ/operando characterizations demonstrate the recurrence of reversible oxygen species under working potentials for enhanced activity and durability. It is theoretically revealed that Rh-RuO2 passes through a more optimal reaction path of lattice oxygen mediated mechanism-oxygen vacancy site mechanism induced by the synergistic interaction of defects and Ru–O–Rh active sites with the rate-determining step of *O formation, breaking the barrier limitation (*OOH) of the traditional adsorption evolution mechanism.

Date: 2023
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DOI: 10.1038/s41467-023-37008-8

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