Operando identification of the oxide path mechanism with different dual-active sites for acidic water oxidation

Qianqian Ji, Bing Tang, Xilin Zhang, Chao Wang, Hao Tan, Jie Zhao, Ruiqi Liu, Mei Sun, Hengjie Liu, Chang Jiang, Jianrong Zeng, Xingke Cai () and Wensheng Yan ()
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Qianqian Ji: Shenzhen University
Bing Tang: University of Science and Technology of China
Xilin Zhang: Henan Normal University
Chao Wang: University of Science and Technology of China
Hao Tan: University of Science and Technology of China
Jie Zhao: Shenzhen University
Ruiqi Liu: University of Science and Technology of China
Mei Sun: University of Science and Technology of China
Hengjie Liu: University of Science and Technology of China
Chang Jiang: Xiamen University
Jianrong Zeng: Chinese Academy of Sciences
Xingke Cai: Shenzhen University
Wensheng Yan: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract The microscopic reaction pathway plays a crucial role in determining the electrochemical performance. However, artificially manipulating the reaction pathway still faces considerable challenges. In this study, we focus on the classical acidic water oxidation based on RuO2 catalysts, which currently face the issues of low activity and poor stability. As a proof-of-concept, we propose a strategy to create local structural symmetry but oxidation-state asymmetric Mn4-δ-O-Ru4+δ active sites by introducing Mn atoms into RuO2 host, thereby switching the reaction pathway from traditional adsorbate evolution mechanism to oxide path mechanism. Through advanced operando synchrotron spectroscopies and density functional theory calculations, we demonstrate the synergistic effect of dual-active metal sites in asymmetric Mn4-δ-O-Ru4+δ microstructure in optimizing the adsorption energy and rate-determining step barrier via an oxide path mechanism. This study highlights the importance of engineering reaction pathways and provides an alternative strategy for promoting acidic water oxidation.

Date: 2024
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DOI: 10.1038/s41467-024-52471-7

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