Operando identification of the oxide path mechanism with different dual-active sites for acidic water oxidation
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 RuO<sub>2</sub> 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 Mn<sup>4-δ</sup>-O-Ru<sup>4+δ</sup> active sites by introducing Mn atoms into RuO<sub>2</sub> 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 Mn<sup>4-δ</sup>-O-Ru<sup>4+δ</sup> 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.
Authors
- Hengjie Liu (ORCID: https://orcid.org/0000-0001-6499-3935)
- Hao Tan (ORCID: https://orcid.org/0000-0001-9221-4871)
- Qianqian Ji (ORCID: https://orcid.org/0000-0001-5801-2600)
- Bing Tang
- Chang Jiang (ORCID: https://orcid.org/0000-0003-0334-1567)
- Wensheng Yan (ORCID: https://orcid.org/0000-0001-6297-4589)
- Jianrong Zeng (ORCID: https://orcid.org/0000-0003-4867-1893)
- Xingke Cai (ORCID: https://orcid.org/0000-0003-3878-4456)
- Chao Wang (ORCID: https://orcid.org/0000-0002-3378-6594)
- Xilin Zhang (ORCID: https://orcid.org/0000-0002-7141-5700)
- Ruiqi Liu (ORCID: https://orcid.org/0009-0003-9113-7327)
- Jie Zhao (ORCID: https://orcid.org/0000-0002-0451-0919)
- Mei Sun
Institutions
- University of Science and Technology of China (CN)
- Shenzhen University (CN)
- Xiamen University (CN)
- Chinese Academy of Sciences (CN)
- Hefei National Center for Physical Sciences at Nanoscale (CN)
- Shanghai Advanced Research Institute (CN)
- Institute for Advanced Study (DE)
- Shenzhen Institutes of Advanced Technology (CN)
- National Synchrotron Radiation Laboratory (CN)
- Henan Normal University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-09-16
- DOI
- https://doi.org/10.1038/s41467-024-52471-7
- Citations
- 119
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 12.18
Funders
- Salt Science Research Foundation
- National Natural Science Foundation of China
- University of Science and Technology of China
- National Synchrotron Radiation Laboratory
- National Key Research and Development Program of China
- Beijing Synchrotron Radiation Facility