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Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction

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Abstract

Exploring the atomic interaction mechanisms of dense single-atom catalysts (SACs) is of great significance for their application in oxygen reduction reaction (ORR). However, the intrinsic mechanism of the site-distance effect on the catalytic performance has been largely ignored. Here, we demonstrate the site-distance effect of Fe-Rhx@NC catalysts in ORR theoretically and experimentally. Bader charge analysis reveals that the strong interaction between Fe and Rh atoms at a certain atomic distance (dFe-Rh) alters the catalytic electronic structure, facilitating the optimization of catalyst adsorption strength. Motivated by the theoretical calculations, we designed and synthesized the Fe-Rhx@NC catalysts through a spatial confinement strategy. The characterization results prove that the Fe-Rh2@NC has the optimal dFe-Rh, which improves its intrinsic ORR activity, providing a half wave potential of 0.91 V, higher than that of the commercial Pt/C (0.86 V). This study emphasizes the importance of determining the basic mechanism of the site-distance effect in dissimilar metal atoms catalysts, which is conducive to the design of efficient catalyst systems for practical applications.

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Acknowledgements

This work was supported by the National Key R&D Program of China (2021YFA1600800 and 2020YFA0710203), the National Natural Science Foundation of China (12025505, 22002147, 22179125 and 12205304), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0450200), the University of China Innovation Program of Anhui Province (GXXT-2020-053), the Youth Innovation Promotion Association CAS (2015366 and 2022458), and the Fellowship of China Postdoctoral Science Foundation (2021TQ0319). We would thank NSRL, BSRF, and SSRF for the synchrotron beam time. We would thank XFNANO. We would thank the supercomputing system in the Supercomputing Center of University of Science and Technology of China for the calculations. We are grateful for the technical support from Experimental Center of Engineering and Materials Science, USTC.

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  1. These authors contributed equally to this work

Authors and Affiliations

  1. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China

    Tong Liu, Yudan Chen, Airong Xu, Xiaokang Liu, Dong Liu, Sicheng Li, Hui Huang, Li Xu, Shuaiwei Jiang, Tao Ding & Tao Yao

  2. Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China

    Tao Ding & Tao Yao

  3. Institutes of Physical Science and Information Technology, Anhui University, Hefei, 230601, China

    Qiquan Luo

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  1. Tong Liu
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  2. Yudan Chen
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Correspondence to Tao Ding or Tao Yao.

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Supporting information The supporting information is available online at chem.scichina.com and link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Liu, T., Chen, Y., Xu, A. et al. Regulating atomic Fe-Rh site distance for efficient oxygen reduction reaction. Sci. China Chem. 67, 1352–1359 (2024). https://doi.org/10.1007/s11426-023-1889-6

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  • DOI: https://doi.org/10.1007/s11426-023-1889-6

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