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Dual-metal catalysts with synergistic effect exhibit enormous potential for sustainable electrocatalytic applications and mechanism research. Compared with mono-metal-site catalysts, dual-metal-site catalysts exhibit higher efficiency for the oxygen evolution reaction (OER) due to reduced energy barrier of the process involving proton-coupled multi-electron transfer. Herein, we construct dual-metal Fe-Co sites coordinated with nitrogen in graphene (FeCo-NG), which exhibits high OER performance with onset overpotential of only 126 mV and Tafel slope of 120 mV·dec−1, showing that the rate-determining step is controlled by the single-electron transfer step. Theoretical calculations reveal that the FeN4 site exhibits lower OER overpotential than the CoN4 site due to appropriate adsorption energy of OOH* on the former, while the O* adsorbed on the adjacent Co site could stabilize the OOH* on the FeN4 site through hydrogen bond interaction.


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Synergy between isolated Fe and Co sites accelerates oxygen evolution

Show Author's information Tianmi Tang1,§Zhiyao Duan2,§( )Didar Baimanov3,4,§Xue Bai1Xinyu Liu5Liming Wang3Zhenlu Wang1( )Jingqi Guan1( )
Institute of Physical Chemistry, College of Chemistry, Jilin University, 2519 Jiefang Road, Changchun 130021, China
State Key Laboratory of Solidification Processing, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi’an 710072, China
CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety & CAS-HKU Joint Laboratory of Metallomics on Health and Environment, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
University of Chinese Academy of Sciences, Beijing 100049, China
School of Physical Science and Technology, ShanghaiTech University, No.393 Middle Huaxia Road, Pudong New District, Shanghai 201210, China

§ Tianmi Tang, Zhiyao Duan, and Didar Baimanov contributed equally to this work.

Abstract

Dual-metal catalysts with synergistic effect exhibit enormous potential for sustainable electrocatalytic applications and mechanism research. Compared with mono-metal-site catalysts, dual-metal-site catalysts exhibit higher efficiency for the oxygen evolution reaction (OER) due to reduced energy barrier of the process involving proton-coupled multi-electron transfer. Herein, we construct dual-metal Fe-Co sites coordinated with nitrogen in graphene (FeCo-NG), which exhibits high OER performance with onset overpotential of only 126 mV and Tafel slope of 120 mV·dec−1, showing that the rate-determining step is controlled by the single-electron transfer step. Theoretical calculations reveal that the FeN4 site exhibits lower OER overpotential than the CoN4 site due to appropriate adsorption energy of OOH* on the former, while the O* adsorbed on the adjacent Co site could stabilize the OOH* on the FeN4 site through hydrogen bond interaction.

Keywords: theoretical calculation, oxygen evolution reaction, Fe-N-C, Co-N-C, dual-atom catalysis

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Publication history
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Acknowledgements

Publication history

Received: 01 July 2022
Revised: 30 August 2022
Accepted: 01 September 2022
Published: 22 October 2022
Issue date: February 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22075099 and 31971322), the Education Department of Jilin Province (Nos. JJKH20220967KJ and JJKH20220968CY), the Natural Science Foundation of Jilin Province (No. 20220101051JC), the Natural Science Foundation of Shaanxi Province (No. D5110220052), the Fundamental Research Funds for the Central Universities (No. D5000210743), and Beijing Municipal Health Commission (No. 2021-1G-1191).

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