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Recently, Cu-based single-atom catalysts (SACs) have garnered increasing attention as substitutes for platinum-based catalysts in the oxygen reduction reaction (ORR). Therefore, a facile, economical, and efficient synthetic methodology for the preparation of a high-performance Cu-based SAC electrocatalyst for the ORR is extremely desired, but is also significantly challenging. In this study, we propose a ball-milling method to synthesize isolated metal SACs embedded in S,N-codoped nanocarbon (M-NSDC, M = Cu, Fe, Co, Ni, Mn, Pt, and Pd). In particular, the Cu-NSDC SACs exhibit high electrochemical activity for the ORR with half-wave potential (E1/2) of 0.84 V (vs. reversible hydrogen electrode (RHE), 20 mV higher than Pt/C) in alkaline electrolyte, excellent stability, and electrocatalytic selectivity. Density functional theory (DFT) calculations demonstrated that the desorption of OH* intermediates was the rate-determining step over Cu-NSDC. This study creates a pathway for high-performance ORR single atomic electrocatalysts for fuel cell applications and provides opportunities to convert biowaste materials into commercial opportunities.

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Publication history

Received: 10 January 2022
Revised: 26 February 2022
Accepted: 03 March 2022
Published: 26 April 2022
Issue date: July 2022

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Key Research and Development Program Nanotechnology Specific Project (No. 2020YFA0210900), the National Natural Science Foundation of China (Nos. 21908255, 22078371, 22108315, 21938001, and 21961160741), the Guangdong Provincial Key R&D Programme (No. 2019B110206002), the Science and Technology Key Project of Guangdong Province (No. 2020B010188002), the Guangdong Basic and Applied Basic Research Foundation (No. 2020A1515110864), and the Guangdong Natural Science Foundation (No. 2021A1515010163).

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Email: nanores@tup.tsinghua.edu.cn

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