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Developing cost-effective and high-efficiency oxygen reduction reaction (ORR) catalysts is imperative for promoting the substantial progress of fuel cells and metal-air batteries. The coordination and geometric engineering of single-atom catalysts (SACs) occurred the promising approach to overcome the thermodynamics and kinetics problems in high-efficiency electrocatalysis. Herein, we rationally constructed atomically dispersed Co atoms on porous N-enriched graphene material C2N (CoSA-C2N) for efficient oxygen reduction reaction (ORR). Systematic characterizations demonstrated the active sites for CoSA-C2N is as identified as coordinatively unsaturated Co-N2 moiety, which exhibits ORR intrinsic activity. Structurally, the porous N-enriched graphene framework in C2N could effectively increase the accessibility to the active sites and promote mass transfer rate, contributing to improved ORR kinetics. Consequently, CoSA-C2N exhibited superior ORR performance in both acidic and alkaline conditions as well as impressive long-term durability. The coordination and geometric engineering of SACs will provide a novel approach to advanced catalysts for energy related applications.

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Publication history
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Acknowledgements

Publication history

Received: 09 September 2022
Revised: 12 October 2022
Accepted: 15 October 2022
Published: 23 November 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. 22201262 and 51902013) and Natural Science Foundation of Henan Province (No. 222300420290). The authors also gratefully thank the Natural Science Foundation of Department of Science and Technology of Guizhou province (No. [2019]1297), and Engineering Research Center of Guihzou province (No. [2018]487).

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