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It is challenging for precise governing of electronic configuration of the individually-atomic catalysts toward optimal electrocatalysis, as d-band configuration of a metal center determines the adsorption behavior of reactive species to the center in oxygen reduction reaction (ORR). The addition of Cu atom modifies the d-band center position of Fe central atom, thus strengthening the d–π* orbital interactions. Herein, FeCu-NC catalyst in the nitrogen-doped carbon (NC) support containing individual dual-metal CuN4/FeN4 sites was prepared by the surface confinement strategy of zeolitic imidazolate framework (ZIF), treated as a model catalyst. Experimentally and theoretically co-verified dual-metal CuN4/FeN4 sites highly dispersed in the NC support, enable transferring more electrons from FeN4 sites to *OH intermediates, thereby accelerating the desorption process of *OH species. Superior to those commercial Pt/C, Our FeCu-NC catalyst exhibited extraordinary ORR activity (with a E1/2 as high as 0.87 V) and cycling stability in 0.1 M KOH electrolyte, and thereof demonstrated excellent discharge performance in zinc-air batteries. Our construction of dual-atom catalysts (DACs) provides a strategy for atom-by-atom designing high-efficiency catalysts via orbital regulation.

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Publication history
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Acknowledgements

Publication history

Received: 16 August 2022
Revised: 20 September 2022
Accepted: 22 September 2022
Published: 05 November 2022
Issue date: April 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This research was supported by the National Natural Science Foundation of China (Nos. 51872115 and 52272209) and 2020 International Cooperation Project of the Department of Science and Technology of Jilin Province (No. 20200801001GH).

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