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Developing innovative, easy-to-manufacture, and non-Pt-group-metal (non-PGM) electrocatalysts is essential for the highly efficient oxygen reduction reaction (ORR). Herein, we report a self-sacrificing post-synthetic strategy to synthesize highly loaded Fe-isolated single atoms anchored on the hierarchical porous N,S co-doped carbon matrix (Fe-SAs/S,N-C/rGO). The optimized Fe-SAs/S,N-C/rGO exhibits excellent ORR activity in the pH-universal range with half-wave potentials of 0.89, 0.80, and 0.60 V in alkaline, acidic, and neutral media, comparable to the commercial Pt/C (0.85, 0.81, and 0.64 V, respectively). The homemade liquid Zn-air battery (ZAB) with Fe-SAs/S,N-C/rGO as the cathode catalyst displays an open-circuit voltage (OCV) of ~ 1.61 V, discharging specific capacity of 817.23 mAh·g−1, and long-term durability of ~ 1865 cycles, outperforming those of the device with commercial Pt/C+RuO2 (1.49 V, 657.32 mAh·g−1, and ~ 120 cycles, respectively). Intriguingly, the corresponding flexible solid-state ZAB delivers satisfactory OCV, peak power density, foldability, and cycling stability at room temperature, as well as adaptability at a low temperature of −10 °C. Besides, density functional theory (DFT) calculation reveals that the atomic FeN3S moieties in Fe-SAs/S,N-C/rGO can cause charge redistribution and lower the binding strength of oxygen-containing intermediates, resulting in accelerated ORR kinetics and optimized catalytic activity. This work provides insights into experimental and theoretical guidance towards non-PGM electrocatalysts for efficient energy conversion.

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Publication history
Copyright
Acknowledgements

Publication history

Received: 23 January 2023
Revised: 23 February 2023
Accepted: 27 February 2023
Published: 30 March 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22078028 and 21978026), the National Science Foundation for Young Scientists of China (No. 22209016), and the International Scientific and Technological Cooperation Program of Changzhou (No. CZ20220028). The authors would like to thank the Analysis and Testing Center, NERC Biomass of Changzhou University, the Shiyanjia Lab (www.shiyanjia.com), and the SCI-GO (www.sci-go.com) for materials characterizations as well as the Changzhou University Computer Center for computing services.

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