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Developing innovative and efficient non-precious-metal-group (non-PMG) electrocatalysts is crucial for the wide use of zinc-air batteries (ZABs). Herein, a single-atom catalyst (termed as Fe-N-C/rGO SAC) with unique five N-coordinated Fe (Fe-N5) centers is prepared by pyrolyzing the composite of zeolitic-imidazolate-frameworks-8 (ZIF-8) and graphene oxide (GO). Specifically, the individual Fe site is stabilized by four equatorial and one axial N atoms donated by the N-doped carbon matrix and imidazole ring, respectively, thus forming an asymmetric electron depletion zone over the metal center, which can effectively promote the generation of reactive intermediates and accelerate the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) processes for ZABs. The rechargeable liquid ZAB with Fe-N-C/rGO catalyst exhibits an extremely high energy density (928.25 Wh·kg−1), a remarkable peak power density (107.12 mW·cm−2), and a long cycle life (400 h). Additionally, the corresponding flexible solid-state ZAB displays superior foldability and remarkable cycling stability. This work provides both experimental and theoretical guidance for rational design of non-PMG electrocatalyst-driven ZABs.


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Single-atom Fe-N5 catalyst for high-performance zinc-air batteries

Show Author's information Le LiYin-Juan ChenHao-Ran XingNa LiJia-Wei XiaXing-Yue QianHui XuWei-Zuo LiFeng-Xiang YinGuang-Yu He( )Hai-Qun Chen( )
Key Laboratory of Advanced Catalytic Materials and Technology, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, China

Abstract

Developing innovative and efficient non-precious-metal-group (non-PMG) electrocatalysts is crucial for the wide use of zinc-air batteries (ZABs). Herein, a single-atom catalyst (termed as Fe-N-C/rGO SAC) with unique five N-coordinated Fe (Fe-N5) centers is prepared by pyrolyzing the composite of zeolitic-imidazolate-frameworks-8 (ZIF-8) and graphene oxide (GO). Specifically, the individual Fe site is stabilized by four equatorial and one axial N atoms donated by the N-doped carbon matrix and imidazole ring, respectively, thus forming an asymmetric electron depletion zone over the metal center, which can effectively promote the generation of reactive intermediates and accelerate the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) processes for ZABs. The rechargeable liquid ZAB with Fe-N-C/rGO catalyst exhibits an extremely high energy density (928.25 Wh·kg−1), a remarkable peak power density (107.12 mW·cm−2), and a long cycle life (400 h). Additionally, the corresponding flexible solid-state ZAB displays superior foldability and remarkable cycling stability. This work provides both experimental and theoretical guidance for rational design of non-PMG electrocatalyst-driven ZABs.

Keywords: zinc-air battery, N-doped hierarchical porous carbon/rGO composite, single-atom electrocatalyst, five N-coordinated Fe (Fe-N5) single-atom sites , density functional theory (DFT) study

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Acknowledgements

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Received: 23 February 2022
Revised: 09 April 2022
Accepted: 12 April 2022
Published: 03 June 2022
Issue date: September 2022

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22078028, 22078027, and 21978026). The authors would like to thank the shiyanjia lab (www.shiyanjia.com) for materials characterizations and Changzhou University Computer Center for computing service.

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