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An effective electrocatalyst being highly active in all pH range for oxygen reduction reaction (ORR) is crucial for energy conversion and storage devices. However, most of the high-efficiency ORR catalysis was reported in alkaline conditions. Herein, we demonstrated the preparation of atomically dispersed Fe-Zn pairs anchored on porous N-doped carbon frameworks (Fe-Zn-SA/NC), which works efficiently as ORR catalyst in the whole pH range. It achieves high half-wave potentials of 0.78, 0.85 and 0.72 V in 0.1 M HClO4, 0.1 M KOH and 0.1 M phosphate buffer saline (PBS) solutions, respectively, as well as respectable stability. The performances are even comparable to Pt/C. Furthermore, when assembled into a Zn-air battery, the high power density of 167.2 mW·cm-2 and 120 h durability reveal the feasibility of Fe-Zn-SA/NC in real energy-related devices. Theoretical calculations demonstrate that the superior catalytic activity of Fe-Zn-SA/NC can be contributed to the lower energy barriers of ORR at the Fe-Zn-N6 centers. This work demonstrates the potential of Fe-Zn pairs as alternatives to the Pt catalysts for efficient catalytic ORR and provides new insights of dual-atom catalysts for other energy conversion related catalytic reactions.


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Atomic Fe-Zn dual-metal sites for high-efficiency pH-universal oxygen reduction catalysis

Show Author's information Jie Xu1,§Shuhua Lai1,§Defeng Qi1Min Hu1Xianyun Peng1Yifan Liu2( )Wei Liu1Guangzhi Hu3Heng Xu1Fan Li1Chao Li1Jia He1( )Longchao Zhuo4Jiaqiang Sun5Yuan Qiu1Shusheng Zhang6Jun Luo1Xijun Liu1( )
Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials & Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China
Institute for Ecological Research and Pollution Control of Plateau Lakes, School of Ecology and Environmental Science, Yunnan University, Kunming 650504, China
School of Materials Science and Engineering, Xi'an University of Technology, Xi'an 710048, China
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
College of Chemistry, Zhengzhou University, Zhengzhou 450000, China

Abstract

An effective electrocatalyst being highly active in all pH range for oxygen reduction reaction (ORR) is crucial for energy conversion and storage devices. However, most of the high-efficiency ORR catalysis was reported in alkaline conditions. Herein, we demonstrated the preparation of atomically dispersed Fe-Zn pairs anchored on porous N-doped carbon frameworks (Fe-Zn-SA/NC), which works efficiently as ORR catalyst in the whole pH range. It achieves high half-wave potentials of 0.78, 0.85 and 0.72 V in 0.1 M HClO4, 0.1 M KOH and 0.1 M phosphate buffer saline (PBS) solutions, respectively, as well as respectable stability. The performances are even comparable to Pt/C. Furthermore, when assembled into a Zn-air battery, the high power density of 167.2 mW·cm-2 and 120 h durability reveal the feasibility of Fe-Zn-SA/NC in real energy-related devices. Theoretical calculations demonstrate that the superior catalytic activity of Fe-Zn-SA/NC can be contributed to the lower energy barriers of ORR at the Fe-Zn-N6 centers. This work demonstrates the potential of Fe-Zn pairs as alternatives to the Pt catalysts for efficient catalytic ORR and provides new insights of dual-atom catalysts for other energy conversion related catalytic reactions.

Keywords: oxygen reduction reaction, electrocatalysis, Fe-Zn atomic pairs, pH-universal, Zn-air battery

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Publication history
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Acknowledgements

Publication history

Received: 21 August 2020
Revised: 12 October 2020
Accepted: 17 October 2020
Published: 09 November 2020
Issue date: May 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature

Acknowledgements

This work was financially supported by the National Key R&D Program of China (No. 2017YFA0700104), the National Natural Science Foundation of China (Nos. 22075211, 21601136, 51971157, 51761165012, and 62005173), Project funded by China Postdoctoral Science Foundation (No. 2020TQ0201), Tianjin Science Fund for Distinguished Young Scholars (No. 19JCJQJC61800). The authors also acknowledge National Supercomputing Center in Shenzhen for providing the computational resources and materials studio (version 7.0, DMol3).

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