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Nano Research 2021, 14(4): 998-1003 https://doi.org/10.1007/s12274-020-3141-x
Research Article | Issue | Published: 23 October 2020

Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery

Show Author's Information Wenjie Wu1,§,  Yan Liu2,§,  Dong Liu3,  Wenxing Chen4,  Zhaoyi Song1,  Ximin Wang1,  Yamin Zheng2,  Ning Lu2,  Chunxia Wang1( ),  Junjie Mao2( ),  Yadong Li5
State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, China University of Petroleum, Beijing 102249, China
Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Province Key Laboratory of Optoelectric Materials Science and Technology and Anhui Laboratory of Molecule-Based Materials, Anhui Normal University, Wuhu 241002, China
State key Lab of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemistry, Tsinghua University, Beijing 100084, China

§ Wenjie Wu and Yan Liu contributed equally to this work.

Keywords:
oxygen reduction reaction, non-noble metal, single atomic sites catalysts, nitrogen-doped carbon materials, carbon defect
Topics:
CarbonCopperDoping (additives)ElectrocatalystsElectrolytic reduction OxygenOxygen reduction reaction Porous materialsPrecious metalsZinc
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Wu W, Liu Y, Liu D, et al. Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery. Nano Research, 2021, 14(4): 998-1003. https://doi.org/10.1007/s12274-020-3141-x
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Abstract Full text Electronic supplementary material About this article

The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction (ORR) is intensively increasing. Herein, single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst (Cu1/NC) was prepared by coordination pyrolysis strategy. Remarkably, the Cu1/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V (vs. RHE) in alkaline media, outperforming those of commercial Pt/C (0.851 V) and Cu nanoparticles anchored on N-doped porous carbon (CuNPs/NC-900), but also demonstrates high stability and methanol tolerance. Moreover, the Cu1/NC-900 based Zn-air battery exhibits higher power density, rechargeability and cyclic stability than the one based on Pt/C. Both experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu1/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect, resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR process. This study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.


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About this article

Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery

Show Author's information Wenjie Wu1,§, Yan Liu2,§, Dong Liu3, Wenxing Chen4, Zhaoyi Song1, Ximin Wang1, Yamin Zheng2, Ning Lu2, Chunxia Wang1( ), Junjie Mao2( ), Yadong Li5
State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, China University of Petroleum, Beijing 102249, China
Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Province Key Laboratory of Optoelectric Materials Science and Technology and Anhui Laboratory of Molecule-Based Materials, Anhui Normal University, Wuhu 241002, China
State key Lab of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemistry, Tsinghua University, Beijing 100084, China

§ Wenjie Wu and Yan Liu contributed equally to this work.

Abstract

The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction (ORR) is intensively increasing. Herein, single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst (Cu1/NC) was prepared by coordination pyrolysis strategy. Remarkably, the Cu1/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V (vs. RHE) in alkaline media, outperforming those of commercial Pt/C (0.851 V) and Cu nanoparticles anchored on N-doped porous carbon (CuNPs/NC-900), but also demonstrates high stability and methanol tolerance. Moreover, the Cu1/NC-900 based Zn-air battery exhibits higher power density, rechargeability and cyclic stability than the one based on Pt/C. Both experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu1/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect, resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR process. This study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.

Keywords: oxygen reduction reaction, non-noble metal, single atomic sites catalysts, nitrogen-doped carbon materials, carbon defect

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Publication history
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Acknowledgements

Publication history

Received: 21 August 2020
Revised: 22 September 2020
Accepted: 23 September 2020
Published: 23 October 2020
Issue date: April 2021

Copyright

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

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21804319 and 21971002), the Natural Science Foundation of Anhui province (Nos. 1908085QB45 and 2008085QB81) and the Education Department of Anhui Province Foundation (No. KJ2019A0503). We thank the BL14W1 station in Shanghai Synchrotron Radiation Facility (SSRF) and 1W1B station for XAFS measurement in Beijing Synchrotron Radiation Facility (BSRF). The calculations in this paper have been done on the supercomputing system of the National Supercomputing Center in Changsha.

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