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Nano Research 2022, 15(9): 7959-7967 https://doi.org/10.1007/s12274-022-4497-x
Research Article | Issue | Published: 31 May 2022

Synergistically tuning the graphitic degree, porosity, and the configuration of active sites for highly active bifunctional catalysts and Zn-air batteries

Show Author's Information Yang Gao1,2,  Debin Kong1,3,  Fengli Cao1,  Shuai Teng1,  Tao Liang1,  Bin Luo4,  Bin Wang1,5( ),  Quan-Hong Yang2,  Linjie Zhi1,2,3( )
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
College of New Energy, Research Center for Advanced Chemical Engineering and Energy Materials, China University of Petroleum (East China), Qingdao 266580, China
Nanomaterials Centre, Australian Institute for Bioengineering and Nanotechnology and School of Chemical Engineering, The University of Queensland, Brisbane, QLD 4072, Australia
University of Chinese Academy of Sciences, Beijing 100049, China
Keywords:
electrocatalysis, Zn-air battery, bifunctional, Co–N–C, ZIFs
Topics:
Electrocatalysts
Cite this article:
Gao Y, Kong D, Cao F, et al. Synergistically tuning the graphitic degree, porosity, and the configuration of active sites for highly active bifunctional catalysts and Zn-air batteries. Nano Research, 2022, 15(9): 7959-7967. https://doi.org/10.1007/s12274-022-4497-x
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Abstract Full text Electronic supplementary material About this article

Rational design and tailoring of the structural features of Co–N–C catalysts are urgently required to construct highly efficient bifunctional non-noble metal electrocatalysts for both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Herein, we report a series of carbon-based catalysts with varied structural features, specifically the graphitic degree of carbon, porosity, and the configuration of active sites, and their effects on bifunctional oxygen electrocatalytic reactions. Through the synergistic tuning of these structural factors, the well-tailored Co–N–C catalyst exhibits a high bifunctional electrocatalytic activity, as revealed by a half-wave potential of 0.84 V for ORR and a low overpotential of 420 mV at 10 mA·cm−2 for OER. More impressively, the Zn-air battery using the optimum catalyst delivers excellent performance including a peak power density of 125.2 mW·cm−2 and a specific capacity of 790.8 mAh·gZn−1, as well as stable cycling durability, outperforming the noble metals-based catalysts. The first-principles calculations reveal that the interlayer interaction between the pyridinic N-doped graphene and the confined Co nanoparticles increases the electronic states of the active C atoms near the Fermi level, thus enhancing the adsorption of the HOO* intermediate and generating superior catalytic activity for bifunctional oxygen electrocatalysis. By comprehensively studying the structural factors of catalysts, the bifunctional catalytic behaviors, the use in a practical Zn-air device, and theoretical simulations, this work may also give inspirations to the design, use, and understanding of other kinds of catalysts.


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Electronic supplementary material
About this article

Synergistically tuning the graphitic degree, porosity, and the configuration of active sites for highly active bifunctional catalysts and Zn-air batteries

Show Author's information Yang Gao1,2, Debin Kong1,3, Fengli Cao1, Shuai Teng1, Tao Liang1, Bin Luo4, Bin Wang1,5( ), Quan-Hong Yang2, Linjie Zhi1,2,3( )
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
College of New Energy, Research Center for Advanced Chemical Engineering and Energy Materials, China University of Petroleum (East China), Qingdao 266580, China
Nanomaterials Centre, Australian Institute for Bioengineering and Nanotechnology and School of Chemical Engineering, The University of Queensland, Brisbane, QLD 4072, Australia
University of Chinese Academy of Sciences, Beijing 100049, China

Abstract

Rational design and tailoring of the structural features of Co–N–C catalysts are urgently required to construct highly efficient bifunctional non-noble metal electrocatalysts for both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Herein, we report a series of carbon-based catalysts with varied structural features, specifically the graphitic degree of carbon, porosity, and the configuration of active sites, and their effects on bifunctional oxygen electrocatalytic reactions. Through the synergistic tuning of these structural factors, the well-tailored Co–N–C catalyst exhibits a high bifunctional electrocatalytic activity, as revealed by a half-wave potential of 0.84 V for ORR and a low overpotential of 420 mV at 10 mA·cm−2 for OER. More impressively, the Zn-air battery using the optimum catalyst delivers excellent performance including a peak power density of 125.2 mW·cm−2 and a specific capacity of 790.8 mAh·gZn−1, as well as stable cycling durability, outperforming the noble metals-based catalysts. The first-principles calculations reveal that the interlayer interaction between the pyridinic N-doped graphene and the confined Co nanoparticles increases the electronic states of the active C atoms near the Fermi level, thus enhancing the adsorption of the HOO* intermediate and generating superior catalytic activity for bifunctional oxygen electrocatalysis. By comprehensively studying the structural factors of catalysts, the bifunctional catalytic behaviors, the use in a practical Zn-air device, and theoretical simulations, this work may also give inspirations to the design, use, and understanding of other kinds of catalysts.

Keywords: electrocatalysis, Zn-air battery, bifunctional, Co–N–C, ZIFs

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Publication history
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Acknowledgements

Publication history

Received: 12 March 2022
Revised: 23 April 2022
Accepted: 04 May 2022
Published: 31 May 2022
Issue date: September 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

The authors acknowledge the financial support from the National Natural Science Foundation of China (Nos. 51425302, 51702062, and U20A20131), the National Key R&D Program of China (No. 2021YFA1202802), the China Postdoctoral Science Foundation Funded Project (No. 2021M690801), the CAS Pioneer Hundred Talents Program, and the China University of Petroleum (East China).

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