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Nano Research 2022, 15(5): 4014-4022 https://doi.org/10.1007/s12274-022-4177-x
Research Article | Issue | Published: 15 February 2022

Tuning the reaction path of CO2 electroreduction reaction on indium single-atom catalyst: Insights into the active sites

Show Author's Information Jiawei Zhang1,§,  Gangming Zeng1,§,  Lanlan Chen2,§,  Wenchuan Lai1,  Yuliang Yuan1,  Yangfan Lu3,  Chao Ma1,  Wenhua Zhang2( ),  Hongwen Huang1( )
College of Materials Science and Engineering, Advanced Catalytic Engineer Research Center of the Ministry of Education, Hunan University, Changsha 410082, China
Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China
State Key Lab of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China

§ Jiawei Zhang, Gangming Zeng, and Lanlan Chen contributed equally to this work.

Keywords:
single atom catalysts, CO2 reduction , coordination structure, product selectivity, active sites shift
Topics:
Selective catalytic reduction
Cite this article:
Zhang J, Zeng G, Chen L, et al. Tuning the reaction path of CO2 electroreduction reaction on indium single-atom catalyst: Insights into the active sites. Nano Research, 2022, 15(5): 4014-4022. https://doi.org/10.1007/s12274-022-4177-x
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Abstract Full text Electronic supplementary material About this article

Modulating the local coordination structure of metal single-atom catalysts (SACs) is extensively employed to tune the catalytic activity, but rarely involved in regulating the reaction pathway which fundamentally determines the product selectivity. Herein, we report that the product selectivity of electrochemical CO2 reduction (CO2RR) on the single-atom indium-NxC4−x (1 ≤ x ≤ 4) catalysts could be tuned from formate to CO by varying the carbon and nitrogen occupations in the first coordination sphere. Surprisingly, the optimal In SAC showed great promise for CO production with the maximum Faradic efficiency of 97%, greatly different from the reported In-based catalysts where the formate is the dominant product. Combined experimental verifications and theoretical simulations reveal that the selectivity switch from formate to CO on In SACs originates from active sites shift from indium center to the indium-adjacent carbon atom, where the indium site favors formate formation and the indium-adjacent carbon site prefers the CO pathway. The present work suggests the active sites in metal SACs may shift from the widely accepted metal center to surrounding carbon atoms, thereby offering a new implication to revisit the active sites for metal SACs.


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About this article

Tuning the reaction path of CO2 electroreduction reaction on indium single-atom catalyst: Insights into the active sites

Show Author's information Jiawei Zhang1,§, Gangming Zeng1,§, Lanlan Chen2,§, Wenchuan Lai1, Yuliang Yuan1, Yangfan Lu3, Chao Ma1, Wenhua Zhang2( ), Hongwen Huang1( )
College of Materials Science and Engineering, Advanced Catalytic Engineer Research Center of the Ministry of Education, Hunan University, Changsha 410082, China
Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China
State Key Lab of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China

§ Jiawei Zhang, Gangming Zeng, and Lanlan Chen contributed equally to this work.

Abstract

Modulating the local coordination structure of metal single-atom catalysts (SACs) is extensively employed to tune the catalytic activity, but rarely involved in regulating the reaction pathway which fundamentally determines the product selectivity. Herein, we report that the product selectivity of electrochemical CO2 reduction (CO2RR) on the single-atom indium-NxC4−x (1 ≤ x ≤ 4) catalysts could be tuned from formate to CO by varying the carbon and nitrogen occupations in the first coordination sphere. Surprisingly, the optimal In SAC showed great promise for CO production with the maximum Faradic efficiency of 97%, greatly different from the reported In-based catalysts where the formate is the dominant product. Combined experimental verifications and theoretical simulations reveal that the selectivity switch from formate to CO on In SACs originates from active sites shift from indium center to the indium-adjacent carbon atom, where the indium site favors formate formation and the indium-adjacent carbon site prefers the CO pathway. The present work suggests the active sites in metal SACs may shift from the widely accepted metal center to surrounding carbon atoms, thereby offering a new implication to revisit the active sites for metal SACs.

Keywords: single atom catalysts, CO2 reduction , coordination structure, product selectivity, active sites shift

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Publication history
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Acknowledgements

Publication history

Received: 02 January 2022
Revised: 13 January 2022
Accepted: 17 January 2022
Published: 15 February 2022
Issue date: May 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21905089, 2021RC3065, and 2021RC2053), the National Key Research and Development Program of China (No. 2021YFA1502000), the Science and Technology Innovation Program of Hunan Province (Nos. 2021RC3065 and 2021RC2053), Hunan Provincial Natural Science Foundation of China (No. 2020JJ2001), Shenzhen Science and Technology Program (No. JCYJ20210324120800002), and the Hefei National Laboratory for Physical Sciences at the Microscale (No. KF2020108). The calculations were performed on the supercomputing center of the University of Science and Technology of China (USTC-SCC) and Guangzhou-SCC.

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