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Nano Research 2023, 16(7): 8863-8870 https://doi.org/10.1007/s12274-023-5577-2
Research Article | Issue | Published: 13 March 2023

Interatomic electron transfer promotes electroreduction CO2-to-CO efficiency over a CuZn diatomic site

Show Author's Information Jican Hao1,  Han Zhu1( ),  Qi Zhao2,  Jiace Hao1,  Shuanglong Lu1,  Xiaofan Wang1,  Fang Duan1,  Mingliang Du1( )
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China
School of Biological and Chemical Sciences, Queen Mary University of London, London E1 4NS, UK
Keywords:
in situ characterizations, CO2 electroreduction reaction, CuZn diatomic site, interatomic electron transfer
Topics:
Electrocatalysis Electrocatalysts
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Hao J, Zhu H, Zhao Q, et al. Interatomic electron transfer promotes electroreduction CO2-to-CO efficiency over a CuZn diatomic site. Nano Research, 2023, 16(7): 8863-8870. https://doi.org/10.1007/s12274-023-5577-2
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Abstract Full text Electronic supplementary material About this article

Diatomic site catalysts (DACs) with two adjacent atomic metal species can provide synergistic interactions and more sophisticated functionalities to break the bottleneck of intrinsic drawbacks of single atom catalysts (SACs). Herein, we have designed a CuZn diatomic site (CuZn-DAS) electrocatalyst with unique coordination structure (CuN4–ZnN4) by anchoring and ordering the spatial distance between the metal precursors on the carbon nitride (C3N4) derived N-doped carbon (NC) substrate. The CuZn-DAS/NC shows high activity and selectivity for electroreduction CO2 into CO. The Faradaic efficiency for CO of CuZn-DAS/NC (98.4%) is higher than that of Cu single atomic site on NC (Cu-SAS/NC) (36.4%) and Zn single atomic site on NC (Zn-SAS/NC) (66.8%) at −0.6 V versus reversible hydrogen electrode (vs. RHE). In situ characterizations reveal that the CuZn-DAS is more favorable for the formation and adsorption of *COOH than those of the electrocatalysts with single atomic site. Theorical calculations show that the charge redistribution of Zn site in CuZn-DAS/NC caused by the considerable electron transfers from Zn atoms to the adjacent Cu atoms can reduce the adsorption energy barriers for *COOH and *CO production, improving the activity and CO selectivity.


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Electronic supplementary material
About this article

Interatomic electron transfer promotes electroreduction CO2-to-CO efficiency over a CuZn diatomic site

Show Author's information Jican Hao1, Han Zhu1( ), Qi Zhao2, Jiace Hao1, Shuanglong Lu1, Xiaofan Wang1, Fang Duan1, Mingliang Du1( )
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China
School of Biological and Chemical Sciences, Queen Mary University of London, London E1 4NS, UK

Abstract

Diatomic site catalysts (DACs) with two adjacent atomic metal species can provide synergistic interactions and more sophisticated functionalities to break the bottleneck of intrinsic drawbacks of single atom catalysts (SACs). Herein, we have designed a CuZn diatomic site (CuZn-DAS) electrocatalyst with unique coordination structure (CuN4–ZnN4) by anchoring and ordering the spatial distance between the metal precursors on the carbon nitride (C3N4) derived N-doped carbon (NC) substrate. The CuZn-DAS/NC shows high activity and selectivity for electroreduction CO2 into CO. The Faradaic efficiency for CO of CuZn-DAS/NC (98.4%) is higher than that of Cu single atomic site on NC (Cu-SAS/NC) (36.4%) and Zn single atomic site on NC (Zn-SAS/NC) (66.8%) at −0.6 V versus reversible hydrogen electrode (vs. RHE). In situ characterizations reveal that the CuZn-DAS is more favorable for the formation and adsorption of *COOH than those of the electrocatalysts with single atomic site. Theorical calculations show that the charge redistribution of Zn site in CuZn-DAS/NC caused by the considerable electron transfers from Zn atoms to the adjacent Cu atoms can reduce the adsorption energy barriers for *COOH and *CO production, improving the activity and CO selectivity.

Keywords: in situ characterizations, CO2 electroreduction reaction, CuZn diatomic site, interatomic electron transfer

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Publication history
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Acknowledgements

Publication history

Received: 29 January 2023
Revised: 12 February 2023
Accepted: 13 February 2023
Published: 13 March 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This study was supported by the National Natural Science Foundation of China (Nos. 52073124 and 52273058), the Natural Science Foundation of Jiangsu Province (No. SBK2022030167), the MOE & SAFEA, 111 Project (No. B13025), and the Fundamental Research Funds for the Central Universities. The authors would also like to thank the Central Laboratory, School of Chemical and Material Engineering, Jiangnan University.

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