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Research Article

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

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
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Graphical Abstract

Interatomic electron transfer between Cu and Zn atoms enhances the electroreduction CO2 reaction activity toward CO production.

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

CuZn diatomic siteCO2 electroreduction reactioninteratomic electron transferin situ characterizations

Electronic Supplementary Material

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Nano Research
Volume 16 Issue 7,
July 2023
Pages 8863-8870
DOI: 10.1007/s12274-023-5577-2
Cite this article:
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
Topics:
Electrocatalysis Electrocatalysts

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Received: 29 January 2023
Revised: 12 February 2023
Accepted: 13 February 2023
Published: 13 March 2023
© Tsinghua University Press 2023
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