Achieving highly selective electrochemical CO2 reduction to C2H4 on Cu nanosheets

doi:10.1016/j.jechem.2022.11.058

Journal of Energy Chemistry ›› 2023, Vol. 79 ›› Issue (4): 312-320.DOI: 10.1016/j.jechem.2022.11.058

Achieving highly selective electrochemical CO₂ reduction to C₂H₄ on Cu nanosheets

Huan Xie^a,b,1, Ruikuan Xie^a,1, Zhiyuan Zhang^c, Yongyu Pang^a,d, Yuting Luo^c, Jiong Li^e, Bilu Liu^c, Maria-Magdalena Titirici^f, Guoliang Chai^a,d,*

^aState Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, Fujian, China;
^bJiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, Jiangsu, China;
^cShenzhen Geim Graphene Center (SGC), Tsinghua-Berkeley Shenzhen Institute (TBSI) and Tsinghua Shenzhen International Graduate School (TSIGS), Tsinghua University, Shenzhen 518055, Guangdong, China;
^dSchool of Chemical Science, University of Chinese Academy of Sciences, Beijing 100049, China;
^eShanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China;
^fDepartment of Chemical Engineering, Imperial College London, SW7 2AZ, UK

Received:2022-08-09 Revised:2022-11-30 Accepted:2022-11-30 Online:2023-04-15 Published:2023-05-30
Contact: * E-mail address: g.chai@fjirsm.ac.cn (G. Chai).
About author:¹These authors contributed equally to this work.

Abstract

Abstract: The conversion of CO₂ into value-added chemicals coupled with the storage of intermittent renewable electricity is attractive. CuO nanosheets with an average size and thickness of ~ 30 and ~ 20 nm have been developed, which are in situ reduced into Cu nanosheets during electrochemical CO₂ reduction reac-tion (ECO₂RR). The derived Cu nanosheets demonstrate much higher selectivity for C₂H₄ production than commercial CuO derived Cu powder, with an optimum Faradaic efficiency of 56.2% and a partial current density of C₂H₄ as large as 171.0 mA cm^-2 in a gas diffusion flow cell. The operando attenuated total reflectance-Fourier transform infrared spectra measurements and density functional theory simulations illustrate that the high activity and selectivity of Cu nanosheets originate from the edge sites on Cu nanosheets with a coordinate number around 5 (4-6), which facilitates the formation of *CHO rather than *COH intermediate, meanwhile boosting the C—C coupling reaction of *CO and *CHO intermediates, which are the critical steps for C₂H₄ formation.

Key words: Electrochemical CO₂ reduction, Cu nanosheets, C₂H₄, High selectivity, Coordination number

Huan Xie, Ruikuan Xie, Zhiyuan Zhang, Yongyu Pang, Yuting Luo, Jiong Li, Bilu Liu, Maria-Magdalena Titirici, Guoliang Chai. Achieving highly selective electrochemical CO₂ reduction to C₂H₄ on Cu nanosheets[J]. Journal of Energy Chemistry, 2023, 79(4): 312-320.

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Achieving highly selective electrochemical CO₂ reduction to C₂H₄ on Cu nanosheets

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