Decrypting the Controlled Product Selectivity over Ag-Cu Bimetallic Surface Alloys for Electrochemical CO2 Reduction

Daixing Wei; Yiqing Wang; Chung-Li Dong; Zhengqi Zhang; Xinyu Wang; Yu-Cheng Huang; Yuchuan Shi; Xiaoli Zhao; Jialin Wang; Ran Long; Yujie Xiong; Fan Dong; Mingtao Li; Shaohua Shen

doi:10.1002/anie.202217369

Decrypting the Controlled Product Selectivity over Ag-Cu Bimetallic Surface Alloys for Electrochemical CO₂ Reduction

Angew Chem Int Ed Engl. 2023 May 2;62(19):e202217369. doi: 10.1002/anie.202217369. Epub 2023 Mar 30.

Authors

Daixing Wei¹, Yiqing Wang¹, Chung-Li Dong², Zhengqi Zhang¹, Xinyu Wang³, Yu-Cheng Huang², Yuchuan Shi¹, Xiaoli Zhao⁴, Jialin Wang¹, Ran Long³, Yujie Xiong³, Fan Dong⁴, Mingtao Li¹, Shaohua Shen¹

Affiliations

¹ International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, 710049, China.
² Department of Physics, Tamkang University, New Taipei City, 25137, Taiwan.
³ Hefei National Laboratory for Physical Sciences at the Microscale, Frontiers Science Center for Planetary Exploration and Emerging Technologies, School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, China.
⁴ Research Center for Environmental and Energy Catalysis Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 611731, China.

PMID: 36916416
DOI: 10.1002/anie.202217369

Abstract

Electrochemical CO₂ reduction reaction (ECO₂ RR) with controlled product selectivity is realized on Ag-Cu bimetallic surface alloys, with high selectivity towards C2 hydrocarbons/alcohols (≈60 % faradaic efficiency, FE), C1 hydrocarbons/alcohols (≈41 % FE) and CO (≈74 % FE) achieved by tuning surface compositions and applied potentials. In situ spectral investigations and theoretical calculations reveal that surface-composition-dependent d-band center could tune *CO binding strengths, regulating the *CO subsequent reaction pathways and then the product selectivity. Further adjusting the applied potentials will alter the energy of participated electrons, which leads to controlled ECO₂ RR selectivity towards desired products. A predominant region map, with an indicator proposed to evaluate the thermodynamic predominance of the *CO subsequent reactions, is then provided as a reliable theoretical guidance for the controllable ECO₂ RR product selectivity over bimetallic alloys.

Keywords: Alloys; CO2 Reduction; Controlled Product Selectivity; Electrochemistry.

Abstract

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