Electroreduction Reaction Mechanism of Carbon Dioxide to C2 Products via Cu/Au Bimetallic Catalysis: A Theoretical Prediction

Xia-Guang Zhang; Shishi Feng; Chao Zhan; De-Yin Wu; Yi Zhao; Zhong-Qun Tian

doi:10.1021/acs.jpclett.0c01970

Electroreduction Reaction Mechanism of Carbon Dioxide to C₂ Products via Cu/Au Bimetallic Catalysis: A Theoretical Prediction

J Phys Chem Lett. 2020 Aug 20;11(16):6593-6599. doi: 10.1021/acs.jpclett.0c01970. Epub 2020 Aug 3.

Authors

Xia-Guang Zhang¹, Shishi Feng², Chao Zhan², De-Yin Wu², Yi Zhao², Zhong-Qun Tian²

Affiliations

¹ Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, College of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang 453007, China.
² State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.

PMID: 32787232
DOI: 10.1021/acs.jpclett.0c01970

Abstract

Understanding the bimetallic interfacial effects on the catalytic CO₂ reduction reaction (CO₂RR) is an important and challenging issue. Herein, the geometric structure, electronic structure, and electrocatalytic property of Cu(submonolayer)/Au bimetallic interfaces are investigated by using density functional theory calculation. The results predict that the expansion of the Cu lattice can significantly modulate the CO₂RR performance, the Cu(submonolayer)/Au interface has good surface activity promoting the reduction of CO₂ to C₂ compounds, and the final products of CO₂RR on Cu/Au(111) and Cu/Au(100) surfaces are ethanol and a mixture of ethanol and ethylene, respectively. Furthermore, with regard to surface coverage and adsorption energy being two essential parameters for CO₂RR, we demonstrate that the reaction of *CO and *CHO is the key process for obtaining the C₂ products on the Cu/Au interface. This study offers a useful strategy for improving the surface activity and selectivity for CO₂RR.