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

  • Xia-Guang Zhang*
    Xia-Guang Zhang
    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
    *Email: [email protected]
    More by Xia-Guang Zhang
    Orcidhttp://orcid.org/0000-0002-9223-0852
  • , 
  • Shishi Feng
    Shishi Feng
    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
    More by Shishi Feng
  • , 
  • Chao Zhan
    Chao Zhan
    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
    More by Chao Zhan
  • , 
  • De-Yin Wu*
    De-Yin Wu
    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
    *Email: [email protected]
    More by De-Yin Wu
    Orcidhttp://orcid.org/0000-0001-5260-2861
  • , 
  • Yi Zhao*
    Yi Zhao
    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
    *Email: [email protected]
    More by Yi Zhao
    Orcidhttp://orcid.org/0000-0003-1711-4250
  • , and 
  • Zhong-Qun Tian
    Zhong-Qun Tian
    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
    More by Zhong-Qun Tian
    Orcidhttp://orcid.org/0000-0002-9775-8189
Cite this: J. Phys. Chem. Lett. 2020, 11, 16, 6593–6599
Publication Date (Web):July 27, 2020
https://doi.org/10.1021/acs.jpclett.0c01970
Copyright © 2020 American Chemical Society
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    Abstract

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    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.

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    • Computational details, optimized adsorption configuration of reaction intermediates, mechanisms of hydrogenation of CO2 to C1 compounds, reaction energies of adsorbed intermediates, and coordinates for structures (PDF)

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