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A DFT study of CO2 electrochemical reduction on Pb(211) and Sn(112)

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  • Special Issue Heterogeneous Catalysis Theory
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Abstract

Electrochemical reduction of CO2 has the benefit of turning greenhouse gas emissions into useful resources. We performed a comparative study of the electrochemical reduction of CO2 on stepped Pb(211) and Sn(112) surfaces based on the results of density functional theory slab calculations. We mapped out the potential energy profiles for electrochemical reduction of CO2 to formate and other possible products on both surfaces. Our results show that the first step is the formation of the adsorbed formate (HCOO*) species through an Eley-Rideal mechanism. The formate species can be reduced to HCOO− through a one-electron reduction in basic solution, which produces formic acid as the predominant product. The respective potentials of forming HCOO* are predicted to be −0.72 and −0.58 V on Pb and Sn. Higher overpotentials make other reaction pathways accessible, leading to different products. On Sn(112), CO and CH4 can be generated at −0.65 V following formate formation. In contrast, the limiting potential to access alternative reaction channels on Pb(211) is −1.33 V, significantly higher than that of Sn.

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Authors and Affiliations

  1. Key Laboratory for Green Chemical Technology, School of Chemical Engineering and Technology, Tianjin University; Collaborative Innovation Center of Chemical Science and Engineering, Tianjin, 300072, China

    Chaonan Cui, Hua Wang, Xinli Zhu, Jinyu Han & Qingfeng Ge

  2. Department of Chemistry and Biochemistry, Southern Illinois University, Carbondale, IL, 62901, USA

    Qingfeng Ge

Authors
  1. Chaonan Cui
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  2. Hua Wang
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  3. Xinli Zhu
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  4. Jinyu Han
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  5. Qingfeng Ge
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Correspondence to Hua Wang or Qingfeng Ge.

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Cui, C., Wang, H., Zhu, X. et al. A DFT study of CO2 electrochemical reduction on Pb(211) and Sn(112). Sci. China Chem. 58, 607–613 (2015). https://doi.org/10.1007/s11426-015-5323-z

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  • DOI: https://doi.org/10.1007/s11426-015-5323-z

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