Mechanistic Insights for Low-Overpotential Electroreduction of CO2 to CO on Copper Nanowires

Liang Cao, David Raciti, Chenyang Li, Kenneth J.T. Livi, Paul F. Rottmann, Kevin J. Hemker, Tim Mueller, Chao Wang

Research output: Contribution to journalArticlepeer-review

99 Scopus citations

Abstract

Recent developments of copper (Cu)-based nanomaterials have enabled the electroreduction of CO2 at low overpotentials. The mechanism of low-overpotential CO2 reduction on these nanocatalysts, however, largely remains elusive. We report here a systematic investigation of CO2 reduction on highly dense Cu nanowires, with the focus placed on understanding the surface structure effects on the formation of CO (∗ denotes an adsorption site on the catalyst surface) and the evolution of gas-phase CO product (CO(g)) at low overpotentials (more positive than -0.5 V). Cu nanowires of distinct nanocrystalline and surface structures are studied comparatively to build up the structure-property relationships, which are further interpreted by performing density functional theory (DFT) calculations of the reaction pathway on the various facets of Cu. A kinetic model reveals competition between CO(g) evolution and ∗CO poisoning depending on the electrode potential and surface structures. Open and metastable facets such as (110) and reconstructed (110) are found to be likely the active sites for the electroreduction of CO2 to CO at the low overpotentials.

Original languageEnglish
Pages (from-to)8578-8587
Number of pages10
JournalACS Catalysis
Volume7
Issue number12
DOIs
StatePublished - Dec 1 2017

Bibliographical note

Publisher Copyright:
© 2017 American Chemical Society.

Keywords

  • carbon dioxide reduction
  • copper nanowires
  • density functional theory
  • electrocatalysis

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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