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

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Catal. 2017, 7, 12, 8578-8587
    Research Article

    Mechanistic Insights for Low-Overpotential Electroreduction of CO2 to CO on Copper Nanowires
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    † †Department of Chemical and Biomolecular Engineering, ‡Department of Materials Science and Engineering §Department of Physics and Astronomy, and ∥Department of Mechanical Engineering, Johns Hopkins University, Baltimore, Maryland 21218, United States
    *E-mail for T.M.: [email protected]
    *E-mail for C.W.: [email protected]
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    ACS Catalysis

    Cite this: ACS Catal. 2017, 7, 12, 8578–8587
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    https://doi.org/10.1021/acscatal.7b03107
    Published November 9, 2017
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    Abstract

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    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.

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    • Experimental details of the Cu nanowire synthesis, material characterization, and electrochemical characterization and theoretical details of DFT calculations (PDF)

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    This article is cited by 102 publications.

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    Cite this: ACS Catal. 2017, 7, 12, 8578–8587
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