Selectivity of CO2 Reduction on Copper Electrodes: The Role of the Kinetics of Elementary Steps

Authors

  • Dr. Xiaowa Nie,

    1. William G. Lowrie Department of Chemical & Biomolecular Engineering, The Ohio State University, 221A Koffolt Laboratories, 140 West 19th Ave., Columbus, OH 43210 (USA)
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  • Monica R. Esopi,

    1. Department of Chemical Engineering, Pennsylvania State University, 104 Fenske Lab, University Park, PA 16802 (USA)
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  • Prof. Michael J. Janik,

    Corresponding author
    1. Department of Chemical Engineering, Pennsylvania State University, 104 Fenske Lab, University Park, PA 16802 (USA)
    • Department of Chemical Engineering, Pennsylvania State University, 104 Fenske Lab, University Park, PA 16802 (USA)
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  • Prof. Aravind Asthagiri

    Corresponding author
    1. William G. Lowrie Department of Chemical & Biomolecular Engineering, The Ohio State University, 221A Koffolt Laboratories, 140 West 19th Ave., Columbus, OH 43210 (USA)
    • William G. Lowrie Department of Chemical & Biomolecular Engineering, The Ohio State University, 221A Koffolt Laboratories, 140 West 19th Ave., Columbus, OH 43210 (USA)
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  • We acknowledge the Ohio Supercomputing Center for providing the computational resources for this work. This work was supported by the Center for Atomic Level Catalyst Design, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001058.

Abstract

original image

On the right path: Based on DFT calculations (incorporating the role of water solvation) of the activation barriers of elementary steps, a new path that leads to methane and ethylene for CO2 electroreduction on Cu(111) was identified. Methane formation proceeds through reduction of CO to COH (path II, see picture), which leads to CHx species that can produce both methane and ethylene, as observed experimentally.

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