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Understanding the Origin of Selective Reduction of CO2 to CO on Single-Atom Nickel Catalyst

  • Shi He
    Shi He
    Department of Chemistry, Duke University, Durham, North Carolina 27708, United States
    More by Shi He
  • Dong Ji
    Dong Ji
    Department of Chemistry, Duke University, Durham, North Carolina 27708, United States
    More by Dong Ji
  • Junwei Zhang
    Junwei Zhang
    Material Science and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Jeddah, Kingdom of Saudi Arabia
    More by Junwei Zhang
  • Peter Novello
    Peter Novello
    Department of Chemistry, Duke University, Durham, North Carolina 27708, United States
  • Xueqian Li
    Xueqian Li
    Department of Chemistry, Duke University, Durham, North Carolina 27708, United States
    More by Xueqian Li
  • Qiang Zhang
    Qiang Zhang
    Material Science and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Jeddah, Kingdom of Saudi Arabia
    More by Qiang Zhang
  • Xixiang Zhang
    Xixiang Zhang
    Material Science and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Jeddah, Kingdom of Saudi Arabia
  • , and 
  • Jie Liu*
    Jie Liu
    Department of Chemistry, Duke University, Durham, North Carolina 27708, United States
    *E-mail: [email protected]. Phone: 919-660-1549.
    More by Jie Liu
Cite this: J. Phys. Chem. B 2020, 124, 3, 511–518
Publication Date (Web):December 27, 2019
https://doi.org/10.1021/acs.jpcb.9b09730
Copyright © 2019 American Chemical Society

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    Abstract

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    Electrochemical reduction of CO2 to CO offers a promising strategy for regulating the global carbon cycle and providing feedstock for the chemical industry. Understanding the origin that determines the faradaic efficiency (FE) of reduction of CO2 to CO is critical for developing a highly efficient electrocatalyst. Here, by constructing a single-atom Ni catalyst on nitrogen-doped winged carbon nanofiber (NiSA-NWC), we find that the single-atom Ni catalyst possesses the maximum CO FE of over 95% at −1.6 V vs Ag/AgCl, which is about 30% higher than the standard Ni nanoparticles on the same support. The Tafel analysis reveals that the single-atom Ni catalyst has a preferred reduction of CO2 to CO and a slower rate for the hydrogen evolution reaction. We propose that the domination of singular Ni1+ electronic states and limited hydrogen atom adsorption sites on the single-atom Ni catalyst lead to the observed high FE for CO2 reduction to CO.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcb.9b09730.

    • Structure characterization of NiNP-NWC catalysts, additional characterization of NiNP-NWC, NiSA-NWC, and Ni-WC catalysts, detection of the CO2 reduction products, modeling of catalytic sites, etc. (PDF)

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    This article is cited by 18 publications.

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