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Thiocyanate-Modified Silver Nanofoam for Efficient CO2 Reduction to CO

  • Li Wei*
    Li Wei
    School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, New South Wales 2006, Australia
    *E-mail: [email protected] (L.W.).
    More by Li Wei
  • Hao Li
    Hao Li
    Department of Chemistry and the Oden Institute for Computational and Engineering Sciences, The University of Texas at Austin, 105 E. 24th Street, Stop A5300, Austin, Texas 78712, United States
    More by Hao Li
  • Junsheng Chen
    Junsheng Chen
    School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, New South Wales 2006, Australia
  • Ziwen Yuan
    Ziwen Yuan
    School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, New South Wales 2006, Australia
    More by Ziwen Yuan
  • Qianwei Huang
    Qianwei Huang
    School of Aerospace, Mechanical and Mechatronic Engineering, The University of Sydney, Sydney, New South Wales, 2006, Australia.
  • Xiaozhou Liao
    Xiaozhou Liao
    School of Aerospace, Mechanical and Mechatronic Engineering, The University of Sydney, Sydney, New South Wales, 2006, Australia.
  • Graeme Henkelman
    Graeme Henkelman
    Department of Chemistry and the Oden Institute for Computational and Engineering Sciences, The University of Texas at Austin, 105 E. 24th Street, Stop A5300, Austin, Texas 78712, United States
  • , and 
  • Yuan Chen*
    Yuan Chen
    School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, New South Wales 2006, Australia
    *E-mail: [email protected] (Y.C.).
    More by Yuan Chen
Cite this: ACS Catal. 2020, 10, 2, 1444–1453
Publication Date (Web):December 20, 2019
https://doi.org/10.1021/acscatal.9b04633
Copyright © 2019 American Chemical Society

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    Abstract

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    Ag is a promising electrocatalyst for electrochemical reduction of CO2 to CO due to its relatively low cost and high activity. However, it is challenging to achieve high reaction rates while maintaining good selectivity. Here, we used an H2 bubble-templated electrodeposition method in a thiocyanate (SCN)-containing aqueous electrolyte to synthesize a hierarchically porous Ag nanofoam (AgNF) with curved Ag surfaces modified by SCN. This AgNF demonstrates excellent performance for CO2 reduction with a high CO Faradaic efficiency (FECO) of 97%. It can maintain over 90% FECO in a wide potential window (−0.5 to −1.2 VRHE), enabling the maximum CO selective current density of 33 mA cm–2 and the mass activity of 23.5 A gAg–1, which are the highest values among recently reported Ag-based electrocatalysts. Mechanism studies reveal that the catalytic performance of the AgNF correlates with the density of surface SCN ligands, which exhibit excellent electrochemical stability under negative potentials. Density functional theory calculations suggest that SCN ligands promote the formation of COOH* intermediates by modifying the local electron density at the active sites. Further, the synthesis method is applicable to different catalyst substrates. For example, the AgNF grown on a carbon-based gas diffusion film exhibits an ultrahigh mass activity of 52.1 A gAg–1 and maintains its high CO selectivity simultaneously, demonstrating excellent potentials for practical applications.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.9b04633.

    • SEM and TEM images of AgNPs; estimation of SCN coverage on AgNFs; XPS spectra of AgSCN and Cl 2p region; typical j–t curves and FECO values of AgNF, AgNP, and Ag foil obtained at −1.2 V vs RHE; FECO and FEH2 of Ag catalysts; ECSA measurements; properties and CO2 electrochemical reduction performance at −0.6 V vs RHE of various electrodes; performance comparison of various Ag electrocatalysts for CO2 reduction in aqueous electrolytes; SEM images of the AgNF after 2 h discharging at various potentials; high-resolution XPS spectra of Ag 3d in various samples; HAADF-STEM images, the corresponding EDX elemental maps, Raman spectra, ECSA, FECO, and CO specific current densities of AgNF-R1 and AgNF-R2; and the free energy diagram of HER on different Ag models (PDF)

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