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Surface-Morphology-Dependent Electrolyte Effects on Gold-Catalyzed Electrochemical CO2 Reduction
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    Surface-Morphology-Dependent Electrolyte Effects on Gold-Catalyzed Electrochemical CO2 Reduction
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    Clean Energy Research Center, Korea Institute of Science and Technology, Seoul 02792, Republic of Korea
    Fuel Cell Research Center, Korea Institute of Science and Technology, Seoul 02792, Republic of Korea
    § Division of Energy and Environmental Technology, KIST School, Korea University of Science and Technology, Seoul 02792, Republic of Korea
    Green School, Korea University, Seoul 02841, Republic of Korea
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2017, 121, 41, 22637–22643
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    https://doi.org/10.1021/acs.jpcc.7b06286
    Published September 26, 2017
    Copyright © 2017 American Chemical Society

    Abstract

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    The electrocatalytic property of a flat or an oxide-derived nanostructure Au electrode was investigated using surface sensitive analysis methods such as impedance spectroscopy and Kelvin probe force microscopy (KPFM) when electrochemical conversion of carbon dioxide (CO2) to carbon monoxide (CO) was performed with either KHCO3- or NaHCO3-based neutral electrolyte. A strong dependence on the cation of the electrolyte was exhibited on the flat Au electrode surface. CO selectivity and capacitance dispersion are significantly higher with the KHCO3 electrolyte. On the other hand, the nanostructured Au electrodes, having much more improved activity and durability of CO2 reduction, showed much less electrolyte-dependent catalytic activity. The difference in CO selectivity with KHCO3 and NaHCO3 electrolytes can be explained by the difference in hydration level and consequent adsorption strength of the cations on the flat Au metal electrodes, implying that ion-pairing interactions between the metal, cations, CO2, and its intermediate play an important role in the reduction reaction. The local electric field fluctuation caused by the nanostructured rough Au surface can affect the electric double layer near the electrode surface and suppress the electrolyte-dependency of the reduction. Furthermore, according to X-ray spectroscopy analysis of the electrode after electrolysis, the nanostructured Au electrode is less prone to surface cation deposition. These results provide a basic understanding of the role of electrolyte cations in the CO2 reduction reaction.

    Copyright © 2017 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.7b06286.

    • Electric field map of a rough surface electrode and simulation script, SEM images and elemental maps from energy dispersive analysis of X-rays (EDAX) , and detailed explanation about the calculation of Faradaic efficiency (PDF)

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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2017, 121, 41, 22637–22643
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.7b06286
    Published September 26, 2017
    Copyright © 2017 American Chemical Society

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