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Calculations of the pH-Dependent Onset Potential for CO Electrooxidation on Au(111)

  • Zhiyao Duan
    Zhiyao Duan
    Department of Chemistry and the Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712-0165, United States
    More by Zhiyao Duan
  •  and 
  • Graeme Henkelman*
    Graeme Henkelman
    Department of Chemistry and the Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712-0165, United States
    *E-mail: [email protected]
Cite this: Langmuir 2018, 34, 50, 15268–15275
Publication Date (Web):November 21, 2018
https://doi.org/10.1021/acs.langmuir.8b03644
Copyright © 2018 American Chemical Society

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    Abstract

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    CO electrooxidation on the Au(111) surface exhibits an onset potential that depends strongly on the pH of the electrolyte. In alkaline solution, the onset potential for CO electrooxidation is found, experimentally, to be 0.5 V lower than in acidic media on the reversible hydrogen electrode scale. This phenomenon is explained here with density functional theory which is used to calculate adsorbate binding energies including the electric double layer of the Au(111)/aqueous interface. Our model consists of a charged Au(111) slab and implicit solvation for the electrolyte. The double reference method is used to determine the potential-dependent CO electrooxidation reaction energetics. A microkinetic model, based upon the calculated reaction energetics, confirms the lower onset potential in alkaline media. Our results show that there are three factors contributing to the lower onset potential in base: (1) stronger CO adsorption, (2) attraction between adsorbed CO and OH, and (3) the high concentration of OH in base.

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