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Electrochemical Hydrogen Oxidation on Pt(100): a Combined Direct Molecular Dynamics/Density Functional Theory Study

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Abstract

We have studied the hydrogen oxidation reaction on various catalytic sites at the water/Pt(100) interface with first-principles direct molecular dynamics and minimum energy pathway calculations. The calculations indicate that the mechanism for electro-oxidation of H2 on terrace sites of the Pt(100) surface depends on the concentration of inactive adsorbed hydrogen on the electrode surface. Near the reversible potential, the electro-oxidation follows the Tafel-Volmer homolytic cleavage of H2 at low coverage of adsorbed hydrogen. If the surface is covered with ca. 1 monolayer of hydrogen, however, the oxidation proceeds by the Heyrovsky-Volmer mechanism. We found good agreement between measured and predicted Tafel plots, indicating that hydrogen oxidation/reduction reaction on Pt(100) takes place via the Heyrovsky-Volmer mechanism under ca. 1 monolayer coverage of inactive adsorbed hydrogen.

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Acknowledgments

This work was supported by the NASA-UPR Center for Advanced Nanoscale Materials.

Author Contributions

The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript.

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Author notes

  1. Juan A. Santana

    Present address: Department of Chemistry, University of Puerto Rico at Cayey, P. O. Box 372230, Cayey, PR, 00737-2230, USA

Authors and Affiliations

  1. Department of Chemistry, University of Puerto Rico at Rio Piedras, P.O. Box 23346, San Juan, PR, 00931, USA

    Juan A. Santana, José J. Saavedra-Arias & Yasuyuki Ishikawa

  2. Department of Physics, Universidad Nacional, Heredia, 40101, Costa Rica

    José J. Saavedra-Arias

Authors
  1. Juan A. Santana
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  2. José J. Saavedra-Arias
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  3. Yasuyuki Ishikawa
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Correspondence to Juan A. Santana.

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Santana, J.A., Saavedra-Arias, J.J. & Ishikawa, Y. Electrochemical Hydrogen Oxidation on Pt(100): a Combined Direct Molecular Dynamics/Density Functional Theory Study. Electrocatalysis 6, 534–543 (2015). https://doi.org/10.1007/s12678-015-0272-z

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  • DOI: https://doi.org/10.1007/s12678-015-0272-z

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