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Insights into electrocatalysis.

Alfred B Anderson1

  • 1Department of Chemistry, Case Western Reserve University, Cleveland, Ohio 44106-7078, USA. aba@po.cwru.edu

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|December 14, 2011
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Summary
This summary is machine-generated.

This study calculates reversible potentials for oxygen reduction on platinum electrocatalysts, considering adsorption Gibbs energies. Effective reversible potentials are reduced by Gibbs energy loss, impacting oxygen reduction onset potentials.

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Area of Science:

  • Electrochemistry
  • Surface Science
  • Computational Materials Science

Background:

  • Standard reversible potentials for bulk reactions are modified by reactant/product adsorption on electrocatalyst surfaces.
  • Adsorption Gibbs energies (Δ(ads)G) are crucial for determining surface reversible potentials.
  • Oxygen reduction reaction (ORR) intermediates' adsorption strengths influence overall reaction efficiency.

Purpose of the Study:

  • To calculate reversible potentials for oxygen reduction steps on platinum electrocatalyst surfaces.
  • To assess the accuracy of using adsorption Gibbs energies at the potential of zero charge.
  • To determine the effective reversible potential for the four-electron ORR mechanism on platinum.

Main Methods:

  • Utilized Interface 1.0 computational code to calculate potential-dependent electrochemical interfaces.
  • Employed experimentally determined data for adsorption Gibbs energies of O, OH, and OOH intermediates.
  • Calculated O-O bond dissociation Gibbs energies for key ORR intermediate steps.

Main Results:

  • Reversible potentials for ORR on platinum were accurately benchmarked using Interface 1.0.
  • Using Δ(ads)G at the potential of zero charge provides accuracy within ~0.1 V compared to bulk potentials.
  • The OOH(ads) → O(ads) + OH(ads) step exhibits a ~1.2 eV exergonic Gibbs energy on platinum, reducing the effective reversible potential to ~0.93 V.

Conclusions:

  • Adsorption Gibbs energies significantly influence surface reversible potentials for ORR.
  • The effective reversible potential, not kinetics, dictates the onset potential for four-electron ORR.
  • Calculations suggest the onset potential for ORR on Pt(111) equals its effective reversible potential.