Temperature Dependence of Proton Electroreduction Kinetics at Gold(111) and (210) Surfaces

Abstract

Rate-potential data are reported for proton electroreduction on Au(111) and (210) in acidic perchlorate electrolytes over the temperature range 0-60 C, and examined with regard to temperature dependence of the transfer coefficient alpha. Since the Tafel plots exhibit significant curvature the analysis requires information on the temperature-dependent thermodynamics (i.e. the reaction entropy) for the proton discharge step. This was estimated from temperature-dependent voltammetry of reversible proton discharge to form adsorbed hydrogen on platinum. When evaluated at a constant overpotential for the proton discharge step, alpha for this reaction on both Au(111) and (210) is independent of temperature. An effect of electrocatalysts for proton reduction on Au(111) engendered by prior voltametric oxide formation was also observed. This effect is attributed to formation of surface defects on the basis of recently reported scanning tunneling microscopy data. Surface structural changes are also evident in the morphology of cyclic voltammograms obtained in the double-layer region. Electrochemical effects disappear with time when potential is held in the double layer region, and more rapidly at higher temperatures.

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Document Details

Document Type
Technical Report
Publication Date
May 31, 1991
Accession Number
ADA237460

Entities

People

  • A. Hamelin
  • L. Stoicoviciu
  • Michael J. Weaver
  • S. C. Chang

Organizations

  • Purdue University

Tags

Communities of Interest

  • Materials and Manufacturing Processes

DTIC Thesaurus Topics

  • Charge Transfer
  • Chemical Reactions
  • Chemistry
  • Curvature
  • Electrochemical Reactions
  • Electrodes
  • Entropy
  • Microscopy
  • Military Research
  • Perchlorates
  • Platinum
  • Protons
  • Quantum Tunneling
  • Reversible
  • Scanning
  • Thermodynamics
  • Universities

Fields of Study

  • Materials science

Readers

  • Electrochemical Engineering/ Fuel Cell Technologies
  • Electrochemical Surface Science

Technology Areas

  • Microelectronics