Density functional theory calculations for the hydrogen evolution reaction in an electrochemical double layer on the Pt(111) electrode

Phys Chem Chem Phys. 2007 Jul 7;9(25):3241-50. doi: 10.1039/b700099e. Epub 2007 May 30.

Abstract

We present results of density functional theory calculations on a Pt(111) slab with a bilayer of water, solvated protons in the water layer, and excess electrons in the metal surface. In this way we model the electrochemical double layer at a platinum electrode. By varying the number of protons/electrons in the double layer we investigate the system as a function of the electrode potential. We study the elementary processes involved in the hydrogen evolution reaction, 2(H(+) + e(-)) --> H(2), and determine the activation energy and predominant reaction mechanism as a function of electrode potential. We confirm by explicit calculations the notion that the variation of the activation barrier with potential can be viewed as a manifestation of the Brønsted-Evans-Polanyi-type relationship between activation energy and reaction energy found throughout surface chemistry.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Algorithms*
  • Cations
  • Electrochemistry
  • Electrodes
  • Hydrogen / chemistry*
  • Models, Theoretical*
  • Platinum / chemistry*
  • Protons*
  • Solvents / chemistry
  • Thermodynamics
  • Water / chemistry

Substances

  • Cations
  • Protons
  • Solvents
  • Water
  • Platinum
  • Hydrogen