An understanding and implications of the coverage of surface free sites in heterogeneous catalysis

Haifeng Wang, Yanglong Guo, Guanzhong Lu*, P. Hu

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

19 Citations (Scopus)

Abstract

The crucial roles of the coverage of surface free sites in determining catalytic activity trend are quantitatively addressed with the help of density functional theory and microkinetics. First, by analyzing activity trends of NO oxidation catalyzed by Ru, Rh, Pd, Os, Ir, and Pt surfaces with full kinetic considerations, we identify that the activity trend is in general determined by the competition between the reaction barrier and the coverage of surface free sites. Second, since the dissociation of many important molecules, such as the dissociation of N(2), O(2), and CO, follows the same Bronsted-Evans-Polanyi relationship, the coverage of surface free sites is usually a decisive term that affects the overall activity. Third, an equation is derived for the coverage of surface free sites and it is found that the coverage of surface free sites contains not only all the key thermodynamic parameters but also all the kinetic properties in the catalytic system. (C) 2009 American Institute of Physics. [DOI: 10.1063/1.3140202]

Original languageEnglish
Article number224701
Number of pages6
JournalJournal of Chemical Physics
Volume130
Issue number22
DOIs
Publication statusPublished - 14 Jun 2009

Keywords

  • DENSITY-FUNCTIONAL THEORY
  • EVANS-POLANYI RELATION
  • AMMONIA-SYNTHESIS
  • REACTOR DESIGN
  • METAL-SURFACES
  • VOLCANO CURVE
  • REDUCTION
  • NOX
  • MECHANISM
  • DISSOCIATION

Cite this