Kinetic Monte Carlo simulation of the preferential oxidation of CO using normally distributed rate probabilities

Sichem Guerrero, E. E. Wolf

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4 Scopus citations

Abstract

This study presents results from a Kinetic Monte Carlo (KMC) simulation of the catalytic preferential oxidation of CO reaction (PROX) on 3D Pt crystallites. A new method of constructing normal distributions of event probabilities is presented based on the log transformation of calculated kinetic rates (log-KMC). This method allows for solving problems where the time scales of particular events are very different (stiff problems) and it was applied to the simulation of the PROX reaction on supported Pt catalysts to probe the experimental results on a catalyst with different crystallite sizes. It was found that the simulation replicated the trends from experimental results when it was assumed that the limiting step of the PROX reaction was oxygen adsorption. Lower Pt dispersions gave place to catalysts showing higher turnover frequencies, or TOF, which is due to large crystallites having lower numbers of less active base sites. This limiting effect is simulated in larger crystallite sizes with more available sites on (1. 1. 1) faces.

Original languageEnglish
Pages (from-to)4477-4487
Number of pages11
JournalChemical Engineering Science
Volume66
Issue number20
DOIs
StatePublished - 15 Oct 2011
Externally publishedYes

Bibliographical note

Funding Information:
The support of this work by a Bayer Postdoctoral Fellowship in Environmental Chemistry through the Center for Environmental Science and Technology at the University of Notre Dame is gratefully acknowledged. The authors thank Prof. Francisco Gracia from the Chemical Engineering Department of Universidad de Chile for his interest and technical advice during this project.

Keywords

  • Crystallite size effects
  • Heterogeneous catalysis
  • Monte Carlo
  • PROX reaction
  • Stiff problems
  • Surface reactions

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