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“First-Principles” kinetic monte carlo simulations revisited: CO oxidation over RuO2(110)


Hess, Franziska; Farkas, Attila; Seitsonen, Ari P; Over, Herbert (2012). “First-Principles” kinetic monte carlo simulations revisited: CO oxidation over RuO2(110). Journal of Computational Chemistry, 33(7):757-766.

Abstract

First principles-based kinetic Monte Carlo (kMC) simulations are performed for the CO oxidation on RuO2(110) under steady-state reaction conditions. The simulations include a set of elementary reaction steps with activation energies taken from three different ab initio density functional theory studies. Critical comparison of the simulation results reveals that already small variations in the activation energies lead to distinctly different reaction scenarios on the surface, even to the point where the dominating elementary reaction step is substituted by another one. For a critical assessment of the chosen energy parameters, it is not sufficient to compare kMC simulations only to experimental turnover frequency (TOF) as a function of the reactant feed ratio. More appropriate benchmarks for kMC simulations are the actual distribution of reactants on the catalyst's surface during steady-state reaction, as determined by in situ infrared spectroscopy and in situ scanning tunneling microscopy, and the temperature dependence of TOF in the from of Arrhenius plots. (c) 2012 Wiley Periodicals, Inc.

Abstract

First principles-based kinetic Monte Carlo (kMC) simulations are performed for the CO oxidation on RuO2(110) under steady-state reaction conditions. The simulations include a set of elementary reaction steps with activation energies taken from three different ab initio density functional theory studies. Critical comparison of the simulation results reveals that already small variations in the activation energies lead to distinctly different reaction scenarios on the surface, even to the point where the dominating elementary reaction step is substituted by another one. For a critical assessment of the chosen energy parameters, it is not sufficient to compare kMC simulations only to experimental turnover frequency (TOF) as a function of the reactant feed ratio. More appropriate benchmarks for kMC simulations are the actual distribution of reactants on the catalyst's surface during steady-state reaction, as determined by in situ infrared spectroscopy and in situ scanning tunneling microscopy, and the temperature dependence of TOF in the from of Arrhenius plots. (c) 2012 Wiley Periodicals, Inc.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:March 2012
Deposited On:18 Jan 2013 15:32
Last Modified:07 Dec 2017 15:21
Publisher:Wiley-Blackwell
ISSN:0192-8651
Publisher DOI:https://doi.org/10.1002/jcc.22902
Other Identification Number:ISI:000300502900005

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