Journal article

Publication year: 2012

Pages: 757-766

Journal: Journal of Computational Chemistry

Volume number: 33

Issue number: 7

ISSN: 0192-8651

DOI Link: https://doi.org/10.1002/jcc.22902

Publisher: Wiley

Abstract: 
First principles-based kinetic Monte Carlo (kMC) simulations are performed for the CO oxidation on RuO(2) (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.

Harvard Citation style: Hess, F., Farkas, A., Seitsonen, A. and Over, H. (2012) "First-principles" kinetic Monte Carlo simulations revisited: CO oxidation over RuO2 (110)., Journal of Computational Chemistry, 33(7), pp. 757-766. https://doi.org/10.1002/jcc.22902

APA Citation style: Hess, F., Farkas, A., Seitsonen, A., & Over, H. (2012). "First-principles" kinetic Monte Carlo simulations revisited: CO oxidation over RuO2 (110).. Journal of Computational Chemistry. 33(7), 757-766. https://doi.org/10.1002/jcc.22902