Repository: Freie Universit├Ąt Berlin, Math Department

Adlayer inhomogeneity without lateral interactions: Rationalizing correlation effects in CO oxidation at RuO2(110) with first-principles kinetic Monte Carlo

Matera, S. and Meskine, H. and Reuter, K. (2011) Adlayer inhomogeneity without lateral interactions: Rationalizing correlation effects in CO oxidation at RuO2(110) with first-principles kinetic Monte Carlo. The Journal of Chemical Physics, 134 (6). 064713.

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Abstract

Microkinetic modeling of surface chemical reactions still relies heavily on the mean-field based rate equation approach. This approach is expected to be most accurate for systems without appreciable lateral interactions among the adsorbed chemicals, and there in particular for the uniform adlayers resulting in poisoned regimes with predominant coverage of one species. Using first-principles kinetic Monte Carlo simulations and the CO oxidation at RuO2(110) as a showcase, we demonstrate that even in this limit mean-field rate equations fail to predict the catalytic activity by orders of magnitude. This deficiency is traced back to the inability to account for the vacancy pair formation that is kinetically driven by the ongoing reactions.

Item Type:Article
Subjects:Mathematical and Computer Sciences > Mathematics > Applied Mathematics
Divisions:Department of Mathematics and Computer Science > Institute of Mathematics > Geophysical Fluid Dynamics Group
ID Code:2018
Deposited By: Ulrike Eickers
Deposited On:17 Feb 2017 11:22
Last Modified:03 Mar 2017 14:42

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