Matera, S. and Meskine, H. and Reuter, K. (2011) Adlayer inhomogeneity without lateral interactions: Rationalizing correlation effects in CO oxidation at RuO2(110) with firstprinciples 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 meanfield 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 firstprinciples kinetic Monte Carlo simulations and the CO oxidation at RuO2(110) as a showcase, we demonstrate that even in this limit meanfield 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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