We have developed a method to couple kinetic Monte Carlo simulations of surface reactions at a molecular scale to transport equations at a macroscopic scale. This method is applicable to steady state reactors. We use a finite difference upwinding scheme and a gap-tooth scheme to efficiently use a limited amount of kinetic Monte Carlo simulations. In general the stochastic kinetic Monte Carlo results do not obey mass conservation so that unphysical accumulation of mass could occur in the reactor. We have developed a method to perform mass balance corrections that is based on a stoichiometry matrix and a least-squares problem that is reduced to a non-singular set of linear equations that is applicable to any surface catalyzed reaction. The implementation of these methods is validated by comparing numerical results of a reactor simulation with a unimolecular reaction to an analytical solution. Furthermore, the method is applied to two reaction mechanisms. The first is the ZGB model for CO oxidation in which inevitable poisoning of the catalyst limits the performance of the reactor. The second is a model for the oxidation of NO on a Pt(111) surface, which becomes active due to lateral interaction at high coverages of oxygen. This reaction model is based on ab initio density functional theory calculations from literature.
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7 February 2013
Research Article|
February 01 2013
Coupling of kinetic Monte Carlo simulations of surface reactions to transport in a fluid for heterogeneous catalytic reactor modeling
C. Schaefer;
C. Schaefer
a)
Eindhoven University of Technology
, P.O. Box 513, 5600 MB Eindhoven, The Netherlands
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A. P. J. Jansen
A. P. J. Jansen
b)
Eindhoven University of Technology
, P.O. Box 513, 5600 MB Eindhoven, The Netherlands
Search for other works by this author on:
a)
Electronic mail: [email protected].
b)
Electronic mail: [email protected].
J. Chem. Phys. 138, 054102 (2013)
Article history
Received:
November 06 2012
Accepted:
January 11 2013
Citation
C. Schaefer, A. P. J. Jansen; Coupling of kinetic Monte Carlo simulations of surface reactions to transport in a fluid for heterogeneous catalytic reactor modeling. J. Chem. Phys. 7 February 2013; 138 (5): 054102. https://doi.org/10.1063/1.4789419
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