Matera, S. and Maestri, M. and Cuoci, A. and Reuter, K. (2014) PredictiveQuality Surface Reaction Chemistry in Real Reactor Models: Integrating FirstPrinciples Kinetic Monte Carlo Simulations into Computational Fluid Dynamics. ACS Catalysis, 4 (11). pp. 40814092.

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Abstract
We present a numerical framework to integrate firstprinciples kinetic Monte Carlo (1pkMC) based microkinetic models into the powerful computational fluid dynamics (CFD) package CatalyticFoam. This allows for the simultaneous account of a predictivequality surface reaction kinetics inside an explicitly described catalytic reactor geometry. Crucial means toward an efficient and stable implementation are the exploitation of the disparate time scales of surface chemistry and gasphase transport, as well as the reliable interpolation of irregularly gridded 1pkMC data by means of an errorbased modified Shepard approach. We illustrate the capabilities of the framework using the CO oxidation at Pd(100) and RuO2(110) model catalysts in different reactor configurations and fluid dynamic conditions as showcases. These showcases underscore both the necessity and value of having reliable treatments of the surface chemistry and flow inside integrated multiscale catalysis simulations when aiming at an atomicscale understanding of the catalytic function in nearambient environments. Our examples highlight how intricately this function is affected by specifics of the reactor geometry and heat dissipation channels on the one end, and on the other end by characteristics of the intrinsic catalytic activity that are only captured by treatments beyond prevalent meanfield rate equations.
Item Type:  Article 

Uncontrolled Keywords:  CO oxidation; computational fluid dynamics; firstprinciples kinetic Monte Carlo; heterogeneous catalysis; multiscale modeling 
Subjects:  Mathematical and Computer Sciences > Mathematics > Applied Mathematics 
Divisions:  Department of Mathematics and Computer Science > Institute of Mathematics > Geophysical Fluid Dynamics Group 
ID Code:  2032 
Deposited By:  Ulrike Eickers 
Deposited On:  17 Feb 2017 11:21 
Last Modified:  03 Mar 2017 14:42 
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