Mesoscopic Modeling of Chemical Surface
Reactions
Reactions
such as those encountered in heterogeneous catalysis form a specific class
of non-equilibrium, nonlinear systems: they take place on low-dimensional
supports, the surfaces, exhibiting a particularly restricted geometry.
Because of this geometrical restriction, fluctuation-induced nanometric
self-organization can spontaneously arise and can lead to a
compartmentalization of the reactants and the products. We use mesoscopic
stochastic simulations and theoretical approaches to model the dynamics at
these scales and to understand the connection between the microscopic
details of the processes and the macroscopic rate laws for concentrations.
In particular, we study the propagation of waves, the emergence of
coherent oscillatory and explosive behaviors and apply these techniques
for the modeling of experimental systems such as the
H2+O2/Rh reaction with co-adsorbed potassium or the
NO+H2 reaction on platinum.
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PEEM-image of the hydrogen-oxygen
reaction on Rhodium in the presence of potassium. Bright regions
correspond to high K coverages.
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Numerical integration of a simple
surface anihilation model with an additional promoter species.
Regions which are richer in the promoter appear
brighter.
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Kinetic Monte Carlo simulation showing
the spatiotemporal development of a "surface explosion" during the
reduction of NO by hydrogen on Pt. NO particles appear black, H
appears grey and empty surface sites are blank.
References:
- Y. De Decker and A. S. Mikhailov, "Nanoscale Pattern Formation
in Surface Reactions", Progress of Theoretical
Physics – Supplements 165, 119-143 (2006).
- Y. De Decker and A. S. Mikhailov,
"Promoter-Induced Nonlinear Pattern Formation in Surface Chemical Reactions ",
Journal of Physical Chemistry B 108 (38),14759-14765 (2004).
- Y. De Decker, H. Marbach, M. Hinz,
S. Günther, M. Kiskinova, A. S. Mikhailov, and R. Imbihl,"Promoter-Induced
Reactive Phase Separation in Surface Reactions", Physical Review
Letters, 92 , p 198305(1)-198305(4) (2004)
- Y. De Decker, G. A. Tsekouras, A.
Provata, Th. Erneux and G. Nicolis, "Propagating
waves in one-dimensional discrete networks of coupled units", Physical
Review E, 69 , 036203 (2004).
- Y. De Decker, F. Baras, N. Kruse and G.
Nicolis, "Modeling the NO + H2 reaction on a Pt field emitter
tip: Mean-field analysis and Monte Carlo simulations", Journal of Chemical
Physics, 117 , p.10244-10257 (2002).
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