First-principles kinetic Monte Carlo simulations for heterogeneous catalysis : Application to the Co oxidation at RuO2(110)
By Karsten Reuter, Matthias Scheffler. 2005
272 citations recorded by the source corpus.
We describe a first-principles statistical mechanics approach enabling us to simulate the steady-state situation of heterogeneous catalysis. In a first step, density-functional theory together with transition-state theory is employed to obtain the energetics of the relevant elementary processes. Subsequently the statistical mechanics problem is solved by the kinetic Monte Carlo method, which accounts for the correlations, fluctuations, and spatial distributions of the chemicals at the surface of the catalyst under steady-state conditions. Applying this approach to the catalytic oxidation of CO at RuO2110, we determine the surface atomic structure and composition in reactive environments ranging from ultra-high vacuum UHV to technologically relevant conditions, i.e., up to pressures of several atmospheres and elevated temperatures. We also compute the CO2 formation rates turnover frequencies. The results are in quantitative agreement with all existing experimental data. We find that the high catalytic activity of this system is intimately connected with a disordered, dynamic surface “phase” with significant compositional fluctuations. In this active state the catalytic function results from a self-regulating interplay of several elementary processes.
Subfields: Atomic and Molecular Physics, and Optics, Catalysis, Materials Chemistry
View Paper: https://www.semanticscholar.org/paper/daef7f1fa3af90b360d9282bb7133b75bf0281a5
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In Atomic and Molecular Physics, and Optics
In Catalysis
In Materials Chemistry
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- Thomas Bligaard
- Jeff Greeley
- B. Roldán Cuenya
- S. Qiao
- Yao Zheng
- Y. Jiao
- M. Mavrikakis
Citations in the corpus
- CatMAP: A Software Package for Descriptor-Based Microkinetic Mapping of Catalytic Trends (2015, background): “There are different levels of kinetic modeling, varying in complexity from mean-field models with a single rate-determining step to stochastic simulations such as kinetic Monte Carlo [1–6].”