First-principles approach to in-situ model catalyst studies
Chemical and Thermal Process Engineering
Physical Chemistry of Solids and Surfaces, Material Characterisation
Final Report Abstract
The present project has provided important steps forwards in multiscale modeling of heterogeneous catalysis for problems with many reacting species. The 1p-kMC model developed during the first part of this work has uncovered very complex interaction effects and highlighted the importance of detailed modeling. In particular, it has shown that questions of relative stability between metallic and oxide terminations in oxidation catalysis can be strongly dependent on the detailed composition of the gas feeds. The second part of this work has produced a novel interpolation method which was proven clearly superior to existing methods for functions with the challenging characteristics of 1p-kMC-based reactivity maps. This development opens the way to employing the successful coupling approach developed by Matera et al. to more complex 1p-kMC models containing larger numbers of reactive species.
Publications
- “Synergistic Inhibition of Oxide Formation in Heterogeneous Catalysis: A First-Principles Kinetic Monte Carlo Study of NO + CO Oxidation at Pd(100)”, ACS Catal. 2016, 6, 5191–5197
J.M. Lorenzi, S. Matera, K. Reuter
(See online at https://doi.org/10.1021/acscatal.6b01344) - “Local-Metrics Error-Based Shepard Interpolation as Surrogate for Highly Non-Linear Material Models in High Dimensions”, J. Chem. Phys. 2017, 147, 164106
J.M. Lorenzi, T. Stecher, K. Reuter, S. Matera
(See online at https://doi.org/10.1063/1.4997286) - “Electrons to Reactors Multiscale Modelling: Catalytic CO Oxidation over RuO2 ”, ACS Catal. 2018, 8, 5002–5016
J.E. Sutton, J.M. Lorenzi, J.T. Krogel, Q. Xiong, S. Pannala, S. Matera, A. Savara
(See online at https://doi.org/10.1021/acscatal.8b00713)
