First-principles approach to in-situ model catalyst studies

• Applicant: Professor Dr. Karsten Reuter
• Subject Area: Theoretical Chemistry: Molecules, Materials, Surfaces ; Chemical and Thermal Process Engineering ; Physical Chemistry of Solids and Surfaces, Material Characterisation
• Term: from 2013 to 2017
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 235493617

• Final Report Year: 2018

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
  
• “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
  
• “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