Microkinetic Modeling and Simulation

Research directions

(FWF funded projects: SFB TACO, OEAD)

The developments in operando methodology enable to relate the catalyst state to its performance under reactive conditions. However, in many cases the interpretation and verification of the obtained experimental spectra/images/patterns relies on theoretical support, e.g. by calculating structures, adsorption and activation energies for single crystal surfaces, nanoparticles and clusters, complemented by micro-kinetic reaction modelling. Clearly, if calculations are performed for realistic gas pressures (coverage) and temperatures, they are even more relevant for operando studies.

Group members

Dr. Alexander Genest (Postdoc)
Parinya Tangpakonsab, PhD Student
Prof. Notker Roesch (Guest Scientist)

Collaboration Partners

Prof. Henrik Grönbeck, opens an external URL in a new window (Centre for Catalysis and Department of Applied Physics, Chalmers University of Technology, Gothenburg, Sweden): DFT calculations of the structure and adsorption/reactions on metal, oxide and metal-oxide surfaces and interfaces; microkinetic modeling of kinetic phase diagrams and oscillatory reactions

Prof. Dr. Dr.h.c. Notker Rösch, opens an external URL in a new window, FRSC (Department Chemie, Technische Universität München TUM, Garching, Germany): DFT and microkinetic modeling of isomerisation/hydrogeantion on model catalysts

Prof. Konstantin Neyman, opens an external URL in a new window (Departament de Química Física & Institut de Química Teòrica i Computacional (IQTC-UB), Universitat de Barcelona, Spain): DFT calculations of the structure and adsorption/reactions on bimetallic surfaces

Dr. Sergey M. Kozlov, opens an external URL in a new window (King Abdullah University of Science and Technology (KAUST), Saudi Arabia): DFT studies of CO adsorption on Cu clusters, steps and terraces

Prof. Peter Blaha, opens an external URL in a new window (IMC, TU Wien): DFT studies CO adsorption on metals and oxides

Publications

Active sites and deactivation of room temperature CO oxidation on Co3O4 catalysts: Combined experimental and computational investigations
Nevzat Yigit, Alexander Genest, Schamil Terloev, Jury Möller, Günther Rupprechter
Journal of Physics: Condensed Matter, 34 (2022) 354001 (10pp)
https://doi.org/10.1088/1361-648X/ac718b , opens an external URL in a new window

CO Adsorption and Disproportionation on Smooth and Defect-Rich Ir(111)
Xia Li, Thomas Haunold, Stefan Werkovits, Laurence D. Marks, Peter Blaha, Günther Rupprechter
Journal of Physical Chemistry C, 126 (2022) 6578–6589
https://doi.org/10.1021/acs.jpcc.2c01141, opens an external URL in a new window

The origin of the particle-size-dependent selectivity in 1-butene isomerization and hydrogenation on Pd/Al2O3 catalysts
A. Genest, J. Silvestre-Albero, W.-Q. Li, N. Rösch, G. Rupprechter
Nature Communications 12 (2021) 6098  (8 pages)
DOI: https://doi.org/10.1038/s41467-021-26411-8, opens an external URL in a new window

High-performance water gas shift induced by asymmetric oxygen vacancies: gold clusters supported by ceria-praseodymia mixed oxides
J. Shi, H. Li, A. Genest, W. Zhao, P. Qi, T. Wang, G. Rupprechter
Applied Catalysis B: Environmental, 301 (2022) 120789 (13 pages)
DOI: https://doi.org/10.1016/j.apcatb.2021.120789, opens an external URL in a new window

Catalytic transformations of 1-Butene over palladium. A combined experimental and theoretical studyV. Markova, J. Philbin, W. Zhao, A. Genest, J. Silvestre-Albero, G. Rupprechter, N. Rösch
ACS Catalysis 8 (2018) 5675-5685
DOI: https://doi.org/10.1021/acscatal.8b01013, opens an external URL in a new window

Recently studied topics

  • Acive sites and (deactovation) mechanism of romm temperature CO oxidation on Co3O4: Journal of Physics: Condensed Matter, 34 (2022) 354001
  • DFT calculations and microkinetic modeling of atmospheric pressure reaction kinetics of 1-butene hydrogenation/isomerization on Pd/Al2O3 model catalysts: Nature Communications, 12 (2021) 6098
  • DFT modeling of the formation energy of oxygen vacancies, the binding energy of water, and the asymmetry of the O# site, explaining the effects on WGS on Au clusters supported by CePrOx mixed oxides: Applied Catalysis B: Enironmental, 301 (2022) 120789 in press
  • 1-butene isomerization/hydrogenation on Pd single crystals (LEED, batch reactor kinetics (GC), DFT, mikrokinetic modeling) ACS Catalysis 8 (2018) 5675-5685