Dissertation

Highly Accurate Simulations and Benchmarking of Molecule-Surface Reactions

Heterogeneous catalyzed processes are highly significant to the chemical industry. Dissociative chemisorption (DC) of molecules on surfaces is always considered as a step with a high degree of rate control for heterogeneous catalysis.

Author

T. Tchakoua

Date

04 July 2023

Links

Thesis in Leiden Repository

Our ability to comprehend the different mechanisms underlying DC on metal surfaces could benefit significantly from the availability of an accurate database for the barrier heights of elementary molecule-metal surface reactions. In this work, we used a recent implementation of specific reaction parameter (SRP) to density-functional theory (DFT) (SRP-DFT) to develop potential energy surfaces (PESs) for molecule-surface reactions. The PESs were used for molecular beam simulations and compared with molecular beam experiments. The barrier heights extracted from these PESs are now used for benchmarking.

• density functional theory
• heterogeneous catalysis
• molecular beam
• quantum dynamics
• quasi-classical trajectory method
• specific reaction parameter density functionals