Dissertation
Getting the electrons right for O2-on-metal systems
This thesis studies theoretical surface chemistry within the field of heterogeneous catalysis.
- Author
- R.A.B. van Bree
- Date
- 21 October 2025
- Links
- Thesis in Leiden Repository
Heterogeneous catalysis is widely used in the chemical industry and ensures that many different chemical processes can run efficiently. Improving these catalytic processes makes the chemical industry more efficient, economical and cheaper. Such improvements are often still carried out on a trial and error basis. It would be ideal if improvements to catalysts could be guided by fundamental insights into the catalytic reaction. This is where a theoretical model, or computer simulation, of the chemistry on the surface of the catalyst can play a crucial role. The ideal model should describe and ultimately predict the behaviour of the catalyst.
This thesis presents new steps for improving existing models for the chemistry at catalyst surfaces. Specifically, we look at the interactions of oxygen on aluminium and copper surfaces. In these systems, the reactivity of oxygen is overestimated by virtually all common models, so the models require improvement. For oxygen on aluminium, we first present a new application of an existing model that reduces the required computational costs of that model by a factor of ten. Next, we present a new model, and although we see an improvement in reactivity, we still continue to overestimate it. However, for oxygen on copper, this same model is the first known model to underestimate the reactivity. This means that the reactivity of oxygen with copper can be simulated with high accuracy in the future.