Dissertation

Development of highly accurate density functionals for H2 dissociation on transition metals

Metals surfaces form a group of effective catalysts for the reaction of small molecules such as hydrogen (H2).

Author

Smeets, E.W.F.

Date

29 June 2021

Links

Thesis in Leiden Repository

Metals surfaces form a group of effective catalysts for the reaction of small molecules such as hydrogen (H2). In order to improve the predictive power of theory with respect to the catalytic activity of small molecules reacting at metal surfaces, the way in which metal surfaces modify the potential energy of molecules needs to be understood at a fundamental level. Currently density functional theory (DFT) is the only electronic structure method that is accurate enough to achieve chemical accuracy while being cheap enough to make large comparative studies feasible. The work in this thesis is concerned with the creation of highly accurate density functionals that can give a simultaneously good description of the metal surface, the molecule, and the molecule interacting with the metal surface, as well as the description and simulation of supersonic molecular beam experiments and associative desorption experiments needed to validate the obtained results.

• associative desorption
• density functional theory
• generalized gradient approximation
• meta generalized gradient approximation
• molecular beam
• non-local correlation
• quantum dynamics
• quasi-classical trajectory method
• specific reaction parameter density functionals
• transition metal surfaces