Dynamics of H2 on Ti/Al(100) surfaces

Abstract

What is the catalytic role played by titanium in the hydrogen storage material NaAlH4? This thesis aims at unraveling the dynamics of an elementary reaction: H2 dissociation on Ti/Al(100) surfaces. Although this reaction is not the rate limiting step in the hydrogen storage of NaAlH4, it is an important reaction to produce atomic hydrogen for the other reaction steps. To achieve the stated goal, we test a large set of possible slab models to represent the Ti/Al(100) surface. After considering the stability of the slab model itself and the barrier height for H2 dissociation, we carefully select two possible slab models: (1) the 1/2 ML Ti-covered c(2 _ 2)-Ti/Al(100) surface with Ti atoms in the second layer, (2) the 1 ML Ti-covered c(2 _ 2)-Ti/Al(100) surface with Ti atoms in the first and third layers. Using these two slab models, potential energy surfaces (PES) are calculated. The H2 dissociation probabilities and rate constants are then calculated. The results suggest that the 1 ML Ti-covered c(2 _ 2)-Ti/Al(100) surface may be the most realistic model for H2 dissociation on Ti/Al(100) surfaces relevant for the hydrogen storage material NaAlH4. In this thesis, time-dependent wave packet, quasi-classical and classical dynamics, and transition state theory have been imployed to calculate the micro-canonical reaction probabilities and canonical reaction rate constants.