1995/08/24 by J. Goniakowski, M. J. Gillan, M.J. Gillan · 233 citations
Energy · Materials Science · Physics and Astronomy · #Adsorption #Catalytic Processes in Materials Science #Chemical and Physical Properties of Materials #Chemisorption #Density functional theory #Desorption #Dissociation (chemistry) #Pseudopotential #Relaxation (psychology) #Thermal desorption #TiO2 Photocatalysis and Solar Cells #cond-mat.mtrl-sci #mtrl-th
paper · pdf · doi:10.1016/0039-6028(95)01252-4
published in Surface Science 350(1-3), 145-158 (Elsevier BV)
arxiv created 1995/08/24 · openalex publication_date 1996/04/01 · arxiv updated 2009/11/30 · openalex created_date 2016/06/24 · openalex updated_date 2026/08/05
First-principles calculations based on density functional theory and the pseudopotential method have been used to investigate the energetics of H2O adsorption on the (110) surface of TiO2 and SnO2. Full relaxation of all atomic positions is performed on slab systems with periodic boundary conditions, and the cases of full and half coverage are studied. Both molecular and dissociative (H2O → OH- + H+) adsorption are treated, and allowance is made for relaxation of the adsorbed species to unsymmetrical configurations. It is found that for both TiO2 and SnO2 an unsymmetrical dissociated configuration is the most stable. The symmetrical molecularly adsorbed configuration is unstable with respect to lowering of symmetry, and is separated from the fully dissociated configuration by at most a very small energy barrier. The calculated dissociative adsorption energies for TiO2 and SnO2 are in reasonable agreement with the results of thermal desorption experiments. Calculated total and local electronic densities of states for dissociatively and molecularly adsorbed configurations are presented and their relation with experimental UPS spectra is discussed.