A combined molecular dynamics–ab initio study of H2 adsorption on ideal, relaxed, and temperature-reconstructed MgO(111) surfaces

2D periodic ab initio calculations have been performed for H2 interacting with a temperature-reconstructed MgO(111) surface, created from a molecular dynamics (MD) simulation at 300 K. The temperature effects involve both a long-time reconstruction of the surface and instantaneous vibrational displacements. Chemisorption energies of ∼60 μJ/mol were found. Comparisons with adsorption on ideal and relaxed MgO(111) slabs show that the physi- and chemisorption properties for the H2/MgO(111) system are very sensitive to small topological details in the surface structure. The large surface reconstruction at 300 K involves drastic changes of the surface’s adsorption properties. We also find that a low coordination number of the surface ions is not sufficient to make the site attractive for chemisorption.