(345h) Adsorption Energies On Transition Metal Compounds With Varying Degree of Electron Localization: The Effect of gga+u

Computational screening for novel catalytic materials such as transition metal carbides, nitrides, sulfides, or oxides may be a key technology for the development of more energy- and resource-efficient catalytic processes. Many transition metal compounds containing less-precious metals than many conventional catalysts have unique physical and thermochemical properties. However, except transition metal oxides, only a few of these materials find industrial application as heterogeneous catalysts such as iron carbides for Fischer-Tropsch synthesis or iron nitrides for the Haber-Bosch process for instance. The catalytic properties of a large fraction of these materials have not been studied systematically.

Utilizing the adsorption energy of carbon monoxide as probe adsorbate, this work studies the catalytic activity of carbides, nitride, sulfide, or oxide surfaces of scandium with relatively high or molybdenum with relatively low electronic localization respectively. The presented generalized gradient approximation-based electronic-structure calculations are performed with or without fitting the band gap of the studied materials (except for Mo₂C or Mo₂N conductors) via Hubbard-U band structure methods. The computed adsorption energies are compared to the experimental literature to assess accuracy or limitations of these methods for quantitative screening of adsorption energy trends on binary transition metal compounds or complex materials classes such oxycarbides or oxynitrides in the future.