Adsorption energies on transition metal surfaces: towards an accurate and balanced description

Abstract Density functional theory predictions of binding energies and reaction barriers provide invaluable data for analyzing chemical transformations in heterogeneous catalysis. For high accuracy, effects of band structure and coverage, as well as the local bond strength in both covalent and non-covalent interactions, must be reliably described and much focus has been put on improving functionals to this end. Here, we show that a correction from higher-level calculations on small metal clusters can be applied to improve periodic band structure adsorption energies and barriers. We benchmark against 38 reliable experimental covalent and non-covalent adsorption energies and five activation barriers with mean absolute errors of 2.2 kcal mol −1 , 2.7 kcal mol −1 , and 1.1 kcal mol −1 , respectively, which are lower than for functionals widely used and tested for surface science evaluations, such as BEEF-vdW and RPBE.

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