Chemically Accurate Simulation of a Prototypical Surface Reaction: H₂ Dissociation on Cu(111)

• Published in: Science (American Association for the Advancement of Science) Vol. 326; no. 5954; pp. 832 - 834
• Main Authors: Díaz, C, Pijper, E, Olsen, R.A, Busnengo, H.F, Auerbach, D.J, Kroes, G.J
• Format: Journal Article
• Language: English
• Published: Washington, DC American Association for the Advancement of Science 06.11.2009; The American Association for the Advancement of Science
• Subjects: Catalysis; Chemistry; Copper; Degrees of freedom; Energy; Energy value; Exact sciences and technology; Experimental data; General and physical chemistry; Hydrogen; Inelastic scattering; Metal surfaces; Molecules; Phonons; Rotation; Rotational states; Surface physical chemistry; Surface reactions; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry; Potential energy; Surface reaction; Hydrogen; Transition metal; Crystal face; Functional theory; Heterogeneous catalysis; Density functional; Adsorption; Inelastic scattering; Simulation; Dynamics; Potential surface; Calculation; Dissociation; Copper
• ISSN: 0036-8075; 1095-9203
• DOI: 10.1126/science.1178722

Methods for accurately computing the interaction of molecules with metal surfaces are critical to understanding and thereby improving heterogeneous catalysis. We introduce an implementation of the specific reaction parameter (SRP) approach to density functional theory (DFT) that carries the method forward from a semiquantitative to a quantitative description of the molecule-surface interaction. Dynamics calculations on reactive scattering of hydrogen from the copper (111) surface using an SRP-DFT potential energy surface reproduce data on the dissociative adsorption probability as a function of incidence energy and reactant state and data on rotationally inelastic scattering with chemical accuracy (within approximately 4.2 kilojoules per mole).