Surface chemistry. Probing the transition state region in catalytic CO oxidation on Ru

Autor: H, Öström, H, Öberg, H, Xin, J, LaRue, M, Beye, M, Dell'Angela, J, Gladh, M L, Ng, J A, Sellberg, S, Kaya, G, Mercurio, D, Nordlund, M, Hantschmann, F, Hieke, D, Kühn, W F, Schlotter, G L, Dakovski, J J, Turner, M P, Minitti, A, Mitra, S P, Moeller, A, Föhlisch, M, Wolf, W, Wurth, M, Persson, J K, Nørskov, F, Abild-Pedersen, H, Ogasawara, L G M, Pettersson, A, Nilsson
Rok vydání: 2015
Zdroj: Science (New York, N.Y.). 347(6225)
ISSN: 1095-9203
Popis: Femtosecond x-ray laser pulses are used to probe the carbon monoxide (CO) oxidation reaction on ruthenium (Ru) initiated by an optical laser pulse. On a time scale of a few hundred femtoseconds, the optical laser pulse excites motions of CO and oxygen (O) on the surface, allowing the reactants to collide, and, with a transient close to a picosecond (ps), new electronic states appear in the O K-edge x-ray absorption spectrum. Density functional theory calculations indicate that these result from changes in the adsorption site and bond formation between CO and O with a distribution of OC-O bond lengths close to the transition state (TS). After 1 ps, 10% of the CO populate the TS region, which is consistent with predictions based on a quantum oscillator model.
Databáze: OpenAIRE