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

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

doi:10.1126/science.1261747

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

Science. 2015 Feb 27;347(6225):978-82. doi: 10.1126/science.1261747. Epub 2015 Feb 12.

Authors

H Öström¹, H Öberg¹, H Xin², J LaRue³, M Beye⁴, M Dell'Angela⁵, J Gladh¹, M L Ng², J A Sellberg⁶, S Kaya², G Mercurio⁵, D Nordlund⁷, M Hantschmann⁸, F Hieke⁵, D Kühn⁸, W F Schlotter⁹, G L Dakovski⁹, J J Turner⁹, M P Minitti⁹, A Mitra⁹, S P Moeller⁹, A Föhlisch¹⁰, M Wolf¹¹, W Wurth¹², M Persson¹³, J K Nørskov³, F Abild-Pedersen², H Ogasawara⁷, L G M Pettersson¹, A Nilsson¹⁴

Affiliations

¹ Department of Physics, AlbaNova University Center, Stockholm University, SE-10691, Sweden.
² SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
³ SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA. SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA 95305, USA.
⁴ SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA. Helmholtz Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany.
⁵ Physics Department and Center for Free Electron Laser Science, University of Hamburg, Luruper Chausse 149, D-22761 Hamburg, Germany.
⁶ Department of Physics, AlbaNova University Center, Stockholm University, SE-10691, Sweden. SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
⁷ Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
⁸ Helmholtz Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany.
⁹ Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA.
¹⁰ Helmholtz Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany. Fakultät für Physik und Astronomie, Universität Potsdam, Karl-Liebknecht-Strasse 24-25, 14476 Potsdam, Germany.
¹¹ Fritz-Haber Institute of the Max-Planck-Society, Faradayweg 4-6, D-14195 Berlin, Germany.
¹² Physics Department and Center for Free Electron Laser Science, University of Hamburg, Luruper Chausse 149, D-22761 Hamburg, Germany. Deutsches Elektronen-Synchrotron, Photon Science, Notkestrasse 85, D-22607 Hamburg, Germany.
¹³ Surface Science Research Centre and Department of Chemistry, The University of Liverpool, Liverpool, L69 3BX, UK.
¹⁴ Department of Physics, AlbaNova University Center, Stockholm University, SE-10691, Sweden. SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA. Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA. nilsson@slac.stanford.edu.

PMID: 25722407
DOI: 10.1126/science.1261747

Abstract

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.

Publication types

Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.