Real-time elucidation of catalytic pathways in CO hydrogenation on Ru

Journal Article · 30 July 2017 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.7b01549 · OSTI ID:1373419

LaRue, Jerry ^[1]; Krejci, Ondrej ^[2]; Yu, Liang ^[3]; Beye, Martin ^[4]; Ng, May Ling ^[5]; Oberg, Henrik ^[6]; Xin, Hongliang ^[3]; Mercurio, Giuseppe ^[7]; Moeller, Stefan P. ^[5]; Turner, Joshua J. ^[5]; Nordlund, Dennis ^[5]; Coffee, Ryan ^[5]; Minitti, Michael P. ^[5]; Wurth, Wilfried ^[8]; Pettersson, Lars G. M. ^[6]; Ostrom, Henrik ^[6]; Nilsson, Anders ^[6]; Abild-Pedersen, Frank ^[5]; Ogasawara, Hirohito ^[9]

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1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stockholm Univ., Stockholm (Sweden); Chapman Univ., Orange, CA (United States); Fritz-Haber Institute of the Max-Planck-Society, Berlin (Germany)
2. Stockholm Univ., Stockholm (Sweden); Charles Univ. in Prague, Prague (Czech Republic); Institute of Physics of the Czech Academy of Sciences, Prague (Czech Republic)
3. Stanford Univ., Stanford, CA (United States)
4. Helmholtz Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany)
5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
6. Stockholm Univ., Stockholm (Sweden)
7. Univ. of Hamburg and Center for Free Electron Laser Science, Hamburg (Germany)
8. Univ. of Hamburg and Center for Free Electron Laser Science, Hamburg (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
9. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)

Here, the direct elucidation of the reaction pathways in heterogeneous catalysis has been challenging due the short-lived nature of reaction intermediates. Here, we directly measured on ultrafast timescales the initial hydrogenation steps of adsorbed CO on a Ru catalyst surface, which is known as the bottleneck reaction in syngas and CO₂ reforming processes. We initiated the hydrogenation of CO with an ultrafast laser temperature jump and probed transient changes in the electronic structure using real-time x-ray spectroscopy. In combination with theoretical simulations, we verified the formation of CHO during CO hydrogenation.

• Research Organization: SLAC National Accelerator Lab., Menlo Park, CA (United States)
• Sponsoring Organization: USDOE
• Grant/Contract Number: AC02-76SF00515
• OSTI ID: 1373419
• Journal Information: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Vol. 8; ISSN 1948-7185
• Publisher: American Chemical SocietyCopyright Statement
• Country of Publication: United States
• Language: English