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

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 CO 2 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.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [3] ;  [7] ;  [5] ;  [5] ;  [5] ;  [5] ;  [5] ;  [8] ;  [6] ;  [6] ;  [6] ;  [5] ;  [9]
  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)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1373419

LaRue, Jerry, Krejci, Ondrej, Yu, Liang, Beye, Martin, Ng, May Ling, Oberg, Henrik, Xin, Hongliang, Mercurio, Giuseppe, Moeller, Stefan P., Turner, Joshua J., Nordlund, Dennis, Coffee, Ryan, Minitti, Michael P., Wurth, Wilfried, Pettersson, Lars G. M., Ostrom, Henrik, Nilsson, Anders, Abild-Pedersen, Frank, and Ogasawara, Hirohito. Real-time elucidation of catalytic pathways in CO hydrogenation on Ru. United States: N. p., Web. doi:10.1021/acs.jpclett.7b01549.
LaRue, Jerry, Krejci, Ondrej, Yu, Liang, Beye, Martin, Ng, May Ling, Oberg, Henrik, Xin, Hongliang, Mercurio, Giuseppe, Moeller, Stefan P., Turner, Joshua J., Nordlund, Dennis, Coffee, Ryan, Minitti, Michael P., Wurth, Wilfried, Pettersson, Lars G. M., Ostrom, Henrik, Nilsson, Anders, Abild-Pedersen, Frank, & Ogasawara, Hirohito. Real-time elucidation of catalytic pathways in CO hydrogenation on Ru. United States. doi:10.1021/acs.jpclett.7b01549.
LaRue, Jerry, Krejci, Ondrej, Yu, Liang, Beye, Martin, Ng, May Ling, Oberg, Henrik, Xin, Hongliang, Mercurio, Giuseppe, Moeller, Stefan P., Turner, Joshua J., Nordlund, Dennis, Coffee, Ryan, Minitti, Michael P., Wurth, Wilfried, Pettersson, Lars G. M., Ostrom, Henrik, Nilsson, Anders, Abild-Pedersen, Frank, and Ogasawara, Hirohito. 2017. "Real-time elucidation of catalytic pathways in CO hydrogenation on Ru". United States. doi:10.1021/acs.jpclett.7b01549. https://www.osti.gov/servlets/purl/1373419.
@article{osti_1373419,
title = {Real-time elucidation of catalytic pathways in CO hydrogenation on Ru},
author = {LaRue, Jerry and Krejci, Ondrej and Yu, Liang and Beye, Martin and Ng, May Ling and Oberg, Henrik and Xin, Hongliang and Mercurio, Giuseppe and Moeller, Stefan P. and Turner, Joshua J. and Nordlund, Dennis and Coffee, Ryan and Minitti, Michael P. and Wurth, Wilfried and Pettersson, Lars G. M. and Ostrom, Henrik and Nilsson, Anders and Abild-Pedersen, Frank and Ogasawara, Hirohito},
abstractNote = {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.},
doi = {10.1021/acs.jpclett.7b01549},
journal = {Journal of Physical Chemistry Letters},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {7}
}