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

Abstract

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.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [3];  [7];  [5];  [5];  [5];  [5];  [5];  [8];  [6];  [6];  [6];  [5];  [9]
+ Show Author Affiliations
  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:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1373419
Grant/Contract Number:  
AC02-76SF00515
Resource 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
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

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., 2017. Web. doi:10.1021/acs.jpclett.7b01549.
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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. https://doi.org/10.1021/acs.jpclett.7b01549
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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. Mon . "Real-time elucidation of catalytic pathways in CO hydrogenation on Ru". United States. https://doi.org/10.1021/acs.jpclett.7b01549. https://www.osti.gov/servlets/purl/1373419.
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@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 = {Mon Jul 31 00:00:00 EDT 2017},
month = {Mon Jul 31 00:00:00 EDT 2017}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jpclett.7b01549
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Cited by: 9 works
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Figures / Tables:

Figure 1 Figure 1: O K-edge XAS and XES data for CO hydrogenation. Solid or dotted lines represent the smoothed curve, and points represent true measured values from experiments. (a) The laser-induced desorption signal of m/e = 29 (CHO) and m/e = 30 (CH2O) from a (CO + H)/Ru(0001) surface. (b) Omore » K-edge XAS at negative delay for the unpumped system and at 1.5−2.0 ps after laser excitation, and simulated spectra for CO(ads) (black, solid), CHO(ads) (red, dot) and the transition state from CO(ads) to CHO(ads) (TS, blue, dashdot). Vertical bars represent the standard deviation of error depending on incoming photon energy. The inset shows a schematic illustration of the excitation process from the O1s level to the unoccupied 2π* resonance in XAS. (c) O K-edge XES excited with X-rays in the range between 530.2 and 533.0 eV at negative delay for the unpumped system (black) and at 0.0−3.0 ps after laser excitation (red). The inset shows a schematic illustration of the core hole decay process from occupied molecular orbitals back to the O1s in XES. (d) The intensity contrast in the X-ray absorption spectra integrated between 530.2 and 533.0 eV versus time delay. The constant error bar indicates the confidence limit of 1.5%, which corresponds to the standard deviation of peak-to-peak fluctuations of contrast at negative delay, in which Xray measurements were conducted without the laser excitation. Dashed line added as a guide to the eye.« less
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Real-Time Elucidation of Catalytic Pathways in CO Hydrogenation on Ru
text, January 2017

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