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Evidence for the Active Phase of Heterogeneous Catalysts through In Situ Reaction Product Imaging and Multiscale Modeling

Matera, S.; Blomberg, Sara LU ; Hoffmann, M. J.; Zetterberg, Johan LU ; Gustafson, Johan LU ; Lundgren, Edvin LU and Reuter, K. (2015) In ACS Catalysis 5(8). p.4514-4518
Abstract
We use multiscale modeling to analyze laser-induced fluorescence (LIP) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density functional theory-based kinetic Monte Carlo simulations of the active catalyst into fluid-dynamical simulations of the mass transport inside the reactor chamber, we calculate the reaction product concentration directly above the catalyst surface. Comparing corresponding data calculated for different surface models against the measured LIP signals, we can discriminate the one that predominantly actuates the experimentally measured catalytic activity. For the probed CO oxidation reaction conditions, the experimental activity is due to pristine Pd(100) possibly... (More)
We use multiscale modeling to analyze laser-induced fluorescence (LIP) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density functional theory-based kinetic Monte Carlo simulations of the active catalyst into fluid-dynamical simulations of the mass transport inside the reactor chamber, we calculate the reaction product concentration directly above the catalyst surface. Comparing corresponding data calculated for different surface models against the measured LIP signals, we can discriminate the one that predominantly actuates the experimentally measured catalytic activity. For the probed CO oxidation reaction conditions, the experimental activity is due to pristine Pd(100) possibly coexisting with other (oxidic) domains on the surface. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
multiscale modeling, laser-induced fluorescence, oxidation reaction over, Pd(100), catalytic activity, in-situ spectroscopy, density-functional, theory
in
ACS Catalysis
volume
5
issue
8
pages
4514 - 4518
publisher
The American Chemical Society
external identifiers
  • wos:000359395100004
  • scopus:84938723310
ISSN
2155-5435
DOI
10.1021/acscatal.5b00858
language
English
LU publication?
yes
id
6482fa86-ab06-414b-bbce-6e47b92bcea3 (old id 7975508)
date added to LUP
2015-09-24 14:40:38
date last changed
2017-11-12 03:36:17
@article{6482fa86-ab06-414b-bbce-6e47b92bcea3,
  abstract     = {We use multiscale modeling to analyze laser-induced fluorescence (LIP) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density functional theory-based kinetic Monte Carlo simulations of the active catalyst into fluid-dynamical simulations of the mass transport inside the reactor chamber, we calculate the reaction product concentration directly above the catalyst surface. Comparing corresponding data calculated for different surface models against the measured LIP signals, we can discriminate the one that predominantly actuates the experimentally measured catalytic activity. For the probed CO oxidation reaction conditions, the experimental activity is due to pristine Pd(100) possibly coexisting with other (oxidic) domains on the surface.},
  author       = {Matera, S. and Blomberg, Sara and Hoffmann, M. J. and Zetterberg, Johan and Gustafson, Johan and Lundgren, Edvin and Reuter, K.},
  issn         = {2155-5435},
  keyword      = {multiscale modeling,laser-induced fluorescence,oxidation reaction over,Pd(100),catalytic activity,in-situ spectroscopy,density-functional,theory},
  language     = {eng},
  number       = {8},
  pages        = {4514--4518},
  publisher    = {The American Chemical Society},
  series       = {ACS Catalysis},
  title        = {Evidence for the Active Phase of Heterogeneous Catalysts through In Situ Reaction Product Imaging and Multiscale Modeling},
  url          = {http://dx.doi.org/10.1021/acscatal.5b00858},
  volume       = {5},
  year         = {2015},
}