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Stroboscopic operando spectroscopy of the dynamics in heterogeneous catalysis by event-averaging

Knudsen, Jan LU ; Gallo, Tamires LU ; Boix, Virgínia LU ; Strømsheim, Marie Døvre ; D’Acunto, Giulio LU ; Goodwin, Christopher ; Wallander, Harald LU ; Zhu, Suyun LU ; Soldemo, Markus and Lömker, Patrick , et al. (2021) In Nature Communications 12(1).
Abstract

Heterogeneous catalyst surfaces are dynamic entities that respond rapidly to changes in their local gas environment, and the dynamics of the response is a decisive factor for the catalysts’ action and activity. Few probes are able to map catalyst structure and local gas environment simultaneously under reaction conditions at the timescales of the dynamic changes. Here we use the CO oxidation reaction and a Pd(100) model catalyst to demonstrate how such studies can be performed by time-resolved ambient pressure photoelectron spectroscopy. Central elements of the method are cyclic gas pulsing and software-based event-averaging by image recognition of spectral features. A key finding is that at 3.2 mbar total pressure a metallic,... (More)

Heterogeneous catalyst surfaces are dynamic entities that respond rapidly to changes in their local gas environment, and the dynamics of the response is a decisive factor for the catalysts’ action and activity. Few probes are able to map catalyst structure and local gas environment simultaneously under reaction conditions at the timescales of the dynamic changes. Here we use the CO oxidation reaction and a Pd(100) model catalyst to demonstrate how such studies can be performed by time-resolved ambient pressure photoelectron spectroscopy. Central elements of the method are cyclic gas pulsing and software-based event-averaging by image recognition of spectral features. A key finding is that at 3.2 mbar total pressure a metallic, predominantly CO-covered metallic surface turns highly active for a few seconds once the O2:CO ratio becomes high enough to lift the CO poisoning effect before mass transport limitations triggers formation of a √5 oxide.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
12
issue
1
article number
6117
publisher
Nature Publishing Group
external identifiers
  • scopus:85117736508
  • pmid:34675205
ISSN
2041-1723
DOI
10.1038/s41467-021-26372-y
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2021, The Author(s).
id
383c5b8f-3583-44a7-95db-c5e294bbb940
date added to LUP
2021-11-05 10:08:53
date last changed
2024-06-15 19:47:10
@article{383c5b8f-3583-44a7-95db-c5e294bbb940,
  abstract     = {{<p>Heterogeneous catalyst surfaces are dynamic entities that respond rapidly to changes in their local gas environment, and the dynamics of the response is a decisive factor for the catalysts’ action and activity. Few probes are able to map catalyst structure and local gas environment simultaneously under reaction conditions at the timescales of the dynamic changes. Here we use the CO oxidation reaction and a Pd(100) model catalyst to demonstrate how such studies can be performed by time-resolved ambient pressure photoelectron spectroscopy. Central elements of the method are cyclic gas pulsing and software-based event-averaging by image recognition of spectral features. A key finding is that at 3.2 mbar total pressure a metallic, predominantly CO-covered metallic surface turns highly active for a few seconds once the O<sub>2</sub>:CO ratio becomes high enough to lift the CO poisoning effect before mass transport limitations triggers formation of a √5 oxide.</p>}},
  author       = {{Knudsen, Jan and Gallo, Tamires and Boix, Virgínia and Strømsheim, Marie Døvre and D’Acunto, Giulio and Goodwin, Christopher and Wallander, Harald and Zhu, Suyun and Soldemo, Markus and Lömker, Patrick and Cavalca, Filippo and Scardamaglia, Mattia and Degerman, David and Nilsson, Anders and Amann, Peter and Shavorskiy, Andrey and Schnadt, Joachim}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Stroboscopic operando spectroscopy of the dynamics in heterogeneous catalysis by event-averaging}},
  url          = {{http://dx.doi.org/10.1038/s41467-021-26372-y}},
  doi          = {{10.1038/s41467-021-26372-y}},
  volume       = {{12}},
  year         = {{2021}},
}