Stroboscopic operando spectroscopy of the dynamics in heterogeneous catalysis by event-averaging
(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.
(Less)
- author
- organization
- publishing date
- 2021-12
- 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
- 2025-02-09 19:43:13
@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}}, }