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Catalytic Oxidation of Carbon Monoxide on a Curved Pd Crystal : Spatial Variation of Active and Poisoning Phases in Stationary Conditions

Schiller, Frederik; Ilyn, Max; Pérez-Dieste, Virginia; Escudero, Carlos; Huck-Iriart, Cristián; Ruiz Del Arbol, Nerea; Hagman, Benjamin LU ; Merte, Lindsay R. LU ; Bertram, Florian LU and Shipilin, Mikhail LU , et al. (2018) In Journal of the American Chemical Society 140(47). p.16245-16252
Abstract

Understanding nanoparticle catalysis requires novel approaches in which adjoining crystal orientations can be studied under the same reactive conditions. Here we use a curved palladium crystal and near-ambient pressure X-ray photoemission spectroscopy to characterize chemical species during the catalytic oxidation of CO in a whole set of surfaces vicinal to the (111) direction simultaneously. By stabilizing the reaction at fixed temperatures around the ignition point, we observe a strong variation of the catalytic activity across the curved surface. Such spatial modulation of the reaction stage is straightforwardly mapped through the photoemission signal from active oxygen species and poisoning CO, which are shown to coexist in a... (More)

Understanding nanoparticle catalysis requires novel approaches in which adjoining crystal orientations can be studied under the same reactive conditions. Here we use a curved palladium crystal and near-ambient pressure X-ray photoemission spectroscopy to characterize chemical species during the catalytic oxidation of CO in a whole set of surfaces vicinal to the (111) direction simultaneously. By stabilizing the reaction at fixed temperatures around the ignition point, we observe a strong variation of the catalytic activity across the curved surface. Such spatial modulation of the reaction stage is straightforwardly mapped through the photoemission signal from active oxygen species and poisoning CO, which are shown to coexist in a transient regime that depends on the vicinal angle. Line-shape analysis and direct comparison with ultrahigh vacuum experiments help identifying and quantifying all such surface species, allowing us to reveal the presence of surface oxides during reaction ignition and cooling-off.

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Contribution to journal
publication status
published
subject
in
Journal of the American Chemical Society
volume
140
issue
47
pages
8 pages
publisher
The American Chemical Society
external identifiers
  • scopus:85057221867
ISSN
1520-5126
DOI
10.1021/jacs.8b09428
language
English
LU publication?
yes
id
7cbbc143-baa0-4aa2-a501-3f04ecf1358a
date added to LUP
2018-12-03 13:31:22
date last changed
2018-12-03 13:31:22
@article{7cbbc143-baa0-4aa2-a501-3f04ecf1358a,
  abstract     = {<p>Understanding nanoparticle catalysis requires novel approaches in which adjoining crystal orientations can be studied under the same reactive conditions. Here we use a curved palladium crystal and near-ambient pressure X-ray photoemission spectroscopy to characterize chemical species during the catalytic oxidation of CO in a whole set of surfaces vicinal to the (111) direction simultaneously. By stabilizing the reaction at fixed temperatures around the ignition point, we observe a strong variation of the catalytic activity across the curved surface. Such spatial modulation of the reaction stage is straightforwardly mapped through the photoemission signal from active oxygen species and poisoning CO, which are shown to coexist in a transient regime that depends on the vicinal angle. Line-shape analysis and direct comparison with ultrahigh vacuum experiments help identifying and quantifying all such surface species, allowing us to reveal the presence of surface oxides during reaction ignition and cooling-off.</p>},
  author       = {Schiller, Frederik and Ilyn, Max and Pérez-Dieste, Virginia and Escudero, Carlos and Huck-Iriart, Cristián and Ruiz Del Arbol, Nerea and Hagman, Benjamin and Merte, Lindsay R. and Bertram, Florian and Shipilin, Mikhail and Blomberg, Sara and Gustafson, Johan and Lundgren, Edvin and Ortega, J. Enrique},
  issn         = {1520-5126},
  language     = {eng},
  number       = {47},
  pages        = {16245--16252},
  publisher    = {The American Chemical Society},
  series       = {Journal of the American Chemical Society},
  title        = {Catalytic Oxidation of Carbon Monoxide on a Curved Pd Crystal : Spatial Variation of Active and Poisoning Phases in Stationary Conditions},
  url          = {http://dx.doi.org/10.1021/jacs.8b09428},
  volume       = {140},
  year         = {2018},
}