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Bridging the Pressure Gap in CO Oxidation

Blomberg, Sara LU ; Hejral, Uta LU ; Shipilin, Mikhail LU ; Albertin, Stefano LU ; Karlsson, Hanna LU ; Hulteberg, Christian LU orcid ; Lömker, Patrick ; Goodwin, Christopher ; Degerman, David and Gustafson, Johan LU , et al. (2021) In ACS Catalysis 11(15). p.9128-9135
Abstract

Performing fundamental operando catalysis studies under realistic conditions is a key to further develop and increase the efficiency of industrial catalysts. Operando X-ray photoelectron spectroscopy (XPS) experiments have been limited to pressures, and the relevance for industrial applications has been questioned. Herein, we report on the CO oxidation experiment on Pd(100) performed at a total pressure of 1 bar using XPS. We investigate the light-off regime and the surface chemical composition at the atomistic level in the highly active phase. Furthermore, the observed gas-phase photoemission peaks of CO2, CO, and O2 indicate that the kinetics of the reaction during the light-off regime can be... (More)

Performing fundamental operando catalysis studies under realistic conditions is a key to further develop and increase the efficiency of industrial catalysts. Operando X-ray photoelectron spectroscopy (XPS) experiments have been limited to pressures, and the relevance for industrial applications has been questioned. Herein, we report on the CO oxidation experiment on Pd(100) performed at a total pressure of 1 bar using XPS. We investigate the light-off regime and the surface chemical composition at the atomistic level in the highly active phase. Furthermore, the observed gas-phase photoemission peaks of CO2, CO, and O2 indicate that the kinetics of the reaction during the light-off regime can be followed operando, and by studying the reaction rate of the reaction, the activation energy is calculated. The reaction was preceded by an in situ oxidation study in 7% O2 in He and a total pressure of 70 mbar to confirm the surface sensitivity and assignment of the oxygen-induced photoemission peaks. However, oxygen-induced photoemission peaks were not observed during the reaction studies, but instead, a metallic Pd phase is present in the highly active regime under the conditions applied. The novel XPS setup utilizes hard X-rays to enable high-pressure studies, combined with a grazing incident angle to increase the surface sensitivity of the measurement. Our findings demonstrate the possibilities of achieving chemical information of the catalyst, operando, on an atomistic level, under industrially relevant conditions.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
CO oxidation, high pressure, operando, Pd(100), XPS
in
ACS Catalysis
volume
11
issue
15
pages
8 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:34476111
  • scopus:85111185145
ISSN
2155-5435
DOI
10.1021/acscatal.1c00806
language
English
LU publication?
yes
id
271a77e1-d7d2-4e3c-96a7-2c46fb7dc105
date added to LUP
2021-08-10 08:32:28
date last changed
2024-12-29 10:35:46
@article{271a77e1-d7d2-4e3c-96a7-2c46fb7dc105,
  abstract     = {{<p>Performing fundamental <i>operando </i>catalysis studies under realistic conditions is a key to further develop and increase the efficiency of industrial catalysts. <i>Operando </i>X-ray photoelectron spectroscopy (XPS) experiments have been limited to pressures, and the relevance for industrial applications has been questioned. Herein, we report on the CO oxidation experiment on Pd(100) performed at a total pressure of 1 bar using XPS. We investigate the light-off regime and the surface chemical composition at the atomistic level in the highly active phase. Furthermore, the observed gas-phase photoemission peaks of CO<sub>2</sub>, CO, and O<sub>2</sub> indicate that the kinetics of the reaction during the light-off regime can be followed <i>operando</i>, and by studying the reaction rate of the reaction, the activation energy is calculated. The reaction was preceded by an in situ oxidation study in 7% O<sub>2</sub> in He and a total pressure of 70 mbar to confirm the surface sensitivity and assignment of the oxygen-induced photoemission peaks. However, oxygen-induced photoemission peaks were not observed during the reaction studies, but instead, a metallic Pd phase is present in the highly active regime under the conditions applied. The novel XPS setup utilizes hard X-rays to enable high-pressure studies, combined with a grazing incident angle to increase the surface sensitivity of the measurement. Our findings demonstrate the possibilities of achieving chemical information of the catalyst, <i>operando</i>, on an atomistic level, under industrially relevant conditions. </p>}},
  author       = {{Blomberg, Sara and Hejral, Uta and Shipilin, Mikhail and Albertin, Stefano and Karlsson, Hanna and Hulteberg, Christian and Lömker, Patrick and Goodwin, Christopher and Degerman, David and Gustafson, Johan and Schlueter, Christoph and Nilsson, Anders and Lundgren, Edvin and Amann, Peter}},
  issn         = {{2155-5435}},
  keywords     = {{CO oxidation; high pressure; operando; Pd(100); XPS}},
  language     = {{eng}},
  number       = {{15}},
  pages        = {{9128--9135}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Catalysis}},
  title        = {{Bridging the Pressure Gap in CO Oxidation}},
  url          = {{http://dx.doi.org/10.1021/acscatal.1c00806}},
  doi          = {{10.1021/acscatal.1c00806}},
  volume       = {{11}},
  year         = {{2021}},
}