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Ambient pressure operando catalytic characterization by combining PM-IRRAS with planar laser-induced fluorescence and surface optical reflectance imaging

Rämisch, Lisa LU ; Pfaff, Sebastian LU ; Gericke, Sabrina M. LU ; Lundgren, Edvin LU and Zetterberg, Johan LU orcid (2024) In Catalysis Today 427.
Abstract

We present a combination of optical operando techniques that allow us to bridge the pressure gap in heterogeneous catalysis. By combining Polarization Modulated - InfraRed Reflection Absorption Spectroscopy (PM-IRRAS) with two dimensional-Surface Optical Reflectance (2D-SOR) and Planar Laser Induced Fluorescence (PLIF), we can simultaneously measure the adsorbed species on the catalyst surface, monitor the surface oxide formation across the catalyst surface and image the gas phase right above the catalyst surface, respectively. In a single measurement, we are able to follow heterogeneous catalytic reactions temporally- and spatially resolved with all three optical techniques, which are additionally supported by Mass Spectrometry (MS).... (More)

We present a combination of optical operando techniques that allow us to bridge the pressure gap in heterogeneous catalysis. By combining Polarization Modulated - InfraRed Reflection Absorption Spectroscopy (PM-IRRAS) with two dimensional-Surface Optical Reflectance (2D-SOR) and Planar Laser Induced Fluorescence (PLIF), we can simultaneously measure the adsorbed species on the catalyst surface, monitor the surface oxide formation across the catalyst surface and image the gas phase right above the catalyst surface, respectively. In a single measurement, we are able to follow heterogeneous catalytic reactions temporally- and spatially resolved with all three optical techniques, which are additionally supported by Mass Spectrometry (MS). To validate the experimental setup, we perform two experiments studying CO oxidation on Pd(100) at 150 mbar and 910 mbar by ramping the sample temperature. PM-IRRAS and 2D-SOR reveal that the formation of well-defined ultrathin surface oxide coincides with the disappearance of CO adsorption on the surface. At the same time, PLIF and MS confirm the simultaneous transition into a mass-transfer-limited (MTL) regime. A difference between 150 and 910 mbar can be seen in the light-off temperature caused by different partial pressures of CO and in the spatial distribution of the gas cloud across the surface in space caused by gas diffusion. This emphasizes the need for spatially-resolved gas phase diagnostics in heterogeneous catalysis. The combination of all techniques aids our understanding of the gas-surface interaction.

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author
; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Gas phase imaging, Mass spectrometry, Operando catalysis, PM-IRRAS, Reactor development, Reflectance microscopy, Surface spectroscopy
in
Catalysis Today
volume
427
article number
114441
publisher
Elsevier
external identifiers
  • scopus:85175580656
ISSN
0920-5861
DOI
10.1016/j.cattod.2023.114441
language
English
LU publication?
yes
id
ef600282-f809-474a-b77b-b853033bb7fd
date added to LUP
2023-11-23 15:08:33
date last changed
2023-12-05 12:36:14
@article{ef600282-f809-474a-b77b-b853033bb7fd,
  abstract     = {{<p>We present a combination of optical operando techniques that allow us to bridge the pressure gap in heterogeneous catalysis. By combining Polarization Modulated - InfraRed Reflection Absorption Spectroscopy (PM-IRRAS) with two dimensional-Surface Optical Reflectance (2D-SOR) and Planar Laser Induced Fluorescence (PLIF), we can simultaneously measure the adsorbed species on the catalyst surface, monitor the surface oxide formation across the catalyst surface and image the gas phase right above the catalyst surface, respectively. In a single measurement, we are able to follow heterogeneous catalytic reactions temporally- and spatially resolved with all three optical techniques, which are additionally supported by Mass Spectrometry (MS). To validate the experimental setup, we perform two experiments studying CO oxidation on Pd(100) at 150 mbar and 910 mbar by ramping the sample temperature. PM-IRRAS and 2D-SOR reveal that the formation of well-defined ultrathin surface oxide coincides with the disappearance of CO adsorption on the surface. At the same time, PLIF and MS confirm the simultaneous transition into a mass-transfer-limited (MTL) regime. A difference between 150 and 910 mbar can be seen in the light-off temperature caused by different partial pressures of CO and in the spatial distribution of the gas cloud across the surface in space caused by gas diffusion. This emphasizes the need for spatially-resolved gas phase diagnostics in heterogeneous catalysis. The combination of all techniques aids our understanding of the gas-surface interaction.</p>}},
  author       = {{Rämisch, Lisa and Pfaff, Sebastian and Gericke, Sabrina M. and Lundgren, Edvin and Zetterberg, Johan}},
  issn         = {{0920-5861}},
  keywords     = {{Gas phase imaging; Mass spectrometry; Operando catalysis; PM-IRRAS; Reactor development; Reflectance microscopy; Surface spectroscopy}},
  language     = {{eng}},
  publisher    = {{Elsevier}},
  series       = {{Catalysis Today}},
  title        = {{Ambient pressure operando catalytic characterization by combining PM-IRRAS with planar laser-induced fluorescence and surface optical reflectance imaging}},
  url          = {{http://dx.doi.org/10.1016/j.cattod.2023.114441}},
  doi          = {{10.1016/j.cattod.2023.114441}},
  volume       = {{427}},
  year         = {{2024}},
}