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Breakdown of the Structure–Function Relationship on a Polycrystalline Pd Catalyst Surface Illustrated by Dynamic CO Oxidation

Prumbs, Julia LU ; Küst, Ulrike LU orcid ; Gericke, Sabrina M. LU ; Rämisch, Lisa LU ; Scardamaglia, Mattia LU ; Temperton, Robert LU ; Shavorskiy, Andrey LU ; Zetterberg, Johan LU orcid and Knudsen, Jan LU orcid (2026) In ACS Catalysis 16(8). p.7281-7288
Abstract

Real catalysts consisting of nanoparticles host many nanofacets. Each nanofacet changes its structure and function in response to its local environment but is also affected by neighboring nanofacets. Time-resolved operando experiments close to realistic conditions at polycrystals mimicking real catalyst particles are unfortunately challenging but could be highly rewarding. Here, we demonstrate how such studies can be performed with time-resolved ambient pressure X-ray photoelectron spectroscopy in the millibar regime and how the local surface composition/adsorbates and gas composition can be measured simultaneously for grains on a Pd polycrystal. For the CO oxidation reaction, we demonstrate how the ignition and extinction are... (More)

Real catalysts consisting of nanoparticles host many nanofacets. Each nanofacet changes its structure and function in response to its local environment but is also affected by neighboring nanofacets. Time-resolved operando experiments close to realistic conditions at polycrystals mimicking real catalyst particles are unfortunately challenging but could be highly rewarding. Here, we demonstrate how such studies can be performed with time-resolved ambient pressure X-ray photoelectron spectroscopy in the millibar regime and how the local surface composition/adsorbates and gas composition can be measured simultaneously for grains on a Pd polycrystal. For the CO oxidation reaction, we demonstrate how the ignition and extinction are gas-phase-driven and grain-independent, while the surface structure near the extinction point is highly grain-dependent.

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author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
APXPS, CO oxidation, extinction, FT-APXPS, ignition, palladium, polycrystals, time-resolved
in
ACS Catalysis
volume
16
issue
8
pages
8 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:105036416890
ISSN
2155-5435
DOI
10.1021/acscatal.5c08153
language
English
LU publication?
yes
id
89144309-3595-4a41-b3a3-a19d2c68dbd7
date added to LUP
2026-05-21 11:47:24
date last changed
2026-05-26 08:03:09
@article{89144309-3595-4a41-b3a3-a19d2c68dbd7,
  abstract     = {{<p>Real catalysts consisting of nanoparticles host many nanofacets. Each nanofacet changes its structure and function in response to its local environment but is also affected by neighboring nanofacets. Time-resolved operando experiments close to realistic conditions at polycrystals mimicking real catalyst particles are unfortunately challenging but could be highly rewarding. Here, we demonstrate how such studies can be performed with time-resolved ambient pressure X-ray photoelectron spectroscopy in the millibar regime and how the local surface composition/adsorbates and gas composition can be measured simultaneously for grains on a Pd polycrystal. For the CO oxidation reaction, we demonstrate how the ignition and extinction are gas-phase-driven and grain-independent, while the surface structure near the extinction point is highly grain-dependent.</p>}},
  author       = {{Prumbs, Julia and Küst, Ulrike and Gericke, Sabrina M. and Rämisch, Lisa and Scardamaglia, Mattia and Temperton, Robert and Shavorskiy, Andrey and Zetterberg, Johan and Knudsen, Jan}},
  issn         = {{2155-5435}},
  keywords     = {{APXPS; CO oxidation; extinction; FT-APXPS; ignition; palladium; polycrystals; time-resolved}},
  language     = {{eng}},
  number       = {{8}},
  pages        = {{7281--7288}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Catalysis}},
  title        = {{Breakdown of the Structure–Function Relationship on a Polycrystalline Pd Catalyst Surface Illustrated by Dynamic CO Oxidation}},
  url          = {{http://dx.doi.org/10.1021/acscatal.5c08153}},
  doi          = {{10.1021/acscatal.5c08153}},
  volume       = {{16}},
  year         = {{2026}},
}