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Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale

Eads, Calley N. LU orcid ; Wang, Weijia LU ; Küst, Ulrike LU orcid ; Prumbs, Julia LU ; Temperton, Robert H. LU ; Scardamaglia, Mattia LU ; Schnadt, Joachim LU orcid ; Knudsen, Jan LU and Shavorskiy, Andrey LU (2025) In Nature Communications 16(1).
Abstract

Catalytic studies traditionally rely on steady-state conditions resulting in time-averaged datasets that do not differentiate between active and spectator species. This limitation can cause misinterpretations of catalytic function, as the signal of short-lived intermediates responsible for producing desired reaction products is often masked by more intense spectator species. Time-resolved ambient pressure X-ray photoelectron spectroscopy (tr-APXPS) mitigates this issue by combining microsecond time resolution under reaction conditions. Using tr-APXPS, we investigate the oxidation of CO over Pt(111) by concurrently tracking reaction products, surface intermediates, and catalyst response. Our findings reveal that chemisorbed oxygen,... (More)

Catalytic studies traditionally rely on steady-state conditions resulting in time-averaged datasets that do not differentiate between active and spectator species. This limitation can cause misinterpretations of catalytic function, as the signal of short-lived intermediates responsible for producing desired reaction products is often masked by more intense spectator species. Time-resolved ambient pressure X-ray photoelectron spectroscopy (tr-APXPS) mitigates this issue by combining microsecond time resolution under reaction conditions. Using tr-APXPS, we investigate the oxidation of CO over Pt(111) by concurrently tracking reaction products, surface intermediates, and catalyst response. Our findings reveal that chemisorbed oxygen, rather than Pt surface oxide, is the main species reacting with CO to form CO2, supporting a primary Langmuir-Hinshelwood mechanism. The results shed new light on a heavily-debated reaction in catalysis. Beyond using CO pulses to determine active species, we demonstrate how careful tuning of pulsing parameters can be used for dynamic catalyst operation to enhance CO2 formation.

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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
16
issue
1
article number
1216
publisher
Nature Publishing Group
external identifiers
  • pmid:39890813
  • scopus:85217731981
ISSN
2041-1723
DOI
10.1038/s41467-025-56576-5
language
English
LU publication?
yes
id
8a0a4fcf-1af2-4782-a535-d0785687a319
date added to LUP
2025-06-09 09:53:46
date last changed
2025-07-07 12:46:50
@article{8a0a4fcf-1af2-4782-a535-d0785687a319,
  abstract     = {{<p>Catalytic studies traditionally rely on steady-state conditions resulting in time-averaged datasets that do not differentiate between active and spectator species. This limitation can cause misinterpretations of catalytic function, as the signal of short-lived intermediates responsible for producing desired reaction products is often masked by more intense spectator species. Time-resolved ambient pressure X-ray photoelectron spectroscopy (tr-APXPS) mitigates this issue by combining microsecond time resolution under reaction conditions. Using tr-APXPS, we investigate the oxidation of CO over Pt(111) by concurrently tracking reaction products, surface intermediates, and catalyst response. Our findings reveal that chemisorbed oxygen, rather than Pt surface oxide, is the main species reacting with CO to form CO<sub>2</sub>, supporting a primary Langmuir-Hinshelwood mechanism. The results shed new light on a heavily-debated reaction in catalysis. Beyond using CO pulses to determine active species, we demonstrate how careful tuning of pulsing parameters can be used for dynamic catalyst operation to enhance CO<sub>2</sub> formation.</p>}},
  author       = {{Eads, Calley N. and Wang, Weijia and Küst, Ulrike and Prumbs, Julia and Temperton, Robert H. and Scardamaglia, Mattia and Schnadt, Joachim and Knudsen, Jan and Shavorskiy, Andrey}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale}},
  url          = {{http://dx.doi.org/10.1038/s41467-025-56576-5}},
  doi          = {{10.1038/s41467-025-56576-5}},
  volume       = {{16}},
  year         = {{2025}},
}