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Catalytic Oxidation of CO on a Curved Pt(111) Surface : Simultaneous Ignition at All Facets through a Transient CO-O Complex

Garcia-Martinez, Fernando ; García-Fernández, Carlos ; Simonovis, Juan Pablo ; Hunt, Adrian ; Walter, Andrew ; Waluyo, Iradwikanari ; Bertram, Florian LU ; Merte, Lindsay R. LU ; Shipilin, Mikhail LU and Pfaff, Sebastian LU , et al. (2020) In Angewandte Chemie - International Edition 59(45). p.20037-20043
Abstract

The catalytic oxidation of CO on transition metals, such as Pt, is commonly viewed as a sharp transition from the CO-inhibited surface to the active metal, covered with O. However, we find that minor amounts of O are present in the CO-poisoned layer that explain why, surprisingly, CO desorbs at stepped and flat Pt crystal planes at once, regardless of the reaction conditions. Using near-ambient pressure X-ray photoemission and a curved Pt(111) crystal we probe the chemical composition at surfaces with variable step density during the CO oxidation reaction. Analysis of C and O core levels across the curved crystal reveals that, right before light-off, subsurface O builds up within (111) terraces. This is key to trigger the simultaneous... (More)

The catalytic oxidation of CO on transition metals, such as Pt, is commonly viewed as a sharp transition from the CO-inhibited surface to the active metal, covered with O. However, we find that minor amounts of O are present in the CO-poisoned layer that explain why, surprisingly, CO desorbs at stepped and flat Pt crystal planes at once, regardless of the reaction conditions. Using near-ambient pressure X-ray photoemission and a curved Pt(111) crystal we probe the chemical composition at surfaces with variable step density during the CO oxidation reaction. Analysis of C and O core levels across the curved crystal reveals that, right before light-off, subsurface O builds up within (111) terraces. This is key to trigger the simultaneous ignition of the catalytic reaction at different Pt surfaces: a CO-Pt-O complex is formed that equals the CO chemisorption energy at terraces and steps, leading to the abrupt desorption of poisoning CO from all crystal facets at the same temperature.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
CO oxidation, curved surfaces, ignition, near-ambient pressure photoemission, subsurface oxygen
in
Angewandte Chemie - International Edition
volume
59
issue
45
pages
7 pages
publisher
John Wiley & Sons Inc.
external identifiers
  • scopus:85089978636
  • pmid:32701180
ISSN
1433-7851
DOI
10.1002/anie.202007195
project
Combined techniques for studies of catalysis
language
English
LU publication?
yes
id
3406c102-0b9b-4fd2-9637-9dde8acecff1
date added to LUP
2020-09-24 12:47:17
date last changed
2024-05-15 17:51:44
@article{3406c102-0b9b-4fd2-9637-9dde8acecff1,
  abstract     = {{<p>The catalytic oxidation of CO on transition metals, such as Pt, is commonly viewed as a sharp transition from the CO-inhibited surface to the active metal, covered with O. However, we find that minor amounts of O are present in the CO-poisoned layer that explain why, surprisingly, CO desorbs at stepped and flat Pt crystal planes at once, regardless of the reaction conditions. Using near-ambient pressure X-ray photoemission and a curved Pt(111) crystal we probe the chemical composition at surfaces with variable step density during the CO oxidation reaction. Analysis of C and O core levels across the curved crystal reveals that, right before light-off, subsurface O builds up within (111) terraces. This is key to trigger the simultaneous ignition of the catalytic reaction at different Pt surfaces: a CO-Pt-O complex is formed that equals the CO chemisorption energy at terraces and steps, leading to the abrupt desorption of poisoning CO from all crystal facets at the same temperature.</p>}},
  author       = {{Garcia-Martinez, Fernando and García-Fernández, Carlos and Simonovis, Juan Pablo and Hunt, Adrian and Walter, Andrew and Waluyo, Iradwikanari and Bertram, Florian and Merte, Lindsay R. and Shipilin, Mikhail and Pfaff, Sebastian and Blomberg, Sara and Zetterberg, Johan and Gustafson, Johan and Lundgren, Edvin and Sánchez-Portal, Daniel and Schiller, Frederik and Ortega, J. Enrique}},
  issn         = {{1433-7851}},
  keywords     = {{CO oxidation; curved surfaces; ignition; near-ambient pressure photoemission; subsurface oxygen}},
  language     = {{eng}},
  month        = {{11}},
  number       = {{45}},
  pages        = {{20037--20043}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Angewandte Chemie - International Edition}},
  title        = {{Catalytic Oxidation of CO on a Curved Pt(111) Surface : Simultaneous Ignition at All Facets through a Transient CO-O Complex}},
  url          = {{http://dx.doi.org/10.1002/anie.202007195}},
  doi          = {{10.1002/anie.202007195}},
  volume       = {{59}},
  year         = {{2020}},
}