Catalytic Oxidation of CO on a Curved Pt(111) Surface : Simultaneous Ignition at All Facets through a Transient CO-O Complex
(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.
(Less)
- author
- organization
- publishing date
- 2020-11-02
- 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
- 2024-09-05 04:38:17
@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}}, }