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Formation of Epitaxial PdO(100) During the Oxidation of Pd(100)

Mehar, Vikram ; Edström, Helen LU ; Shipilin, Mikhail LU ; Hejral, Uta LU ; Wu, Chengjun ; Kadiri, Aravind ; Albertin, Stefano LU ; Hagman, Benjamin LU ; von Allmen, Kim LU orcid and Weigmann, Tim , et al. (2023) In The Journal of Physical Chemistry Letters 14(38). p.8493-8499
Abstract
The catalytic oxidation of CO and CH4 can be strongly influenced by the structures of oxide phases that form on metallic catalysts during reaction. Here, we show that an epitaxial PdO(100) structure forms at temperatures above 600 K during the oxidation of Pd(100) by gaseous O atoms as well as exposure to O2-rich mixtures at millibar partial pressures. The oxidation of Pd(100) by gaseous O atoms preferentially generates an epitaxial, multilayer PdO(101) structure at 500 K, but initiating Pd(100) oxidation above 600 K causes an epitaxial PdO(100) structure to grow concurrently with PdO(101) and produces a thicker and rougher oxide. We present evidence that this change in the oxidation behavior is caused by a... (More)
The catalytic oxidation of CO and CH4 can be strongly influenced by the structures of oxide phases that form on metallic catalysts during reaction. Here, we show that an epitaxial PdO(100) structure forms at temperatures above 600 K during the oxidation of Pd(100) by gaseous O atoms as well as exposure to O2-rich mixtures at millibar partial pressures. The oxidation of Pd(100) by gaseous O atoms preferentially generates an epitaxial, multilayer PdO(101) structure at 500 K, but initiating Pd(100) oxidation above 600 K causes an epitaxial PdO(100) structure to grow concurrently with PdO(101) and produces a thicker and rougher oxide. We present evidence that this change in the oxidation behavior is caused by a temperature-induced change in the stability of small PdO domains that initiate oxidation. Our discovery of the epitaxial PdO(100) structure may be significant for developing relationships among oxide structure, catalytic activity, and reaction conditions for applications of oxidation catalysis. (Less)
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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
chemical structure, epitaxy, oxidation, oxides, surface analysis
in
The Journal of Physical Chemistry Letters
volume
14
issue
38
pages
7 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:37721973
  • scopus:85174640403
ISSN
1948-7185
DOI
10.1021/acs.jpclett.3c01958
language
English
LU publication?
yes
id
9d4cae56-8c83-44cc-ab30-6b4f603fa67f
date added to LUP
2023-10-25 15:26:51
date last changed
2023-12-14 10:11:36
@article{9d4cae56-8c83-44cc-ab30-6b4f603fa67f,
  abstract     = {{The catalytic oxidation of CO and CH<sub>4</sub> can be strongly influenced by the structures of oxide phases that form on metallic catalysts during reaction. Here, we show that an epitaxial PdO(100) structure forms at temperatures above 600 K during the oxidation of Pd(100) by gaseous O atoms as well as exposure to O<sub>2</sub>-rich mixtures at millibar partial pressures. The oxidation of Pd(100) by gaseous O atoms preferentially generates an epitaxial, multilayer PdO(101) structure at 500 K, but initiating Pd(100) oxidation above 600 K causes an epitaxial PdO(100) structure to grow concurrently with PdO(101) and produces a thicker and rougher oxide. We present evidence that this change in the oxidation behavior is caused by a temperature-induced change in the stability of small PdO domains that initiate oxidation. Our discovery of the epitaxial PdO(100) structure may be significant for developing relationships among oxide structure, catalytic activity, and reaction conditions for applications of oxidation catalysis.}},
  author       = {{Mehar, Vikram and Edström, Helen and Shipilin, Mikhail and Hejral, Uta and Wu, Chengjun and Kadiri, Aravind and Albertin, Stefano and Hagman, Benjamin and von Allmen, Kim and Weigmann, Tim and Pfaff, Sebastian and Drnec, Jakub and Zetterberg, Johan and Lundgren, Edvin and Merte, Lindsay and Gustafson, Johan and Weaver, Jason}},
  issn         = {{1948-7185}},
  keywords     = {{chemical structure; epitaxy; oxidation; oxides; surface analysis}},
  language     = {{eng}},
  month        = {{09}},
  number       = {{38}},
  pages        = {{8493--8499}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{The Journal of Physical Chemistry Letters}},
  title        = {{Formation of Epitaxial PdO(100) During the Oxidation of Pd(100)}},
  url          = {{http://dx.doi.org/10.1021/acs.jpclett.3c01958}},
  doi          = {{10.1021/acs.jpclett.3c01958}},
  volume       = {{14}},
  year         = {{2023}},
}