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Strain Dependent Light-off Temperature in Catalysis Revealed by Planar Laser-Induced Fluorescence

Blomberg, Sara LU ; Zetterberg, Johan LU ; Zhou, Jianfeng LU ; Merte, Lindsay R. LU ; Gustafson, Johan LU ; Shipilin, Mikhail LU ; Trinchero, Adriana; Miccio, Luis A.; Magaña, Ana and Ilyn, Maxim, et al. (2017) In ACS Catalysis 7(1). p.110-114
Abstract

Understanding how specific atom sites on metal surfaces lower the energy barrier for chemical reactions is vital in catalysis. Studies on simplified model systems have shown that atoms arranged as steps on the surface play an important role in catalytic reactions, but a direct comparison of how the light-off temperature is affected by the atom orientation on the step has not yet been possible due to methodological constraints. Here we report in situ spatially resolved measurements of the CO2 production over a cylindrical-shaped Pd catalyst and show that the light-off temperature at different parts of the crystal depends on the step orientation of the two types of steps (named A and B). Our finding is supported by density... (More)

Understanding how specific atom sites on metal surfaces lower the energy barrier for chemical reactions is vital in catalysis. Studies on simplified model systems have shown that atoms arranged as steps on the surface play an important role in catalytic reactions, but a direct comparison of how the light-off temperature is affected by the atom orientation on the step has not yet been possible due to methodological constraints. Here we report in situ spatially resolved measurements of the CO2 production over a cylindrical-shaped Pd catalyst and show that the light-off temperature at different parts of the crystal depends on the step orientation of the two types of steps (named A and B). Our finding is supported by density functional theory calculations, revealing that the steps, in contrast to what has been previously reported in the literature, are not directly involved in the reaction onset but have the role of releasing stress.

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organization
publishing date
type
Contribution to journal
publication status
published
keywords
CO oxidation, cylindrical crystal, density functional theory, planar laser-induced fluorescence, steps
in
ACS Catalysis
volume
7
issue
1
pages
5 pages
publisher
The American Chemical Society
external identifiers
  • scopus:85019747583
  • wos:000391783200012
ISSN
2155-5435
DOI
10.1021/acscatal.6b02440
language
English
LU publication?
yes
id
7ed17991-cabc-4cb1-9c42-65160d86b0b2
date added to LUP
2017-08-17 15:14:22
date last changed
2017-09-18 11:41:53
@article{7ed17991-cabc-4cb1-9c42-65160d86b0b2,
  abstract     = {<p>Understanding how specific atom sites on metal surfaces lower the energy barrier for chemical reactions is vital in catalysis. Studies on simplified model systems have shown that atoms arranged as steps on the surface play an important role in catalytic reactions, but a direct comparison of how the light-off temperature is affected by the atom orientation on the step has not yet been possible due to methodological constraints. Here we report in situ spatially resolved measurements of the CO<sub>2</sub> production over a cylindrical-shaped Pd catalyst and show that the light-off temperature at different parts of the crystal depends on the step orientation of the two types of steps (named A and B). Our finding is supported by density functional theory calculations, revealing that the steps, in contrast to what has been previously reported in the literature, are not directly involved in the reaction onset but have the role of releasing stress.</p>},
  author       = {Blomberg, Sara and Zetterberg, Johan and Zhou, Jianfeng and Merte, Lindsay R. and Gustafson, Johan and Shipilin, Mikhail and Trinchero, Adriana and Miccio, Luis A. and Magaña, Ana and Ilyn, Maxim and Schiller, Frederik and Ortega, J Enrique and Bertram, Florian and Grönbeck, Henrik and Lundgren, Edvin},
  issn         = {2155-5435},
  keyword      = {CO oxidation,cylindrical crystal,density functional theory,planar laser-induced fluorescence,steps},
  language     = {eng},
  month        = {01},
  number       = {1},
  pages        = {110--114},
  publisher    = {The American Chemical Society},
  series       = {ACS Catalysis},
  title        = {Strain Dependent Light-off Temperature in Catalysis Revealed by Planar Laser-Induced Fluorescence},
  url          = {http://dx.doi.org/10.1021/acscatal.6b02440},
  volume       = {7},
  year         = {2017},
}