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Dynamic response of chlorine atoms on a RuO2(110) model catalyst surface

Hofmann, Jan Philipp; Zweidinger, Stefan; Seitsonen, Ari Paavo; Farkas, Attila; Knapp, Marcus; Balmes, Olivier; Lundgren, Edvin LU ; Andersen, Jesper N LU and Over, Herbert (2010) In Physical Chemistry Chemical Physics 12(47). p.15358-15366
Abstract
The dynamic behavior of surface accommodated chlorine atoms on RuO2(110) was studied by a variety of experimental methods including high resolution core level shift, thermal desorption-, and in situ infrared spectroscopy as well as in situ surface X-ray diffraction in combination with state-of-the-art density functional theory calculations. On the chlorinated RuO2(110) surface the undercoordinated oxygen atoms have been selectively replaced by chlorine. These strongly bound surface chlorine atoms shift from bridging to on-top sites when the sample is annealed in oxygen, while the reverse shift of Cl from on-top into bridge positions is observed during CO exposure; the vacant bridge position is then occupied by either chlorine or CO. For... (More)
The dynamic behavior of surface accommodated chlorine atoms on RuO2(110) was studied by a variety of experimental methods including high resolution core level shift, thermal desorption-, and in situ infrared spectroscopy as well as in situ surface X-ray diffraction in combination with state-of-the-art density functional theory calculations. On the chlorinated RuO2(110) surface the undercoordinated oxygen atoms have been selectively replaced by chlorine. These strongly bound surface chlorine atoms shift from bridging to on-top sites when the sample is annealed in oxygen, while the reverse shift of Cl from on-top into bridge positions is observed during CO exposure; the vacant bridge position is then occupied by either chlorine or CO. For the CO oxidation reaction over chlorinated RuO2(110), the reactant induced site switching of chlorine causes a site-blocking of the catalytically active one-fold coordinatively unsaturated (1f-cus) Ru sites. This site blocking reduces the number of active sites and, even more important, on-top Cl blocks the free migration of the adsorbed reactants along the one-dimensional 1f-cus Ru rows, thus leading to a loss of catalytic activity. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Chemistry Chemical Physics
volume
12
issue
47
pages
15358 - 15366
publisher
Royal Society of Chemistry
external identifiers
  • wos:000284589900004
  • scopus:78649596314
ISSN
1463-9084
DOI
10.1039/c0cp01126f
language
English
LU publication?
yes
id
2613ffa3-3230-44c1-a37f-7ff7b46e0916 (old id 1752099)
date added to LUP
2010-12-29 16:13:25
date last changed
2018-05-29 10:16:34
@article{2613ffa3-3230-44c1-a37f-7ff7b46e0916,
  abstract     = {The dynamic behavior of surface accommodated chlorine atoms on RuO2(110) was studied by a variety of experimental methods including high resolution core level shift, thermal desorption-, and in situ infrared spectroscopy as well as in situ surface X-ray diffraction in combination with state-of-the-art density functional theory calculations. On the chlorinated RuO2(110) surface the undercoordinated oxygen atoms have been selectively replaced by chlorine. These strongly bound surface chlorine atoms shift from bridging to on-top sites when the sample is annealed in oxygen, while the reverse shift of Cl from on-top into bridge positions is observed during CO exposure; the vacant bridge position is then occupied by either chlorine or CO. For the CO oxidation reaction over chlorinated RuO2(110), the reactant induced site switching of chlorine causes a site-blocking of the catalytically active one-fold coordinatively unsaturated (1f-cus) Ru sites. This site blocking reduces the number of active sites and, even more important, on-top Cl blocks the free migration of the adsorbed reactants along the one-dimensional 1f-cus Ru rows, thus leading to a loss of catalytic activity.},
  author       = {Hofmann, Jan Philipp and Zweidinger, Stefan and Seitsonen, Ari Paavo and Farkas, Attila and Knapp, Marcus and Balmes, Olivier and Lundgren, Edvin and Andersen, Jesper N and Over, Herbert},
  issn         = {1463-9084},
  language     = {eng},
  number       = {47},
  pages        = {15358--15366},
  publisher    = {Royal Society of Chemistry},
  series       = {Physical Chemistry Chemical Physics},
  title        = {Dynamic response of chlorine atoms on a RuO2(110) model catalyst surface},
  url          = {http://dx.doi.org/10.1039/c0cp01126f},
  volume       = {12},
  year         = {2010},
}