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In situ studies of the oxidation of HCl over RuO2 model catalysts: Stability and reactivity

Zweidinger, S.; Hofmann, J. P.; Balmes, O.; Lundgren, Edvin LU and Over, H. (2010) In Journal of Catalysis 272(1). p.169-175
Abstract
Structure-activity experiments were performed for the HCl oxidation reaction (Deacon-like process) over RuO2 model catalysts - RuO2(1 1 0) and RuO2(1 0 0) - applying in situ surface X-ray diffraction (SXRD) combined with on-line mass spectrometry. The studied model catalysts turned out to be long-term stable under reaction conditions with gas feed ratios p(HCl):p(O-2) ranging from 1:4 to 4:1 in the mbar pressure regime and temperatures as high as 685 K. Even pure HCl exposure in the mbar regime was not able to reduce RuO2 below 600 K; above 650 K chemical reduction of the oxide sets in. Under strongly oxidizing reaction conditions, the (surface) oxides grow slowly in thickness. On-line reactivity experiments of both types of model... (More)
Structure-activity experiments were performed for the HCl oxidation reaction (Deacon-like process) over RuO2 model catalysts - RuO2(1 1 0) and RuO2(1 0 0) - applying in situ surface X-ray diffraction (SXRD) combined with on-line mass spectrometry. The studied model catalysts turned out to be long-term stable under reaction conditions with gas feed ratios p(HCl):p(O-2) ranging from 1:4 to 4:1 in the mbar pressure regime and temperatures as high as 685 K. Even pure HCl exposure in the mbar regime was not able to reduce RuO2 below 600 K; above 650 K chemical reduction of the oxide sets in. Under strongly oxidizing reaction conditions, the (surface) oxides grow slowly in thickness. On-line reactivity experiments of both types of model catalysts in a batch reactor yield a mean turn-over frequency (TOP) of 0.6 Cl-2 molecules per second and active site for the HCl oxidation at 650 K and initial partial pressures of p(HCl) = 2 mbar and p(O-2) = 0.5 mbar. The HCl oxidation over RuO2 is therefore considered to be structure insensitive. (C) 2010 Elsevier Inc. All rights reserved. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
RuO2, Reactivity, Stability, Surfaces, Heterogeneous catalysis, In situ SXRD, Deacon process
in
Journal of Catalysis
volume
272
issue
1
pages
169 - 175
publisher
Elsevier
external identifiers
  • wos:000279090500019
  • scopus:77953765511
ISSN
1090-2694
DOI
10.1016/j.jcat.2010.02.030
language
English
LU publication?
yes
id
5e5a0092-0596-4723-a347-fea6b161526a (old id 1630084)
date added to LUP
2010-07-22 15:40:37
date last changed
2018-05-29 09:49:37
@article{5e5a0092-0596-4723-a347-fea6b161526a,
  abstract     = {Structure-activity experiments were performed for the HCl oxidation reaction (Deacon-like process) over RuO2 model catalysts - RuO2(1 1 0) and RuO2(1 0 0) - applying in situ surface X-ray diffraction (SXRD) combined with on-line mass spectrometry. The studied model catalysts turned out to be long-term stable under reaction conditions with gas feed ratios p(HCl):p(O-2) ranging from 1:4 to 4:1 in the mbar pressure regime and temperatures as high as 685 K. Even pure HCl exposure in the mbar regime was not able to reduce RuO2 below 600 K; above 650 K chemical reduction of the oxide sets in. Under strongly oxidizing reaction conditions, the (surface) oxides grow slowly in thickness. On-line reactivity experiments of both types of model catalysts in a batch reactor yield a mean turn-over frequency (TOP) of 0.6 Cl-2 molecules per second and active site for the HCl oxidation at 650 K and initial partial pressures of p(HCl) = 2 mbar and p(O-2) = 0.5 mbar. The HCl oxidation over RuO2 is therefore considered to be structure insensitive. (C) 2010 Elsevier Inc. All rights reserved.},
  author       = {Zweidinger, S. and Hofmann, J. P. and Balmes, O. and Lundgren, Edvin and Over, H.},
  issn         = {1090-2694},
  keyword      = {RuO2,Reactivity,Stability,Surfaces,Heterogeneous catalysis,In situ SXRD,Deacon process},
  language     = {eng},
  number       = {1},
  pages        = {169--175},
  publisher    = {Elsevier},
  series       = {Journal of Catalysis},
  title        = {In situ studies of the oxidation of HCl over RuO2 model catalysts: Stability and reactivity},
  url          = {http://dx.doi.org/10.1016/j.jcat.2010.02.030},
  volume       = {272},
  year         = {2010},
}