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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
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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
2016-04-01 10:15:40
date last changed
2022-02-02 08:08:56
@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}},
  keywords     = {{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}},
  doi          = {{10.1016/j.jcat.2010.02.030}},
  volume       = {{272}},
  year         = {{2010}},
}