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An investigation of the reaction mechanism for the promotion of propane oxidation over Pt/Al2O3 by SO2

Hinz, A; Skoglundh, M; Fridell, E and Andersson, Arne LU (2001) In Journal of Catalysis 201(2). p.247-257
Abstract
Total oxidation of propane with oxygen in the absence and the respective presence of SO2 in the feed gas was studied over 1 wt% Pt on gamma -Al2O3 using transient experiments with TAP (temporal analysis of products) and in situ DRIFT spectroscopy. The TAP experiments confirm the promoting role of SO2 on the conversion of propane and, moreover, show an inhibiting effect from SO2 on the conversion of the intermediate products propene and CO. In situ DRIFT spectroscopy reveals the formation of sulphate species on the catalyst surface and indicates the formation of an allylic intermediate in the absence of SO2 only. Interaction between hydrocarbon intermediates and the sulphate species is confirmed by the appearance of thiol fragments in the... (More)
Total oxidation of propane with oxygen in the absence and the respective presence of SO2 in the feed gas was studied over 1 wt% Pt on gamma -Al2O3 using transient experiments with TAP (temporal analysis of products) and in situ DRIFT spectroscopy. The TAP experiments confirm the promoting role of SO2 on the conversion of propane and, moreover, show an inhibiting effect from SO2 on the conversion of the intermediate products propene and CO. In situ DRIFT spectroscopy reveals the formation of sulphate species on the catalyst surface and indicates the formation of an allylic intermediate in the absence of SO2 only. Interaction between hydrocarbon intermediates and the sulphate species is confirmed by the appearance of thiol fragments in the mass spectra. The transient experiments show that propane in the first step is irreversibly adsorbed at the surface. Analysis of the surface residence times of the products formed at the propane pulse in pump-probe experiments provides information about the reaction pathways. Without S02 in the feed gas, propane reacts consecutively in the sequence propane --> propene -->. ethane --> CO --> CO2. In the presence of SO2 the first step of the main route is the breaking of a C-C bond in propane producing ethane and a C-1 fragment, which then form CO and eventually CO2. It is suggested that the promoting effect by SO2 on the conversion of propane is due to the formation of an acidic site at the Pt/Al2O3/SO42- interface. (C) 2001 Academic Press. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
TAP, in situ DRIFT, reaction mechanism, transient experiments, propane oxidation, promotion by SO2, Pt/Al2O3
in
Journal of Catalysis
volume
201
issue
2
pages
247 - 257
publisher
Elsevier
external identifiers
  • wos:000170172200010
  • scopus:0035741904
ISSN
1090-2694
DOI
10.1006/jcat.2001.3248
language
English
LU publication?
yes
id
4076eeef-0e7f-4448-a615-ba3eb7773ccf (old id 3915436)
date added to LUP
2013-07-02 08:44:48
date last changed
2018-01-07 05:32:04
@article{4076eeef-0e7f-4448-a615-ba3eb7773ccf,
  abstract     = {Total oxidation of propane with oxygen in the absence and the respective presence of SO2 in the feed gas was studied over 1 wt% Pt on gamma -Al2O3 using transient experiments with TAP (temporal analysis of products) and in situ DRIFT spectroscopy. The TAP experiments confirm the promoting role of SO2 on the conversion of propane and, moreover, show an inhibiting effect from SO2 on the conversion of the intermediate products propene and CO. In situ DRIFT spectroscopy reveals the formation of sulphate species on the catalyst surface and indicates the formation of an allylic intermediate in the absence of SO2 only. Interaction between hydrocarbon intermediates and the sulphate species is confirmed by the appearance of thiol fragments in the mass spectra. The transient experiments show that propane in the first step is irreversibly adsorbed at the surface. Analysis of the surface residence times of the products formed at the propane pulse in pump-probe experiments provides information about the reaction pathways. Without S02 in the feed gas, propane reacts consecutively in the sequence propane --> propene -->. ethane --> CO --> CO2. In the presence of SO2 the first step of the main route is the breaking of a C-C bond in propane producing ethane and a C-1 fragment, which then form CO and eventually CO2. It is suggested that the promoting effect by SO2 on the conversion of propane is due to the formation of an acidic site at the Pt/Al2O3/SO42- interface. (C) 2001 Academic Press.},
  author       = {Hinz, A and Skoglundh, M and Fridell, E and Andersson, Arne},
  issn         = {1090-2694},
  keyword      = {TAP,in situ DRIFT,reaction mechanism,transient experiments,propane oxidation,promotion by SO2,Pt/Al2O3},
  language     = {eng},
  number       = {2},
  pages        = {247--257},
  publisher    = {Elsevier},
  series       = {Journal of Catalysis},
  title        = {An investigation of the reaction mechanism for the promotion of propane oxidation over Pt/Al2O3 by SO2},
  url          = {http://dx.doi.org/10.1006/jcat.2001.3248},
  volume       = {201},
  year         = {2001},
}