Infra-Red thermography and spatially-resolved capillary inlet mass spectrometry (SpaciMS) have been used to characterize propylene oxidation along a Pt/Al2O3 monolith-supported catalyst, before and after heterogeneous deactivation. The combined techniques clearly show reaction location, and therefore catalyst use, and how these change with thermal and sulphur degradation.
Following the heterogeneous thermal aging, the reaction zones at steady state were broader and located farther into the catalyst relative to those observed with the fresh catalyst. As well, the time for the temperature and concentration waves to travel through the catalyst during back-to-front ignition increased. These effects were more pronounced with 1500 ppm propylene relative to 4500 ppm propylene. Such trends could not be detected based on standard catalyst-outlet measurements. The light-off behaviour was also impacted by the aging, resulting in complex changes to the temperature front propagation, depending on the propylene concentration.
With each sulphur exposure step, light-off temperatures increased and the time for back-to-front ignition during temperature programmed oxidation changed pattern. With 1500 ppm propylene fed, the reaction zones established during steady-state operation shifted farther into the catalyst and increased slightly in width following sulphur treatment; at very high temperature and for 4500 ppm propylene, the reaction zones were very close to the catalyst inlet and virtually indistinguishable between catalyst sulphation states. However, at lower steady-state temperatures for the higher propylene concentration, the catalyst did experience delays in reaction light-off and light-off position moved downstream in the catalyst with sulphur damage.
| Identifer | oai:union.ndltd.org:WATERLOO/oai:uwspace.uwaterloo.ca:10012/5643 |
| Date | January 2010 |
| Creators | Russell, April Elizabeth |
| Source Sets | University of Waterloo Electronic Theses Repository |
| Language | English |
| Detected Language | English |
| Type | Thesis or Dissertation |
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