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- Title
Large Zeolite H-ZSM-5 Crystals as Models for the Methanol-to-Hydrocarbons Process: Bridging the Gap between Single-Particle Examination and Bulk Catalyst Analysis.
- Authors
Hofmann, Jan P.; Mores, Davide; Aramburo, Luis R.; Teketel, Shewangizaw; Rohnke, Marcus; Janek, Jürgen; Olsbye, Unni; Weckhuysen, Bert M.
- Abstract
The catalytic, deactivation, and regeneration characteristics of large coffin-shaped H-ZSM-5 crystals were investigated during the methanol-to-hydrocarbons (MTH) reaction at 350 and 500 °C. Online gas-phase effluent analysis and examination of retained material thereof were used to explore the bulk properties of large coffin-shaped zeolite H-ZSM-5 crystals in a fixed-bed reactor to introduce them as model catalysts for the MTH reaction. These findings were related to observations made at the individual particle level by using polarization-dependent UV-visible microspectroscopy and mass spectrometric techniques after reaction in an in situ microspectroscopy reaction cell. Excellent agreement between the spectroscopic measurements and the analysis of hydrocarbon deposits by means of retained hydrocarbon analysis and time-of-flight secondary-ion mass spectrometry of spent catalyst materials was observed. The obtained data reveal a shift towards more condensed coke deposits on the outer zeolite surface at higher reaction temperatures. Zeolites in the fixed-bed reactor setup underwent more coke deposition than those reacted in the in situ microspectroscopy reaction cell. Regeneration studies of the large zeolite crystals were performed by oxidation in O2/inert gas mixtures at 550 °C. UV-visible microspectroscopic measurements using the oligomerization of styrene derivatives as probe reaction indicated that the fraction of strong acid sites decreased during regeneration. This change was accompanied by a slight decrease in the initial conversion obtained after regeneration. H-ZSM-5 deactivated more rapidly at higher reaction temperature.
- Subjects
ZEOLITES; METHANOL; HYDROCARBONS; SILICATE minerals; ANALCIME
- Publication
Chemistry - A European Journal, 2013, Vol 19, Issue 26, p8533
- ISSN
0947-6539
- Publication type
Article
- DOI
10.1002/chem.201203351