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Effects of Coke Deposits on the Catalytic Performance of Large Zeolite H‐ZSM‐5 Crystals during Alcohol‐to‐Hydrocarbon Reactions as Investigated by a Combination of Optical Spectroscopy and Microscopy
Author(s) -
Nordvang Emily C.,
Borodina Elena,
RuizMartínez Javier,
Fehrmann Rasmus,
Weckhuysen Bert M.
Publication year - 2015
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201503136
Subject(s) - zeolite , catalysis , coke , zsm 5 , methanol , chemistry , hydrocarbon , spectroscopy , photochemistry , crystal (programming language) , single crystal , fluorescence spectroscopy , alcohol , fluorescence , analytical chemistry (journal) , organic chemistry , crystallography , optics , physics , quantum mechanics , computer science , programming language
The catalytic activity of large zeolite H‐ZSM‐5 crystals in methanol (MTO) and ethanol‐to‐olefins (ETO) conversions was investigated and, using operando UV/Vis measurements, the catalytic activity and deactivation was correlated with the formation of coke. These findings were related to in situ single crystal UV/Vis and confocal fluorescence micro‐spectroscopy, allowing the observation of the spatiotemporal formation of intermediates and coke species during the MTO and ETO conversions. It was observed that rapid deactivation at elevated temperatures was due to the fast formation of aromatics at the periphery of the H‐ZSM‐5 crystals, which are transformed into more poly‐aromatic coke species at the external surface, preventing the diffusion of reactants and products into and out of the H‐ZSM‐5 crystal. Furthermore, we were able to correlate the operando UV/Vis spectroscopy results observed during catalytic testing with the single crystal in situ results.