Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 21, Issue 48, Pages 17324-17335Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201503136
Keywords
methanol-to-olefins; fluorescence microscopy; heterogeneous catalysis; UV/Vis spectroscopy; zeolites
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Funding
- Netherlands Research School Combination-Catalysis (NRSC-C)
- European Research Council (ERC) [321140]
- European Community [NMP2-LA-2010-246461]
- CW-NWO
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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 UVNis 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.
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