Effects of Coke Deposits on the Catalytic Performance of Large Zeolite H-ZSM-5 Crystals during Alcohol-to-Hydrocarbons Reactions as Investigated by a Combination of Optical Spectroscopy and Microscopy

Emily Catherine Nordvang, Elena Borodina, Javier Ruiz-Martínez, Rasmus Fehrmann, Bert M. Weckhuysen

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Abstract

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.
Original languageEnglish
JournalChemistry: A European Journal
Volume21
Issue number48
Pages (from-to)17324-17335
Number of pages12
ISSN0947-6539
DOIs
Publication statusPublished - 2015

Bibliographical note

© 2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution Non-Commercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.

Keywords

  • Methanol-to-olefins
  • Fluorescence microscopy
  • Heterogeneous catalysis
  • UV/Vis spectroscopy
  • Zeolites

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