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Faraday Discussions Vol -99

An assessment of hydrocarbon species in the methanol-to-hydrocarbon reaction over a ZSM-5 catalyst

Content Provider	Royal Society of Chemistry (RSC)
Author	Gibson, Emma K. Catlow, C. Richard A. Collier, Paul Parker, Stewart F. McGregor, James Lennon, David Howe, Russell F. Hameed, Ali
Copyright Year	2017
Abstract	A ZSM-5 catalyst is examined in relation to the methanol-to-hydrocarbon (MTH) reaction as a function of reaction temperature and time-on-stream. The reaction profile is characterised using in-line mass spectrometry. Furthermore, the material contained within a catch-pot downstream from the reactor is analysed using gas chromatography-mass spectrometry. For a fixed methanol feed, reaction conditions are selected to define various stages of the reaction coordinate: (i) initial methanol adsorption at a sub-optimum reaction temperature (1 h at 200 °C); (ii) initial stages of reaction at an optimised reaction temperature (1 h at 350 °C); (iii) steady-state operation at an optimised reaction temperature (3 days at 350 °C); and (iv) accelerated ageing (3 days at 400 °C). Post-reaction, the catalyst samples are analysed ex situ by a combination of temperature-programmed oxidation (TPO) and spectroscopically by electron paramagnetic resonance (EPR), diffuse-reflectance infrared and inelastic neutron scattering (INS) spectroscopies. The TPO measurements provide an indication of the degree of ‘coking’ experienced by each sample. The EPR measurements detect aromatic radical cations. The IR and INS measurements reveal the presence of retained hydrocarbonaceous species, the nature of which are discussed in terms of the well-developed ‘hydrocarbon pool’ mechanism. This combination of experimental evidence, uniquely applied to this reaction system, establishes the importance of retained hydrocarbonaceous species in effecting the product distribution of this economically relevant reaction system.
Starting Page	447
Ending Page	471
Page Count	25
File Format	HTM / HTML PDF
ISSN	13596640
Volume Number	197
Journal	Faraday Discussions
DOI	10.1039/c6fd00195e
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Subscribed
Subject Keyword	EPR ZSM-5 Mass spectrometry Gas chromatography\u2013mass spectrometry Methanol Reaction coordinate Adsorption Electron paramagnetic resonance Infrared spectroscopy Neutron diffraction Hydrocarbon
Content Type	Text
Resource Type	Article
Subject	Physics and Astronomy Physical and Theoretical Chemistry

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