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

Suwardiyanto, , Howe, R. F., Gibson, E. K. , Catlow, C. R. A., Hameed, A., McGregor, J., Collier, P., Parker, S. F. and Lennon, D. (2017) An assessment of hydrocarbon species in the methanol-to-hydrocarbon reaction over a ZSM-5 catalyst. Faraday Discussions, 197, pp. 447-471. (doi: 10.1039/c6fd00195e) (PMID:28194458)

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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.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Gibson, Dr Emma and Lennon, Professor David
Authors: Suwardiyanto, , Howe, R. F., Gibson, E. K., Catlow, C. R. A., Hameed, A., McGregor, J., Collier, P., Parker, S. F., and Lennon, D.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Faraday Discussions
Publisher:Royal Society of Chemistry
ISSN:1359-6640
ISSN (Online):1364-5498
Published Online:14 February 2017
Copyright Holders:Copyright © 2017 The Royal Society of Chemistry
First Published:First published in Faraday Discussions 197:447-471
Publisher Policy:Reproduced under a Creative Commons License

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
557001Catalytic Science in the Harwell Research CentreDavid LennonEngineering & Physical Sciences Research Council (EPSRC)EP/I019693/1CHEM - CHEMISTRY
654181Catalytic HDO (UK Catalysis hub)Samuel JacksonEngineering & Physical Sciences Research Council (EPSRC)EP/K014706/1CHEM - CHEMISTRY
652891Towards closing the chlorine cycle in large-scale chemical manufacturing processes (UK Catalysis hub)David LennonEngineering & Physical Sciences Research Council (EPSRC)EP/K014854/1CHEM - CHEMISTRY