Onset of propene oligomerization reactivity in ZSM-5 studied by inelastic neutron scattering spectroscopy

Hawkins, A. P. , Zachariou, A., Parker, S. F., Collier, P., Silverwood, I. P., Howe, R. F. and Lennon, D. (2020) Onset of propene oligomerization reactivity in ZSM-5 studied by inelastic neutron scattering spectroscopy. ACS Omega, 5(14), pp. 7762-7770. (doi: 10.1021/acsomega.9b03503) (PMCID:PMC7160849)

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Abstract

The techniques of quasi-elastic and inelastic neutron scattering (QENS and INS) are applied to investigate the oligomerization of propene over a ZSM-5 zeolite. Investigations are performed at low temperatures, allowing identification of the onset of the oligomerization reaction and observation of the low-energy spectral changes due to intermediate formation that are difficult to observe by optical methods. Oligomerization proceeds via formation of a hydrogen-bonded precursor by an interaction of the propene with an internal acid site followed by protonation and chain growth with protonation being the rate-limiting step. The use of quasi-elastic neutron scattering to observe changes in system mobility with temperature via the elastic window scan technique allows identification of the active temperature range where catalyst activity commences and permits targeting of the more time-consuming INS investigations to conditions of interest. From examination of the product’s spectrum, the structure of the resulting oligomer is deduced to be primarily linear.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Zachariou, Miss Andrea and Lennon, Professor David and Hawkins, Alexander
Authors: Hawkins, A. P., Zachariou, A., Parker, S. F., Collier, P., Silverwood, I. P., Howe, R. F., and Lennon, D.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:ACS Omega
Publisher:American Chemical Society
ISSN:2470-1343
ISSN (Online):2470-1343
Published Online:30 March 2020
Copyright Holders:Copyright © 2020 American Chemical Society
First Published:First published in 5(14):7762-7770
Publisher Policy:Reproduced under a Creative Commons License

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
172233Anderson ICASE 2015 (Selex)Heather LambieEngineering and Physical Sciences Research Council (EPSRC)IND CASE EP/N509176/1S&E - Academic & Student Administration
302860INS studies of the interaction of propene with ZSM-5David LennonScience and Technology Facilities Council (STFC)RB1720047Chemistry
302861QENS studies of the interaction of propene with ZSM-5David LennonScience and Technology Facilities Council (STFC)RB1720048Chemistry
169321Catalytic HDO : Queen's University of Belfast ref R1188CCESamuel JacksonEngineering and Physical Sciences Research Council (EPSRC)EP/K014706/1Chemistry
167781MICA: Determining the therapeutic potential of targeting mTORC-1/2 in chronic lymphocytic leukaemia - a pre-clinical studyAlison MichieMedical Research Council (MRC)MR/K014854/1CS - Paul O'Gorman Leukaemia Research Centre