Onset of Propene Oligomerization Reactivity in ZSM-5 Studied by Inelastic Neutron Scattering Spectroscopy

Alexander P Hawkins, Andrea Zachariou, Stewart F Parker, Paul Collier, Ian P Silverwood, Russell F Howe, David Lennon* (Corresponding Author)

*Corresponding author for this work

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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.

Original languageEnglish
Pages (from-to)7762-7770
Number of pages9
JournalACS Omega
Issue number14
Early online date30 Mar 2020
Publication statusPublished - 14 Apr 2020

Bibliographical note

Johnson Matthey PLC is thanked for supplying the ZSM-5 zeolite and for financial support through the provision of industrial CASE studentships in partnership with the EPSRC (A.P.H., no. EP/P510506/1; A.Z. no. EP/N509176/1). The Science and Technologies Facilities Council is thanked for the provision of neutron beamtime (allocation nos. RB1720047(35) and RB1720048(36)). The resources and support provided by the UK Catalysis Hub via membership of the UK Catalysis Hub consortium and funded by EPSRC (grant nos. EP/K014706/1, EP/K014668/1, EP/K014854/1, EP/K014714/1, and EP/M013219/1) are gratefully acknowledged.


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