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Onset of Propene Oligomerization Reactivity in ZSM‑5 Studied by Inelastic Neutron Scattering Spectroscopy
journal contribution
posted on 2020-03-31, 00:13 authored by Alexander
P. Hawkins, Andrea Zachariou, Stewart F. Parker, Paul Collier, Ian P. Silverwood, Russell F. Howe, David LennonThe
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.
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Inelastic Neutron Scattering Spectroscopysystem mobilityquasi-elastic neutronchain growthhydrogen-bonded precursorrate-limiting stepinelastic neutronINS investigationsZSMidentificationOligomerization proceedswindow scan techniqueoligomerization reactionPropene Oligomerization Reactivitytemperature rangeQENSpropeneprotonationcatalyst activityformationacid site
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