Effect of steam de-alumination on the interactions of propene with H-ZSM-5 zeolites

Russell Howe; Alex  Hawkins; Andrea Zachariou; Stewart F. Parker; P. Collier; Nathan Barrow; Ian Philip  Silverwood; David Lennon

doi:10.1039/D0RA03871G

Effect of steam de-alumination on the interactions of propene with H-ZSM-5 zeolites

Russell Howe, Alex Hawkins, Andrea Zachariou, Stewart F. Parker, P. Collier, Nathan Barrow, Ian Philip Silverwood, David Lennon^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

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Abstract

Steam de-alumination is used to prepare a H-ZSM-5 material representative of industrial acid zeolite catalysts. Characterisation shows extensive loss of zeolite acidity but minimal loss of framework crystallinity in the treated material. The material's interaction with propene is probed by means of inelastic and quasielastic neutron scattering, providing information on the reactivity and mobility of the propene respectively. These results are compared to those previously obtained for propene in the untreated zeolite. The steaming treatment resulted in decreased reactivity of the zeolite toward olefin oligomerization, higher temperatures for reaction initiation, and increased mobility of the propene in the zeolite at all temperatures. Analysis of the motions of the propene revealed by QENS shows the mobility to be comparable to those previously reported for propane in similar materials but occurring at slower velocities due to the greater rigidity and polarisation of the propene molecule.

Original language	English
Pages (from-to)	23136-23147
Number of pages	12
Journal	RSC Advances
Volume	10
Issue number	39
Early online date	17 Jun 2020
DOIs	https://doi.org/10.1039/D0RA03871G
Publication status	Published - Jun 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 (APH (EP/P510506/1, AZ (EP/N509176/1))). Experiments at the ISIS Neutron and Muon Source were made possible by beam time allocations from the Science and Technologies Facilities Council.58–60 We thank Dr Gavin Stenning of the ISIS Materials Characterisation Laboratory for assistance with XRD data collection. The resources and support provided by the UK Catalysis Hub via membership of the UK Catalysis Hub consortium and funded by EPSRC grants EP/R026815/1 and EP/R026939/1 are gratefully acknowledged. This research has been performed with the use of facilities and equipment at the Research Complex at Harwell; the authors are grateful to the Research Complex for this access and support.

Keywords

ELASTIC NEUTRON-SCATTERING
MOLECULAR-DYNAMICS SIMULATION
CATALYTIC CRACKING
LOW-TEMPERATURE
ZSM-5
OLIGOMERIZATION
DIFFUSION
HYDROCARBONS
PROPANE
OLEFINS

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Hawkins_etal_RSC_Effect_of_steam_VOR
This article is Open Access https://creativecommons.org/licenses/by/4.0/
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Cite this

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title = "Effect of steam de-alumination on the interactions of propene with H-ZSM-5 zeolites",

abstract = "Steam de-alumination is used to prepare a H-ZSM-5 material representative of industrial acid zeolite catalysts. Characterisation shows extensive loss of zeolite acidity but minimal loss of framework crystallinity in the treated material. The material's interaction with propene is probed by means of inelastic and quasielastic neutron scattering, providing information on the reactivity and mobility of the propene respectively. These results are compared to those previously obtained for propene in the untreated zeolite. The steaming treatment resulted in decreased reactivity of the zeolite toward olefin oligomerization, higher temperatures for reaction initiation, and increased mobility of the propene in the zeolite at all temperatures. Analysis of the motions of the propene revealed by QENS shows the mobility to be comparable to those previously reported for propane in similar materials but occurring at slower velocities due to the greater rigidity and polarisation of the propene molecule.",

keywords = "ELASTIC NEUTRON-SCATTERING, MOLECULAR-DYNAMICS SIMULATION, CATALYTIC CRACKING, LOW-TEMPERATURE, ZSM-5, OLIGOMERIZATION, DIFFUSION, HYDROCARBONS, PROPANE, OLEFINS",

author = "Russell Howe and Alex Hawkins and Andrea Zachariou and Parker, {Stewart F.} and P. Collier and Nathan Barrow and Silverwood, {Ian Philip} and David Lennon",

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 (APH (EP/P510506/1, AZ (EP/N509176/1))). Experiments at the ISIS Neutron and Muon Source were made possible by beam time allocations from the Science and Technologies Facilities Council.58–60 We thank Dr Gavin Stenning of the ISIS Materials Characterisation Laboratory for assistance with XRD data collection. The resources and support provided by the UK Catalysis Hub via membership of the UK Catalysis Hub consortium and funded by EPSRC grants EP/R026815/1 and EP/R026939/1 are gratefully acknowledged. This research has been performed with the use of facilities and equipment at the Research Complex at Harwell; the authors are grateful to the Research Complex for this access and support. ",

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doi = "10.1039/D0RA03871G",

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AU - Zachariou, Andrea

AU - Parker, Stewart F.

AU - Collier, P.

AU - Barrow, Nathan

AU - Silverwood, Ian Philip

AU - Lennon, David

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N2 - Steam de-alumination is used to prepare a H-ZSM-5 material representative of industrial acid zeolite catalysts. Characterisation shows extensive loss of zeolite acidity but minimal loss of framework crystallinity in the treated material. The material's interaction with propene is probed by means of inelastic and quasielastic neutron scattering, providing information on the reactivity and mobility of the propene respectively. These results are compared to those previously obtained for propene in the untreated zeolite. The steaming treatment resulted in decreased reactivity of the zeolite toward olefin oligomerization, higher temperatures for reaction initiation, and increased mobility of the propene in the zeolite at all temperatures. Analysis of the motions of the propene revealed by QENS shows the mobility to be comparable to those previously reported for propane in similar materials but occurring at slower velocities due to the greater rigidity and polarisation of the propene molecule.

AB - Steam de-alumination is used to prepare a H-ZSM-5 material representative of industrial acid zeolite catalysts. Characterisation shows extensive loss of zeolite acidity but minimal loss of framework crystallinity in the treated material. The material's interaction with propene is probed by means of inelastic and quasielastic neutron scattering, providing information on the reactivity and mobility of the propene respectively. These results are compared to those previously obtained for propene in the untreated zeolite. The steaming treatment resulted in decreased reactivity of the zeolite toward olefin oligomerization, higher temperatures for reaction initiation, and increased mobility of the propene in the zeolite at all temperatures. Analysis of the motions of the propene revealed by QENS shows the mobility to be comparable to those previously reported for propane in similar materials but occurring at slower velocities due to the greater rigidity and polarisation of the propene molecule.

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KW - OLIGOMERIZATION

KW - DIFFUSION

KW - HYDROCARBONS

KW - PROPANE

KW - OLEFINS

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U2 - 10.1039/D0RA03871G

DO - 10.1039/D0RA03871G

M3 - Article

SN - 2046-2069

VL - 10

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EP - 23147

JO - RSC Advances

JF - RSC Advances

IS - 39

ER -

Effect of steam de-alumination on the interactions of propene with H-ZSM-5 zeolites

Abstract

Bibliographical note

Keywords

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