Hawkins, A. P. , Zachariou, A., Parker, S. F., Collier, P., Howe, R. F. and Lennon, D. (2021) Studies of propene conversion over H-ZSM-5 demonstrate the importance of propene as an intermediate in methanol-to-hydrocarbons chemistry. Catalysis Science and Technology, 11(8), pp. 2924-2938. (doi: 10.1039/D1CY00048A)
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Abstract
To investigate its role as an intermediate in methanol-to-hydrocarbons (MTH) chemistry, the reaction of propene over H-ZSM-5 zeolite at temperatures of 473, 573 and 673 K is studied over a period of 6 hours and the post-reaction catalysts examined by inelastic neutron scattering and ancillary analytical techniques. Low temperatures favour production of gasoline-range alkanes and alkenes, whilst the product distribution shifts to a primarily aromatic product stream as reaction temperature increases, with cyclopentadienyl intermediates from the aromatic formation process being detected spectroscopically in the reacted catalysts. The 473 K reaction deactivates the zeolite due to pore blockage from the growth of large, branched oligomer chains but coke build-up at higher temperatures is minimal and primarily consists of pure carbon. No evidence of immobilised poly-methylated aromatic species is observed at any temperature. A scheme for the full propene reaction series is proposed that involves a dual-cycle hydrocarbon pool mechanism like that found in MTH chemistry and supporting propene’s role as an intermediate in that process. Minor differences in the product distribution of the propene-only reactions compared to classical MTH chemistry are identified due to the lack of a significant methylation reaction pathway that results in a more restricted range of substituted products.
| Item Type: | Articles |
|---|---|
| Additional Information: | 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)). The resources and support provided by the UK Catalysis Hub via membership of the UK Catalysis Hubconsortium and funded by EPSRC grants EP/R026815/1 and EP/R026939/1 are gratefully acknowledged. |
| Status: | Published |
| Refereed: | Yes |
| Glasgow Author(s) Enlighten ID: | Zachariou, Miss Andrea and Lennon, Professor David and Hawkins, Alexander |
| Creator Roles: | Hawkins, A.Investigation, Methodology, Visualization, Writing – original draft Zachariou, A.Investigation, Methodology Lennon, D.Conceptualization, Funding acquisition, Project administration, Supervision, Writing – review and editing |
| Authors: | Hawkins, A. P., Zachariou, A., Parker, S. F., Collier, P., Howe, R. F., and Lennon, D. |
| College/School: | College of Science and Engineering > School of Chemistry |
| Journal Name: | Catalysis Science and Technology |
| Publisher: | Royal Society of Chemistry |
| ISSN: | 2044-4753 |
| ISSN (Online): | 2044-4761 |
| Published Online: | 01 March 2021 |
| Copyright Holders: | Copyright © 2021 Royal Society of Chemistry |
| First Published: | First published in Catalysis Science and Technology 11(8): 2924-2938 |
| Publisher Policy: | Reproduced under a Creative Commons License |
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