odell-insightintothree-2019.pdf (1.75 MB)
Insight into three-coordinate aluminum species on ethanol-to-olefin Conversion over ZSM-5 Zeolites
journal contribution
posted on 2019-12-01, 00:00 authored by Z Wang, Luke O'DellLuke O'Dell, X Zeng, C Liu, S Zhao, W Zhang, M Gaborieau, Y Jiang, J HuangCommercial bioethanol can be readily converted into ethylene by a dehydration process using solid acids, such as Brønsted acidic H-ZSM-5 zeolites, and thus, it is an ideal candidate to replace petroleum and coal for the sustainable production of ethylene. Now, strong Lewis acidic extra-framework three-coordinate Al3+ species were introduced into H-ZSM-5 zeolites to improve their catalytic activity. Remarkably, Al3+ species working with Brønsted acid sites can accelerate ethanol dehydration at a much lower reaction temperature and shorten the unsteady-state period within 1–2 h, compared to >9 h for those without Al3+ species, which can significantly enhance the ethanol dehydration efficiency and reduce the cost. The reaction mechanism, studied by solid-state NMR, shows that strong Lewis acidic EFAl-Al3+ species can collaborate with Brønsted acid sites and promote ethanol dehydration either directly or indirectly via an aromatics-based cycle to produce ethylene.
History
Journal
Angewandte chemie - international editionVolume
58Issue
50Pagination
18061 - 18068Publisher
WileyLocation
Chichester, Eng.Publisher DOI
ISSN
1433-7851eISSN
1521-3773Language
engPublication classification
C1 Refereed article in a scholarly journalUsage metrics
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No categories selectedKeywords
Science & TechnologyPhysical SciencesChemistry, MultidisciplinaryChemistryacidityaluminumethanol to olefinMFI zeolitesolid-state NMR spectroscopySOLID-STATE NMRBRONSTED\/LEWIS ACID SYNERGYCATALYTIC DEHYDRATIONP-31 NMRALCOHOL DEHYDRATIONETHYLENE PRODUCTIONHYDROCARBON POOLSILICA-ALUMINASI\/AL RATIOH-ZSM-5
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