Extra‐Framework Aluminum‐Assisted Initial C−C Bond Formation in Methanol‐to‐Olefins Conversion on Zeolite H‐ZSM‐5

Surface methoxy species bound to an extra‐framework Al (SMS‐EFAL) was unambiguously identified by advanced 13C‐{27Al} double‐resonance solid‐state NMR technique in the methanol‐to‐olefins reaction on H‐ZSM‐5 zeolite. The high reactivity of the SMS‐EFAL leads to the formation of surface ethoxy specie...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2018-08, Vol.57 (32), p.10197-10201
Main Authors: Wang, Chao, Chu, Yueying, Xu, Jun, Wang, Qiang, Qi, Guodong, Gao, Pan, Zhou, Xue, Deng, Feng
Format: Article
Language:English
Subjects:
Alkenes
Aluminum
Bonding
C−C bonds
Density functional theory
Ethanol
Ethene
Ethylene
Intermediates
Methanol
methanol conversion
NMR
Nuclear magnetic resonance
solid-state NMR
Zeolites
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Summary:Surface methoxy species bound to an extra‐framework Al (SMS‐EFAL) was unambiguously identified by advanced 13C‐{27Al} double‐resonance solid‐state NMR technique in the methanol‐to‐olefins reaction on H‐ZSM‐5 zeolite. The high reactivity of the SMS‐EFAL leads to the formation of surface ethoxy species and ethanol as the key intermediates for ethene generation in the early reaction stage. A direct route for the initial C−C bond formation in ethene was proposed and corroborated by density functional theory calculations. Surface methoxy species bound to an extra‐framework aluminum atom was identified to play a vital role in the initial C−C bond formation in the early stage of methanol‐to‐olefins conversion on zeolite H‐ZSM‐5. A direct formation pathway to ethene is revealed by the observation of surface ethoxy species and ethanol intermediates.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201805609