Extra‐Framework Aluminum‐Assisted Initial C−C Bond Formation in Methanol‐to‐Olefins Conversion on Zeolite H‐ZSM‐5. Issue 32 (18th July 2018)

• Record Type: Journal Article
• Authors: Wang, Chao; Chu, Yueying; Xu, Jun; Wang, Qiang; Qi, Guodong; Gao, Pan; Zhou, Xue; Deng, Feng
• Is Part Of: Angewandte Chemie international edition. Volume 57:Issue 32(2018)
• Page Start: 10197
• Page End: 10201
• Publication Date: 2018-07-18
• Subjects: aluminum -- C−C bonds -- methanol conversion -- solid-state NMR -- zeolites; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201805609
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Surface methoxy species bound to an extra‐framework Al (SMS‐EFAL) was unambiguously identified by advanced 13 C‐{ 27 Al} 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. Abstract : 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.