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π‐Interactions between Cyclic Carbocations and Aromatics Cause Zeolite Deactivation in Methanol‐to‐Hydrocarbon Conversion

Chao Wang, Min Hu, Yueying Chu, Xue Zhou, Qiang Wang, Guodong Qi, Shenhui Li, Jun Xu, Feng Deng

2020Angewandte Chemie International Edition63 citationsDOI

Abstract

The understanding of catalyst deactivation represents one of the major challenges for the methanol-to-hydrocarbon (MTH) reaction over acidic zeolites. Here we report the critical role of intermolecular π-interactions in catalyst deactivation in the MTH reaction on zeolites H-SSZ-13 and H-ZSM-5. π-interaction-induced spatial proximities between cyclopentenyl cations and aromatics in the confined channels and/or cages of zeolites are revealed by two-dimensional solid-state NMR spectroscopy. The formation of naphtalene as a precursor to coke species is favored due to the reaction of aromatics with the nearby cyclopentenyl cations and correlates with both acid density and zeolite topology.

Topics & Concepts

CarbocationZeoliteHydrocarbonMethanolChemistryChemical engineeringOrganic chemistryPhotochemistryMaterials scienceCatalysisEngineeringZeolite Catalysis and SynthesisAdvanced NMR Techniques and ApplicationsCatalysis and Oxidation Reactions