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Establishing a Link Between the Dual Cycles in Methanol-to-Olefins Conversion on H‑ZSM-5: Aromatization of Cycloalkenes
journal contribution
posted on 2020-03-20, 14:03 authored by Min Hu, Chao Wang, Xiuzhi Gao, Yueying Chu, Guodong Qi, Qiang Wang, Guangtong Xu, Jun Xu, Feng DengThe
aromatization of alkenes in the methanol-to-olefins (MTO) reaction
on H-ZSM-5 zeolites was investigated by solid-state NMR and GC-MS
spectroscopy. The formed cycloalkenes including cyclopentene and cyclohexene
in the MTO reaction show high reactivity toward formation of aromatics.
Cyclohexene tends to form cyclopentene through ring contraction, and
the subsequent ring expansion leads to the production of aromatics.
The ring-contraction/expansion process of cyclohexene is consistent
with the 13C isotopic scrambling in aromatics. Solid-state
NMR experiments evidenced the formation of cyclopentenyl cations and
benzenium ions intermediates in the aromatization of C6 cycloalkenes.
A plausible route to link the alkene-based and aromatic-based cycles
in the MTO reaction on ZSM-5 zeolite was proposed, which is corroborated
by DFT calculations.
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benzenium ions intermediatesSolid-state NMR experimentsZSMcyclohexeneGC-MS spectroscopyring contractionform cyclopentenearomatic-based cycleszeoliteDFT calculations13 CC 6 cycloalkenescyclopentenyl cationsDual CyclesMethanol-to-Olefins ConversionH-ZSMMTO reaction showring expansionMTO reactionformationaromatization
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