期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 41, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202207777
关键词
Ketene Chemistry; Ketene Methylation; Methanol to Olefins; Reaction Mechanism; Zeolites
资金
- National Natural Science Foundation of China [21903079]
- NCCR Catalysis [180544]
- Swiss National Science Foundation
- ETH-Bereich Forschungsanstalten
- PSI CROSS project funding initiative
In this study, the experimental detection of methylketene as the precursor of ethylene on HZSM-5 was reported, providing evidence for the computationally predicted ketene-to-ethylene reaction pathway.
Ketene (CH2=C=O) has been postulated as a key intermediate for the first olefin production in the zeolite-catalyzed chemistry of methanol-to-olefins (MTO) and syngas-to-olefins (STO) processes. The reaction mechanism remains elusive, because the short-lived ethenone ketene and its derivatives are difficult to detect, which is further complicated by the low expected ketene concentration. We report on the experimental detection of methylketene (CH3-CH=C=O) formed by the methylation of ketene on HZSM-5 via operando synchrotron photoelectron photoion coincidence (PEPICO) spectroscopy. Ketene is produced in situ from methyl acetate. The observation of methylketene as the ethylene precursor evidences a computationally predicted ketene-to-ethylene route proceeding via a methylketene intermediate followed by decarbonylation.
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