期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 56, 期 31, 页码 9039-9043出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201703902
关键词
methanol to hydrocarbons; NMR spectroscopy; reaction mechanisms; surface chemistry; zeolites
资金
- National Natural Science Foundation of China [91545104, 21273230, 21473182, 21576256]
- Youth Innovation Promotion Association of the Chinese Academy of Sciences [2014165]
In the past two decades, the reaction mechanism of C-C bond formation from either methanol or dimethyl ether (DME) in the methanol-to-hydrocarbons (MTH) process has been a highly controversial issue. Described here is the first observation of a surface methyleneoxy analogue, originating from the surface-activated DME, by in situ solid-state NMR spectroscopy, a species crucial to the first C-C bond formation in the MTH process. New insights into the first C-C bond formation were provided, thus suggesting DME/methanol activation and direct C-C bond formation by an interesting synergetic mechanism, involving C-H bond breakage and C-C bond coupling during the initial methanol reaction within the chemical environment of the zeolite catalyst.
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