4.8 Article

Direct Mechanism of the First Carbon-Carbon Bond Formation in the Methanol-to-Hydrocarbons Process

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 56, Issue 31, Pages 9039-9043

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201703902

Keywords

methanol to hydrocarbons; NMR spectroscopy; reaction mechanisms; surface chemistry; zeolites

Funding

  1. National Natural Science Foundation of China [91545104, 21273230, 21473182, 21576256]
  2. Youth Innovation Promotion Association of the Chinese Academy of Sciences [2014165]

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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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