Formation Mechanism of the First Carbon–Carbon Bond and the First Olefin in the 
Methanol Conversion into Hydrocarbons

Liu, Yue; Müller, Sebastian; Berger, Daniel; Jelic, Jelena; Reuter, Karsten; Tonigold, Markus; Sanchez-Sanchez, Maricruz; Lercher, Johannes A.

doi:10.1002/anie.201511678

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Formation Mechanism of the First Carbon–Carbon Bond and the First Olefin in the Methanol Conversion into Hydrocarbons

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引用

Liu, Y., Müller, S., Berger, D., Jelic, J., Reuter, K., Tonigold, M., Sanchez-Sanchez, M., & Lercher, J. A. (2016). Formation Mechanism of the First Carbon–Carbon Bond and the First Olefin in the Methanol Conversion into Hydrocarbons. Angewandte Chemie International Edition, 55(19), 5723-5726. doi:10.1002/anie.201511678.

引用: https://hdl.handle.net/21.11116/0000-000A-BC2F-F

要旨

The elementary reactions leading to the formation of the first carbon–carbon bond during early stages of the zeolite-catalyzed methanol conversion into hydrocarbons were identified by combining kinetics, spectroscopy, and DFT calculations. The first intermediates containing a C−C bond are acetic acid and methyl acetate, which are formed through carbonylation of methanol or dimethyl ether even in presence of water. A series of acid-catalyzed reactions including acetylation, decarboxylation, aldol condensation, and cracking convert those intermediates into a mixture of surface bounded hydrocarbons, the hydrocarbon pool, as well as into the first olefin leaving the catalyst. This carbonylation based mechanism has an energy barrier of 80 kJ mol⁻¹ for the formation of the first C−C bond, in line with a broad range of experiments, and significantly lower than the barriers associated with earlier proposed mechanisms.