English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

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

MPS-Authors
There are no MPG-Authors in the publication available
External Resource
No external resources are shared
Fulltext (restricted access)
There are currently no full texts shared for your IP range.
Fulltext (public)
There are no public fulltexts stored in PuRe
Supplementary Material (public)
There is no public supplementary material available
Citation

Liu, Y., Müller, S., Berger, D., Jelic, J., Reuter, K., Tonigold, M., et al. (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.


Cite as: https://hdl.handle.net/21.11116/0000-000A-BC2F-F
Abstract
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.