Intermediates in the methanol-to-hydrocarbons (MTH) reaction: a gas phase study of the unimolecular reactivity of multiply methylated benzenium cations

Svelle S, Bjorgen MA, Kolboe S, Kuck D, Letzel M, Olsbye U, Sekiguchi O, Uggerud E (2006)
CATALYSIS LETTERS 109(1-2): 25-35.

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Abstract
In order to reach a deeper insight into the reaction mechanism of the zeolite catalyzed methanol to hydrocarbons reaction (MTH), the proposed reaction intermediates, i.e., a series of multiply methyl-substituted benzenium ions has been generated in the gas phase by chemical ionization. The fragmentations of the corresponding long-lived (metastable) ions have been investigated. While expulsion of H-2 dominates for the lower homologues, elimination of methane dominates for the higher homologues, accompanied by increasing amounts CH3 center dot. Loss of larger fragments relevant to the MTH-reaction, in particular ethene, propene and even butene, is also observed in minor amounts. This latter finding is consistent with a proposed reaction cycle in the MTH reaction known as the paring mechanism, and the feasibility of this mechanism has thus been demonstrated. The metastable gas-phase ions studied here are considerably more energetic than those residing in a zeolite catalyst, but they were found to decompose with markedly higher selectivity towards alkenes as compared to those activated by collision-induced dissociation (CID).
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Svelle S, Bjorgen MA, Kolboe S, et al. Intermediates in the methanol-to-hydrocarbons (MTH) reaction: a gas phase study of the unimolecular reactivity of multiply methylated benzenium cations. CATALYSIS LETTERS. 2006;109(1-2):25-35.
Svelle, S., Bjorgen, M. A., Kolboe, S., Kuck, D., Letzel, M., Olsbye, U., Sekiguchi, O., et al. (2006). Intermediates in the methanol-to-hydrocarbons (MTH) reaction: a gas phase study of the unimolecular reactivity of multiply methylated benzenium cations. CATALYSIS LETTERS, 109(1-2), 25-35.
Svelle, S., Bjorgen, M. A., Kolboe, S., Kuck, D., Letzel, M., Olsbye, U., Sekiguchi, O., and Uggerud, E. (2006). Intermediates in the methanol-to-hydrocarbons (MTH) reaction: a gas phase study of the unimolecular reactivity of multiply methylated benzenium cations. CATALYSIS LETTERS 109, 25-35.
Svelle, S., et al., 2006. Intermediates in the methanol-to-hydrocarbons (MTH) reaction: a gas phase study of the unimolecular reactivity of multiply methylated benzenium cations. CATALYSIS LETTERS, 109(1-2), p 25-35.
S. Svelle, et al., “Intermediates in the methanol-to-hydrocarbons (MTH) reaction: a gas phase study of the unimolecular reactivity of multiply methylated benzenium cations”, CATALYSIS LETTERS, vol. 109, 2006, pp. 25-35.
Svelle, S., Bjorgen, M.A., Kolboe, S., Kuck, D., Letzel, M., Olsbye, U., Sekiguchi, O., Uggerud, E.: Intermediates in the methanol-to-hydrocarbons (MTH) reaction: a gas phase study of the unimolecular reactivity of multiply methylated benzenium cations. CATALYSIS LETTERS. 109, 25-35 (2006).
Svelle, S., Bjorgen, M. A., Kolboe, S., Kuck, Dietmar, Letzel, Matthias, Olsbye, U., Sekiguchi, O., and Uggerud, E. “Intermediates in the methanol-to-hydrocarbons (MTH) reaction: a gas phase study of the unimolecular reactivity of multiply methylated benzenium cations”. CATALYSIS LETTERS 109.1-2 (2006): 25-35.
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