The "Alkyl" and "Carbenium" Pathways of Methane Activation on Ga-Modified Zeolite BEA: 13C Solid-State NMR and GC-MS Study of Methane Aromatization in the Presence of Higher Alkane Full article
| Journal |
The Journal of Physical Chemistry C
ISSN: 1932-7447 , E-ISSN: 1932-7455 |
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| Output data | Year: 2010, Volume: 114, Number: 49, Pages: 21555-21561 Pages count : 7 DOI: 10.1021/jp1078899 | ||
| Tags | TEMPERATURE NONOXIDATIVE ACTIVATION; DENSITY-FUNCTIONAL THEORY; SHORT-CHAIN ALKANES; NONFRAMEWORK GALLIUM; LIGHT ALKANES; CO-REACTANT; PROPANE; DEHYDROGENATION; HYDROCARBONS; REACTIVITY | ||
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| Affiliations |
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Funding (1)
| 1 | Russian Foundation for Basic Research | 10-03-00555 |
Abstract:
By using 13C solid-state NMR spectroscopy and GC-MS analysis, the activation of methane and coaromatization of methane and propane have been monitored on gallium-modified zeolite BEA at 573−823 K. A noticeable degree involvement of the 13C-label from methane-13C into the aromatic reaction products (benzene, toluene) has been demonstrated. The major intermediate of the methane activation represents gallium-methyl species, which are formed by methane dissociative adsorption on Ga2O3 species of the zeolite. The minor species of methane activation, Ga-methoxy groups, provide the involvement of methane into aromatics by the methylation of aromatic molecules, which are generated exclusively from propane, by the mechanism of electrophilic substitution. Ga-methyl species can serve as methylating nucleophilic agent for the reaction of nucleophilic substitution with participation of aromatic molecules, which contain the electron-withdrawing substitutes.
Cite:
Luzgin M.V.
, Gabrienko A.A.
, Rogov V.A.
, Toktarev A.V.
, Parmon V.N.
, Stepanov A.G.
The "Alkyl" and "Carbenium" Pathways of Methane Activation on Ga-Modified Zeolite BEA: 13C Solid-State NMR and GC-MS Study of Methane Aromatization in the Presence of Higher Alkane
The Journal of Physical Chemistry C. 2010. V.114. N49. P.21555-21561. DOI: 10.1021/jp1078899 WOS Scopus РИНЦ ANCAN OpenAlex
The "Alkyl" and "Carbenium" Pathways of Methane Activation on Ga-Modified Zeolite BEA: 13C Solid-State NMR and GC-MS Study of Methane Aromatization in the Presence of Higher Alkane
The Journal of Physical Chemistry C. 2010. V.114. N49. P.21555-21561. DOI: 10.1021/jp1078899 WOS Scopus РИНЦ ANCAN OpenAlex
Dates:
| Submitted: | Aug 20, 2010 |
| Accepted: | Oct 27, 2010 |
| Published online: | Nov 11, 2010 |
| Published print: | Dec 16, 2010 |
Identifiers:
| Web of science: | WOS:000284990800091 |
| Scopus: | 2-s2.0-78650281081 |
| Elibrary: | 16705776 |
| Chemical Abstracts: | 2010:1401196 |
| Chemical Abstracts (print): | 154:10400 |
| OpenAlex: | W2318053400 |