4.5 Article

Isobutane Transformation to Aromatics on Zn-Modified Zeolites: Intermediates and the Effect of Zn2+ and ZnO Species on the Reaction Occurrence Revealed by 13C MAS NMR

期刊

CHEMPHYSCHEM
卷 23, 期 1, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.202100587

关键词

isobutane; Zn-modified zeolite; aromatization and hydrogenolysis; C-13 MAS NMR; mechanism

资金

  1. Russian Science Foundation [19-43-04101]
  2. Deutsche Forschungsgemeinschaft [HA 1893/22-1]
  3. Russian Science Foundation [19-43-04101] Funding Source: Russian Science Foundation

向作者/读者索取更多资源

Different Zn species and zeolite topology have varying effects on alkane aromatization reactions, with Zn2+ species showing greater efficiency. The presence of more Bronsted acid sites in ZnO/H-BEA promotes the hydrogenolysis pathway.
To clarify the effects of different Zn species, zeolite topology and acidity (quantity of Bronsted acid sites, BAS) on alkane aromatization, isobutane transformation on Zn2+/H-ZSM-5, Zn2+/H-BEA, and ZnO/H-BEA zeolites has been monitored with C-13 MAS NMR. The alkane transformation has been established to occur by aromatization and hydrogenolysis pathways. Zn2+ species is more efficient for the aromatization reaction because aromatic products are formed at lower temperatures on Zn2+/H-BEA and Zn2+/H-ZSM-5 than on ZnO/H-BEA. The larger quantity of BAS in ZnO/H-BEA seems to provide a higher degree of the hydrogenolysis pathway on this catalyst. The mechanism of the alkane aromatization is similar for the zeolites of different topology and containing different Zn species, with the main reaction steps being the following: (i) isobutane dehydrogenation to isobutene via isobutylzinc; (ii) isobutene stabilization as a pi-complex on Zn sites; (iii) isobutene oligomerization via the alkene insertion into Zn-C bond of methyl-sigma-allylzinc formed from the pi-complex; (iv) oligomer dehydrogenation with intermediate formation of polyene carbanionic structures; (v) aromatics formation via further polyene dehydrogenation, protonation, cyclization, deprotonation steps with BAS involvement.

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