(1)H and (13)C MAS NMR studies of light alkanes activation over MFI zeolite modified by Zn vapour.
The early stages of methane, ethane and propane conversion were studied by in situ (1)H and (13)C MAS NMR techniques over fully exchanged Zn(2+)/MFI catalyst obtained by the reaction with zinc vapour. The in situ techniques revealed strong interaction of alkanes with Zn(2+) cations evidenced by significant shift of the corresponding NMR lines. Besides that, the formation of methyl zinc, ethyl zinc and n-propyl zinc species along with bridging and silanol surface OH-groups was detected already at the ambient temperature. These results pointed to dissociative adsorption of alkanes over (ZO)-Zn(2+)-(OZ) and (ZO)-Zn(2+)-(OSi) active sites of the catalyst. The dissociative adsorption was shown to be a dead-end surface reaction in the case of methane starting reactant, while in the case of ethane and propane, it appeared to be responsible for the initiation of the catalytic cycle leading to alkenes and dihydrogen formation and regeneration of zinc containing catalytic sites.
Kolyagin
Yuriy G
YG
Department of Chemistry, Moscow State University, Lenin Hills 1/3, 119991 Moscow, Russia.
Ivanova
Irina I
II
Pirogov
Yuri A
YA
D000473:Alkanes / Q000737:chemistry*; D002247:Carbon Isotopes / Q000032:analysis / Q000737:chemistry*; D002384:Catalysis; D003198:Computer Simulation; D005740:Gases / Q000737:chemistry; D009682:Magnetic Resonance Spectroscopy / Q000379:methods*; D008956:Models, Chemical; D008958:Models, Molecular; D008968:Molecular Conformation; D011522:Protons; D017641:Zeolites / Q000032:analysis / Q000737:chemistry*; D015032:Zinc / Q000737:chemistry*
D000473:Alkanes; D002247:Carbon Isotopes; D005740:Gases; D011522:Protons; D017641:Zeolites; D015032:Zinc