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Studies on the Direct Methane Conversion over Supported Mo, V, and Ag Catalysts

Author: ZuoShaoJun
Tutor: BaoXinHe
School: Dalian Institute of Chemical Physics
Course: Physical and chemical
Keywords: methane activation selective oxidation Mo/MCM-22 VOx/SiO2 Ag/ZSM-5 Ag/SBA-15 O_γspecies nano silver particles
CLC: O643.32
Type: PhD thesis
Year: 2005
Downloads: 281
Quote: 2
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Abstract


Methane activation is of great industrial and scientific importance towards understanding the nature of scission of C-H of CH4, which is the most stable molecular in alkane family. The present work was focused on the study of methane direct conversion and four parts were included: （1） By combining the characterization results of the fresh and used Mo/MCM-22 catalysts and the time-on-stream reaction results for methane selective oxidation to C1-oxygenates, the following conclusions were drawn: the isolated tetrahedral molybdenum oxo-species is responsible for HCHO formation, while the octahedral polyoxomolybdate species will give rise to the total oxidation of methane. （2） VOx/SiO2 catalysts with different kinds of vanadia species were prepared with different methods and characterized in many respects and the fresh and used VOx/SiO2 catalysts were also compared. It was found that vanadia species were self-dispersed and partially reduced during methane selective oxidation. We also concluded that CO2 was produced via two mechanisms: One by the sequence reaction of CH4→HCHO→CO→CO2 over the monomeric vanadia species, and the other by the direct oxidation of methane to CO2 over the oligomeric vanadia species. （3） The different amounts of Ag+ were supported on zeolite with different methods and the nonoxidative coupling of methane was tested. It was found that isolated Ag+ ions play a crucial role in the catalytic coupling of methane under nonoxidative conditions, which was also confirmed by the result of DFT calculation.

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Chemical kinetics,catalysis > Catalytic > Catalytic reaction
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