EFFICIENT SHAPE-SELECTIVE OXIDATIVE DESULFURIZATION BY PHOSPHOTUNGSTIC ACID/NANOCRYSTALLINE CATALYST TS-1

Abstract

Abstract: The catalyst (HPW-Nano-TS-1) with phosphotungstic acid (HPW) supported on nanocrystalline TS-1 was synthesized by impregnation method. The results of 31P MAS-NMR, FT-IR and UV-VIS characterization indicated that the preservation of the Keggin structure in HPW-Nano-TS-1 catalysts was confirmed. Catalytic oxidative desulfurization reaction and adsorption desulfurization over synthesized catalysts with model oil consisting of n-octane solution of organic sulfur was investigated. The time for the adsorption of thiophene, benzothiophene and dibenzothiophene over the nanocrystalline TS-1 and HPW-Nano-TS-1 samples gradually increased, and the saturated adsorption amount decreased accordingly. The introduction of HPW enhances the oxidative removal activity of nanocrystalline TS-1 for macromolecular dibenzothiophene. The removal rates of thiophene and dibenzothiophene were 98.5% and 58.0% at 60 °C, respectively. The order of removal of organic sulfide in the three models from easy to difficult is: thiophene > dibenzothiophene > benzothiophene, clearly different in the order of easy removal of benzothiophene from conventional microporous zeolite or polyoxometalate catalysts. It is due to the effects of shape-selectivity, diffusion effect as well as the electron cloud density of nanocrystalline TS-1 zeolite and HPW on the oxidation reaction of organic sulfur molecules.

Key words: Shape selectivity, oxidative desulfurization, polyoxometallate, nanocrystalline TS-1, hydrogen peroxide

CLC Number:

References

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