Characterization of Tungsten-Based Catalyst Used for Selective Oxidation of Cyclopentene to Glutaraldehyde

Abstract

Abstract: Tungsten-containing hexagonal mesoporous silica(W-HMS) supported tungsten oxide catalysts (WO_x/W-HMS) was prepared for the selective oxidation of cyclopentene with aqueous hydrogen peroxide to glutaraldehyde.X-ray diffraction(XRD) results indicated that the crystal form of the active phase(tungsten oxide) of the WO_x/W-HMS catalysts was dependent on the W loading and calcination temperature.X-ray photoelectron spectroscopy(XPS) analysis revealed that the dispersed tungsten oxides on the surface of W-HMS support consisted of a mixture of W(V) and W(VI).It was found that a high content of amorphous W species in(5+)oxidation state resulted in the high catalytic activity.When the Wloading was up to 12%(by mass) or the catalyst precursor was treated at temperature of 623 K,the catalytic activity decreased due to the presence of WO₃ crystallites and the oxidation of W(V) to W(VI) on the catalyst surface.Furthermore,NH₃-temperature-programmed-desorption (NH₃-TPD) analysis showed that the effects of W loading and calcination temperature on the acidity of the catalysts were related to the catalytic activity.Ahigh selectivity of 80.2% for glutaraldehyde with a complete conversion of cyclopentene was obtained over 8% WO_x/W-HMS catalyst calcined at 573 K after 14 h of reaction.

Key words: cyclopentene, glutaraldehyde, tungsten, hexagonal mesoporous silica, oxidation

摘要： Tungsten-containing hexagonal mesoporous silica(W-HMS) supported tungsten oxide catalysts (WO_x/W-HMS) was prepared for the selective oxidation of cyclopentene with aqueous hydrogen peroxide to glutaraldehyde.X-ray diffraction(XRD) results indicated that the crystal form of the active phase(tungsten oxide) of the WO_x/W-HMS catalysts was dependent on the W loading and calcination temperature.X-ray photoelectron spectroscopy(XPS) analysis revealed that the dispersed tungsten oxides on the surface of W-HMS support consisted of a mixture of W(V) and W(VI).It was found that a high content of amorphous W species in(5+)oxidation state resulted in the high catalytic activity.When the Wloading was up to 12%(by mass) or the catalyst precursor was treated at temperature of 623 K,the catalytic activity decreased due to the presence of WO₃ crystallites and the oxidation of W(V) to W(VI) on the catalyst surface.Furthermore,NH₃-temperature-programmed-desorption (NH₃-TPD) analysis showed that the effects of W loading and calcination temperature on the acidity of the catalysts were related to the catalytic activity.Ahigh selectivity of 80.2% for glutaraldehyde with a complete conversion of cyclopentene was obtained over 8% WO_x/W-HMS catalyst calcined at 573 K after 14 h of reaction.

关键词: cyclopentene, glutaraldehyde, tungsten, hexagonal mesoporous silica, oxidation

ZHU Zhiqing, BIAN Wei. Characterization of Tungsten-Based Catalyst Used for Selective Oxidation of Cyclopentene to Glutaraldehyde[J]. , 2008, 16(6): 895-900.

朱志庆, 卞炜. Characterization of Tungsten-Based Catalyst Used for Selective Oxidation of Cyclopentene to Glutaraldehyde[J]. , 2008, 16(6): 895-900.

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