介孔钨锆复合氧化物载铂催化剂制备及其催化甘油氢解性能
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摘要
使用共沉淀-浸渍法制备介孔钨锆复合氧化物。通过X线衍射(XRD)、NH_3程序升温脱附(NH_3-TPD)、透射电子显微镜(TEM)和N_2物理吸附-脱附等方法对介孔钨锆复合氧化物进行表征。通过连续流动的固定床反应器考察钨锆复合氧化物载铂催化剂对甘油氢解反应的催化性能。结果表明:与商业Zr(OH)_4制备的钨锆复合氧化物相比,由共沉淀法制得的Zr(OH)_4制备的钨锆复合氧化物具有最大的总酸量和最多的弱酸含量。并且由共沉淀-浸渍法制备的介孔钨锆复合氧化物颗粒团聚现象较少,更加疏松分散,具有最大的介孔(17. 8 nm)、最小的平均粒径(9. 3 nm)和最大的比表面积(87 m~2/g),其在负载铂后对甘油氢解反应的活性也最高。
Mesoporous tungsten-zirconium composite oxides were prepared via coprecipitationimpregnation. The tungsten-zirconium composite oxides were characterized by X-ray diffraction( XRD),NH_3-temperature programmed desorption( NH_3-TPD),transmission electron microscope( TEM) and N_2 adsorption-desorption. Glycerol hydrogenolysis activity was evaluated over platinum-supported catalysts of a series of tungsten-zirconium composite oxides in a fixed-bed continuous flow reactor. Results showed that compared to the commercial zirconium hydroxide,the tungsten-zirconium composite oxide prepared with synthetic tetragonal zirconia had maximum total acidity,and maximum weak acidity percentage. The particles of the tungsten-zirconium composite oxide prepared with synthetic zirconium hydroxide dispersed well,the mesopore was maximum( 17. 8 nm),the average was minimum( 9. 3 nm) and specific surface area was maximum( 87 m~2/g). The activity of platinum-supported catalyst of the tungsten-zirconium composite oxide prepared with synthetic zirconium hydroxide was better than the others.
Mesoporous tungsten-zirconium composite oxides were prepared via coprecipitationimpregnation. The tungsten-zirconium composite oxides were characterized by X-ray diffraction( XRD),NH_3-temperature programmed desorption( NH_3-TPD),transmission electron microscope( TEM) and N_2 adsorption-desorption. Glycerol hydrogenolysis activity was evaluated over platinum-supported catalysts of a series of tungsten-zirconium composite oxides in a fixed-bed continuous flow reactor. Results showed that compared to the commercial zirconium hydroxide,the tungsten-zirconium composite oxide prepared with synthetic tetragonal zirconia had maximum total acidity,and maximum weak acidity percentage. The particles of the tungsten-zirconium composite oxide prepared with synthetic zirconium hydroxide dispersed well,the mesopore was maximum( 17. 8 nm),the average was minimum( 9. 3 nm) and specific surface area was maximum( 87 m~2/g). The activity of platinum-supported catalyst of the tungsten-zirconium composite oxide prepared with synthetic zirconium hydroxide was better than the others.
引文
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[6] HINO M,ARATA K. Synthesis of solid superacid of tungsten oxide supported on zirconia and its catalytic action for reactions of butane and pentane[J]. Journal of the Chemical Society,Chemical Communications,1988,18(18):1259.
[7] YORI J C,PARERA J M. Influence of the crystalline structure of Zr O2on the metallic properties of Pt in Pt/WO3-Zr O2catalysts[J]. Catalysis Letters,2000,65(4):205.
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[9] SUN W,ZHAO Z,GUO C,et al. Study of the alkylation of isobutane with n-butene over WO3/Zr O2strong solid acid:1.effect of the preparation method,WO3loading,and calcination temperature[J]. Industrial&Engineering Chemistry Research,2000,39(10):3717.
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[11] KOURIEH R,BENNICI S,MARZO M,et al. Investigation of the WO3/Zr O2surface acidic properties for the aqueous hydrolysis of cellobiose[J]. Catalysis Communications,2012,19:119.
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[16] TAGUCHI A,SCHUTH F. Ordered mesoporous materials in catalysis[J]. Microporous and Mesoporous Materials,2005,77(1):1.
[17] MELEZHYK O V,PRUDIUS S V,BREI V V. Sol-gel polymertemplate synthesis of mesoporous WO3/Zr O2[J]. Microporous and Mesoporous Materials,2001,49(1):39.
[18] SARKAR A,PRAMANIK S,ACHARIYA A,et al. A novel sol-gel synthesis of mesoporous Zr O2-Mo O3/WO3mixed oxides[J].Microporous and Mesoporous Materials,2008,115(3):426.
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