Highly ordered mesoporous zirconia-polyoxometalate nanocomposite materials for catalytic oxidation of alkenes

Highly ordered mesoporous zirconia-polyoxometalate nanocomposite materials for catalytic oxidation of alkenes
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DOI:
10.1039/c0jm03395b
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发表时间:
2011-02
影响因子:
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通讯作者:
G. Armatas;Georgios Bilis;M. Louloudi
G. Armatas;Georgios Bilis;M. Louloudi
中科院分区:
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文献类型:
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作者:
G. Armatas;Georgios Bilis;M. Louloudi

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通过表面活性剂辅助的溶胶-凝胶共聚法制备了一系列有序的介孔ZrO 2基杂多酸纳米复合材料。这些材料的孔壁由具有不同PMA负载量(即12、22和37重量%)的纳米晶四元ZrO 2和Keggin型12-磷钼酸(PMA)组分组成。小角X射线散射、高分辨透射电镜和N2物理吸附测量表明,介孔材料具有六方p6 mm对称性,具有大的内部BET表面积和窄尺寸的孔。根据EDX,FT-IR和漫反射UV/维斯/NIR光谱,掺入的PMA簇保持完整的Keggin结构到介孔框架中。所制备的ZrO 2-PMA纳米复合材料在氧化催化方面具有很大的应用潜力,在以过氧化氢为氧化剂的烯烃氧化反应中表现出优异的稳定性和催化活性。
A series of well-ordered mesoporous ZrO2-based heteropoly acid nanocomposite frameworks has been prepared through a surfactant-assisted sol–gel copolymerization route. The pore walls of these materials consist of nanocrystalline tetragonal ZrO2 and Keggin-type 12-phosphomolybdic acid (PMA) components with different PMA loadings, i.e. 12, 22 and 37 wt%. Small angle X-ray scattering, high-resolution TEM and N2 physisorption measurements indicated mesoporous property in hexagonal p6mm symmetry with large internal BET surface areas and narrow-sized pores. The incorporated PMA clusters preserve intact their Keggin structure into the mesoporous frameworks according to EDX, FT-IR and diffuse-reflectance UV/vis/NIR spectroscopy. The obtained ZrO2–PMA nanocomposites demonstrated great application potential in oxidative catalysis, exhibiting exceptional stability and catalytic activity in oxidation of alkenes using hydrogen peroxide as oxidant.