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首页> 外文期刊>Journal of the American Chemical Society >Solvent Evaporation Induced Aggregating Assembly Approach to Three-Dimensional Ordered Mesoporous Silica with Ultralarge Accessible Mesopores
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Solvent Evaporation Induced Aggregating Assembly Approach to Three-Dimensional Ordered Mesoporous Silica with Ultralarge Accessible Mesopores

机译:具有超大可及中孔的三维有序介孔二氧化硅的溶剂蒸发诱导聚集组装方法

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摘要

A solvent evaporation induced aggregating assembly (EIAA) method has been demonstrated for synthesis of highly ordered mesoporous silicas (OMS) in the acidic tetra-hydrofuran (THF)/H_2O mixture by using poly(ethylene oxide)-b-poly(methyl methacrylate) (PEO-b-PMMA) as the template and tetraethylorthosilicate (TEOS) as the silica precursor. During the continuous evaporation of THF (a good solvent for PEO-b-PMMA) from the reaction solution, the template molecules, together with silicate oligomers, were driven to form composite micelles in the homogeneous solution and further assemble into large particles with ordered mesostructure. The obtained ordered mesoporous silicas possess a unique crystal-like morphology with a face centered cubic (fcc) mesostructure, large pore size up to 37.0 nm, large window size (8.7 nm), high BET surface area (508 m~2/g), and large pore volume (1.46 cm~3/g). Because of the large accessible mesopores, uniform gold nanoparticles (ca. 4.0 nm) can be introduced into mesopores of the OMS materials using the in situ reduction method. The obtained Au/OMS materials were successfully applied to fast catalytic reduction of 4-nitrophenol in the presence of NaHB_4 as the reductant. The supported catalysts can be reused for catalytic reactions without significant decrease in catalysis performance even after 10 cycles.
机译:已证明使用溶剂蒸发诱导聚集组件(EIAA)方法可通过使用聚(环氧乙烷)-b-聚(甲基丙烯酸甲酯)在酸性四氢呋喃(THF)/ H_2O混合物中合成高度有序的介孔二氧化硅(OMS) (PEO-b-PMMA)作为模板,原硅酸四乙酯(TEOS)作为二氧化硅前体。在从反应溶液中连续蒸发THF(PEO-b-PMMA的良溶剂)的过程中,模板分子与硅酸盐低聚物一起被驱动在均匀溶液中形成复合胶束,并进一步组装成具有规则介孔结构的大颗粒。获得的有序介孔二氧化硅具有独特的晶体状形态,具有面心立方(fcc)介孔结构,最大孔径可达37.0 nm,窗口尺寸较大(8.7 nm),BET表面积高(508 m〜2 / g) ,大孔体积(1.46 cm〜3 / g)。由于存在较大的中孔,因此可以使用原位还原方法将均匀的金纳米颗粒(约4.0 nm)引入OMS材料的中孔。在作为还原剂的NaHB_4存在下,将获得的Au / OMS材料成功应用于快速催化还原4-硝基苯酚。负载的催化剂即使在10个循环后也可以重新用于催化反应而不会显着降低催化性能。

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  • 来源
    《Journal of the American Chemical Society》 |2011年第50期|p.20369-20377|共9页
  • 作者单位

    Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Advanced Materials Lab,Fudan University, Shanghai 200433, China;

    Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Advanced Materials Lab,Fudan University, Shanghai 200433, China;

    Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Advanced Materials Lab,Fudan University, Shanghai 200433, China;

    Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Advanced Materials Lab,Fudan University, Shanghai 200433, China;

    Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Advanced Materials Lab,Fudan University, Shanghai 200433, China;

    Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Advanced Materials Lab,Fudan University, Shanghai 200433, China;

    Chemical Engineering Department, College of Engineering, King Saud University, Kingdom of Saudi Arabia;

    Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Advanced Materials Lab,Fudan University, Shanghai 200433, China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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