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多级孔钛硅分子筛的合成
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摘要
多级孔钛硅分子筛由于具有多尺度的孔道分布,活性中心可接近性强,而在大分子化合物氧化反应中表现出良好的催化活性。在众多多级孔分子筛的制备方法中,直接合成法过程简单,容易实现。本研究通过在常规水热合成过程中直接引入无机铵盐扩孔,从而制备得到了多级孔钛硅分子筛。分析表征发现,与常规钛硅分子筛相比,合成的多级孔分子筛钛含量和晶型没有明显变化,但是锐钛矿型非骨架钛明显减少,插入到分子筛骨架的钛更多。研究还发现,多级孔分子筛具有双介孔分布。由TEM结果可以确认,多级孔钛硅分子筛的介孔主要是小晶粒之间聚集生长形成的晶间孔。在苯酚羟基化评价反应中,多级孔钛硅分子筛具有更高的邻苯二酚产物选择性,这表明分子筛的择型性能被削弱,晶内扩散性能得到增强,表现出多级孔分子筛的反应效果。由于具有高骨架钛含量和更宽的孔径分布,合成的多级孔钛硅分子筛具有较高的1-辛烯氧化催化活性。
Due to its wide pore size distribution and thus high accessibility to active centers,hierarchical TS-1 demonstrates good catalytic activity in large molecules oxidation reactions.In this presentation,ammonium salt is introduced to the traditional hydrothermal synthesis method to prepare hierarchical TS-1.Analysis results show that the Ti content and crystal structure of hierarchical TS-1 remain the same as traditional TS-1,but anatase content is clearly lower which indicates more Ti species are incorporated into framework.Furthermore,two different average size of mesoporous is found,and it is confirmed by TEM images that the intracrystalline pores of hierarchical TS-1 crystal are ascribed to the aggregation of small crystal particles.Higher ortho-product selectivity in phenol hydroxylation reaction and better catalytic performance in 1-octene oxidation reaction indicate improved mass transfer capability of hierarchical TS-1.
引文
[1]Li,K.;Valla J.;Garcia-Martinez,J.Chem.Cat.Chem.2014,6:46.

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