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作 者:孙博[1] 郭勇[1] 徐乐[2] 黄哲昊[1] 吴鹏[2] 车顺爱[1]
机构地区:[1]上海交通大学化学化工学院金属基复合材料国家重点实验室,上海200240 [2]华东师范大学化学系上海市绿色化学与化工过程绿色化重点实验室,上海200062
出 处:《化学学报》2012年第23期2419-2424,共6页Acta Chimica Sinica
基 金:supported by the National Natural Science Foundation of China(Nos.20890121,20925310 and U1162102);Ministry of Science and Technology(Nos.2009CB930403 and 2012BAE05B02)~~
摘 要:利用简单微乳液自组装体系,制备了介孔二氧化硅与Y型或Ti-MWW沸石晶体复合形成的沸石/介孔二氧化硅微球(ZMMS).硅源正硅酸四丁酯与阳离子型季铵盐表面活性剂形成稳定的O/W微乳液形成大颗粒,沸石颗粒由于疏水作用而进入油相,同时,季铵盐表面活性剂和正硅酸四丁酯组装形成介孔材料.优化合成条件可以有效控制复合微球的沸石/介孔二氧化硅质量比(0~2.3)和直径(186~965μm).两种沸石/介孔二氧化硅复合微球材料的介孔孔径分别为3.98 nm(Y型沸石)和3.75 nm(Ti-MWW型沸石).Ti-MWW沸石/介孔二氧化硅复合微球在液相催化环氧化反应中表现出良好的机械强度,并且能够达到与Ti-MWW沸石原粉相当的催化活性.Zeolite/mesoporous silica composite microspheres (ZMMS) have been prepared by self-assembling mesoporous silica phase with Y or Ti-MWW zeolites crystallites in a simple microemulsion system. The synthesis process involved the formation of a stable OAV microemulsion from silica precursor of tetrabutyl orthosilicate and cationic quaternary ammonium surfactants as well as a simultaneous assembling of zeolite into the oil phase by their hydrophobic interaction, in which mesoporous silica was formed by self-assembling of surfactant and silica source. Through optimizing synthesis conditions, the ZMMS materials were prepared to possess controllable mass ratio of zeolite to mesoporous silica (0--2.3) and sphere diameter (186--965μm). The mesopore sizes of the ZMMSs were 3.75 (zeolite-Y/MMSs) and 3.98 nm (Ti-MWW/MMSs). In the liquid-phase ammoximation of cyclohexanone, Ti-MWW/mesoporous silica microspheres showed a high mechanical stability and a catalytic activity comparable to the parent Ti-MWW powders.
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