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作 者:周炜[1] 孟凡磊[1] 须沁华[1] 董家騄[1] 淳远[1]
机构地区:[1]南京大学化学系,南京大学介观材料教育部重点实验室,南京210093
出 处:《化学学报》2004年第15期1425-1429,FJ03,共6页Acta Chimica Sinica
基 金:国家自然科学基金 (No.34456545);南京大学分析测试中心资助项目
摘 要:采用三甲基氯硅烷和正十八烷基三氯硅烷对TS 1沸石样品进行表面修饰 ,制备出了两亲性含钛沸石样品 .这类两亲性含钛沸石能分布于水、油两相界面处 .改性后样品的骨架未遭破坏 ,其中钛仍然保持了四配位骨架钛的状态 ,但其晶貌发生了某些改变 .这类两亲性样品在不加共溶剂及静置的反应条件下 ,对 1 辛烯和双氧水的相界面环氧化催化反应表现出优良的催化活性 .尤其是三甲基氯硅烷改性后的TS 1沸石 ,在相界面催化反应中 ,具有比改性前高得多的活性 .我们还发现 ,在该相界面催化反应条件中 ,相界面的面积和催化剂用量是两个最重要的影响因素 ,当相界面面积 (cm2 )与催化剂用量(mg)的比例控制在 0 .15左右时 ,两亲性TS 1沸石的催化活性达到最高值 .Amphiphilic TS-1 zeolites were prepared from TS-1 zeolite modified with trimethylchlorosilane and n-octadecyltrichlorosilane respectively. These amphiphilic zeolites were oriented at the water-organic boundary. Samples after modification retained their original crystal structure and Ti in these zeolites remained tetrahedral coordination, while the crystal morphology was changed. These amphiphilic Ti-containing zeolites showed good catalytic performance in the 1-octene and aqueous hydrogen peroxide phase-boundary epoxidation reaction without adding co-solvents and stirring. Especially by the TS-1 modified with trimethylchlonosilane, much higher catalytic activity was achieved than by parent TS-1 zeolite in the phase-boundary catalysis. In phase-boundary catalysis, the area of the phase-boundary and the amount of catalyst are the two important affecting factors. The amphiphilic TS-1 zeolite showed the highest catalytic activity when the ratio of the area of the phase-boundary (in cm(2)) to the usage of catalyst (in mg) was around 0.15.
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