文献类型：期刊文献

中文题名：硅烷化对Ti/HMS分子筛催化性能的影响

英文题名：Influence of Silylation on Catalytic Performance of Ti/HMS Molecular Sieve

作者：李学峰[1];高焕新[2];金国杰[2];丁琳[2];陈璐[2];杨洪云[2];何欣[2];陈庆龄[1]

机构：[1]华东理工大学化学与分子工程学院,上海200237;[2]中国石化上海石油化工研究院,上海201208

年份：2007

卷号：28

期号：6

起止页码：551

中文期刊名：催化学报

外文期刊名：CHINESE JOURNAL OF CATALYSIS

收录：CSTPCD;;Scopus;WOS:【SCI-EXPANDED(收录号:WOS:000248066300014)】；北大核心:【北大核心2004】；CSCD:【CSCD2011_2012】；

基金：国家重点基础研究发展规划(973计划;2003CB615805).

语种：中文

中文关键词：钛;HMS分子筛;水热合成;气相沉积;硅烷化;丙烯;环氧化

外文关键词：titanium; HMS molecular sieve; hydrothermal synthesis; chemical vapor deposition; silylation; propylene; epoxidation

摘要：分别用水热法和气相沉积法制备了Ti/HMS分子筛,采用三甲基氯硅烷(TMCS)和六甲基二硅氮烷(HMDSZ)对Ti/HMS样品进行了气相硅烷化,并用X射线衍射、N2吸附、红外光谱、29Si核磁共振和紫外-可见光谱对样品进行了表征.丙烯环氧化反应的测定结果表明,硅烷化可显著提高环氧化催化活性.水热法制备的Ti/HMS经HMDSZ硅烷化后的催化活性比经TMCS硅烷化后的稍高;气相沉积法制备的Ti/HMS经HMDSZ硅烷化后的催化活性远高于经TMCS硅烷化后的催化活性.这是由于TMCS不但能与分子筛表面的硅羟基反应,而且能破坏分子筛骨架中的Si-O-Ti甚至Si-O-Si键,形成新的羟基,导致样品的亲水性较强,同时还能对气相沉积法制备的Ti/HMS中的四配位骨架钛产生破坏作用.
Ti/HMS samples were prepared by hydrothermal synthesis （HTS） and chemical vapor deposition （CVD） methods and then silylated by trimethylchlorosilane （TMCS） and hexamethyldisilazane （HMDSZ） in a vapor phase. The samples were characterized by XRD, N2 adsorption, FT-IR, ^29Si NMR, and DRUV-Vis, and their catalytic performance for the epoxidation of propylene using cumene hydroperoxide as oxidant was measured. The silylation could promote remarkably the catalytic performance. The Ti/HMS silylated by HMDSZ had much higher catalytic activity than that silylated by TMCS. This is because TMCS could not only react with silanol but also break Si-O-Ti and Si-O-Si bonds to form new silanol, which led to higher hydrophilicity for the silylated samples than those silylated by HMDSZ. The silylation with TMCS partially destroyed the tetraco- ordinated framework titanium species in Ti/HMS, but this did not occur in the silylation with HMDSZ.