TS-1分子筛的无机法合成及其催化苯酚羟基化性能  

Synthesis of TS-1 Using Inorganic SiO_2-TiO_2 Precursor and Its Catalytic Performance for Hydroxylation of Phenol

作　　者：张海娇[1] 姚明恺[1] 谢伟[1] 刘月明[1] 吴鹏[1] 

机构地区：[1]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：《催化学报》2007年第10期895-899,共5页

基　　金：国家自然科学基金(20473027);上海市科委(05DZ22306);国家重点基础研究发展计划(973计划;2006CB202508);高等学校博士学科点专项科研基金(20050269013);华东师范大学2006年优秀博士研究生培养基金

摘　　要：以无机固体硅胶和硫酸钛为原料,利用无机盐在多孔载体表面自发分散的基本原理,通过热处理先形成具有类似于钛硅分子筛Si-O-Ti键的无机SiO2-TiO2前驱体,然后以四丙基氢氧化铵为模板剂,通过水热晶化成功合成了TS-1分子筛.X射线衍射、傅里叶变换红外光谱和紫外-可见光谱表征表明,SiO2-TiO2前驱体中钛主要呈高分散状态,其中高分散的钛在水热晶化过程中基本进入了TS-1分子筛骨架,而以锐钛矿相存在的钛则基本不变.当SiO2-TiO2前驱体处理温度为450℃,SiO2/TiO2摩尔比为40,晶化温度为160～170℃,晶化时间为48～72h时,合成的TS-1分子筛对苯酚羟基化反应的催化活性最好,与经典有机法合成的TS-1分子筛的催化活性相当.An inorganic SiO2-TiO2 precursor having Si-O-Ti bonds similar to those present in titaniumsilicate molecular sieve was prepared through spontaneous dispersion of Ti（SO4）2 on amorphous porous silica by thermal treatment. A TS-1 molecular sieve was then synthesized successfully using the inorganic SiO2-TiO2 precursor by hydrothermal crystallization templated by tetrapropylammonium hydroxide. Characterization using X-ray diffraction, Fourier transform infrared spectroscopy, and ultraviolet-visible absorption spectroscopy showed that a higher proportion of titanium species in the precursor with Si-O-Ti bonds was incorporated into the TS-1 framework during the crystallization process, while the titanium species as a bulk TiO2 phase remained unchanged. Conditions affecting the catalytic performance of TS-1 were investigated in detail. The results indicated that the proper conditions were that the treatment temperature for precursor was about 450 ℃, the molar ratio of silica to titanium was 40, the crystallization temperature was about 160-170 ℃, and the crystallization time was about 48-72 h. TS-1 prepared under the above conditions showed that the activity for hydroxylation of phenol was comparable to TS-1 made by the classical method.

关 键 词：TS-1分子筛 自发分散 二氧化硅 二氧化钛 前驱体 苯酚 羟基化 

分 类 号：O643.32[理学—物理化学]