催化学报

催化学报 ›› 2007, Vol. 28 ›› Issue (10): 895-899.

• 研究论文 • 上一篇    下一篇

TS-1分子筛的无机法合成及其催化苯酚羟基化性能

张海娇,姚明恺,谢伟,刘月明,吴鹏   

  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
  • 收稿日期:2007-10-25 出版日期:2007-10-25 发布日期:2011-10-28

Synthesis of TS-1 Using Inorganic SiO2-TiO2 Precursor and Its Catalytic Performance for Hydroxylation of Phenol

ZHANG Haijiao, YAO Mingkai, XIE Wei, LIU Yueming*, WU Peng   

  1. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Department of Chemistry, East China Normal University, Shanghai 200062, China
  • Received:2007-10-25 Online:2007-10-25 Published:2011-10-28

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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48～72 h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.

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

Abstract: An inorganic SiO2-TiO2 precursor havingSi-O-Tibonds 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 usingX-raydiffraction, Fourier transform infrared spectroscopy, and ultraviolet-visible absorption spectroscopy showed that a higher proportion of titanium species in the precursor withSi-O-Tibonds 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.

Key words: TS-1, spontaneous dispersion, silica, titania, precursor, phenol, hydroxylation