两亲性Ti-V-β沸石的制备及其相界面催化反应性能的研究  

Amphiphilic Ti-V-β Zeolites: Preparation and Phase-boundary Catalysis

作　　者：肖质文[1] 李艳凤[1] 何震[1] 喻铃[1] 何红运[1] 

机构地区：[1]湖南师范大学化学生物学及中药分析教育部重点实验室,长沙410081

出　　处：《无机化学学报》2008年第11期1880-1884,共5页Chinese Journal of Inorganic Chemistry

基　　金：湖南省自然科学基金(No.08JJ3026)资助项目

摘　　要：采用三甲基氯硅烷(TMS)和正十八烷基三氯硅烷(OTS)对Ti-V-β沸石样品进行表面修饰,制备出了两亲性TMS-Ti-V-β和OTS-Ti-V-β沸石,通过XRD,FTIR,UV-Vis,SEM和低温氮气吸附-脱附等手段对样品进行了表征。同改性前样品相比,两亲性Ti-V-β沸石骨架未遭破坏,只是晶貌发生了一些改变。其BET比表面积和BJH孔容均稍有下降(Ti-V-β为428m2·g-1和0.54cm3·g-1,TMS-Ti-V-β为382m2·g-1和0.40cm3·g-1,OTS-Ti-V-β为290m2·g-1和0.28cm3·g-1)。这类两亲性沸石能分布于水、油两相界面处,在不加共溶剂及静置的反应条件下,对环己烯水化的相界面反应表现出优良的催化活性(环己烯的水合率和环己醇的选择性分别为:Ti-V-β0.61%和76%、OTS-Ti-V-β2.01%和90%、TMS-Ti-V-β7.35%和95%)。可以看出,三甲基氯硅烷改性后的TMS-Ti-V-β沸石在相界面催化反应中,具有比改性前高得多的活性。Amphiphilic TMS-Ti-V-β and OTS-Ti-V-β zeolites were prepared by modifying Ti-V-β zeolites with trimethylchlorosilane and n-octadecyhrichlorosilane, respectively. All the samples were characterized by XRD, FTIR, UV-Vis, SEM, and low temperature N2 adsorption-desorption. Modified samples retained their original crystal structure, while their crystal morphology was somewhat changed. N2 adsorption indicates that these amphiphilic zeolites have a little smaller surface area and BJH volume of pores compared with their parent zeolites（BET surface area and BJH volume of pores of zeolites are 428 m^2·g^-1 and 0.54cm^3·g^-1 for Ti-V-β, 382 m^2·g^-1 and 0.40 cm^3·g^-1 for TMS-Ti-V-β, and 290 m^2·g^-1 and 0.28 cm^3·g^-1 for OTS-Ti-V-β, respectively）. These amphiphilic Ti-V-β zeolites can be distributed at the water-organic phase boundary. They both show good catalytic performance in the phase- boundary reactions of cyclohexene hydration without co-solvents and stirring （the hydration yield of cyclohexene and the selectivity of cycloheanol are 0.61% and 76% for Ti-V-β, 2.01% and 90% for OTS-Ti-V-β, and 7.35% and 95% for TMS-Ti-V-β, respectively）. The experimental results indicate that the Ti-V-β zeolite modified with trimethylchlomsilane, TMS-Ti-V-β, has much higher catalytic activity than its parent Ti-V-β zeolite in the phase- boundary catalysis.

关 键 词：两亲性沸石 制备 相界面催化 

分 类 号：O611.4[理学—无机化学]