三丁基锡/SBA-15功能配合物的合成、表征及对Friedel-Crafts反应的选择性催化  

Synthesis,Characterization and Catalytic Performance Toward the Friedel-Crafts Acylation of Tributyltin Functionalized SBA-15

作　　者：荆涛[1] 覃志乐[1] 宋伟明[1] 赵云鹏[1] 邓启刚[1] 

机构地区：[1]齐齐哈尔大学化学与化学工程学院,齐齐哈尔161006

出　　处：《应用化学》2013年第8期945-950,共6页Chinese Journal of Applied Chemistry

基　　金：黑龙江省自然科学基金资助项目(B201010);黑龙江省教育厅(12511595)

摘　　要：将三丁基氯化锡与SBA-15介孔分子筛在N2气气氛中进行回流反应,得到有机锡无机配合物(C4H9)3Sn-O-SBA-15[Bu3SnS]。利用X射线衍射(XRD)、透射电子显微镜(TEM)、氮气吸附脱附、固体核磁(NMR)和吡啶吸附脱附红外光谱分析(Py-IR)等方法对产物的组成、结构和性质进行了表征。结果表明,产物Bu3SnS具有高度有序的六方介孔结构,与SBA-15相比,Bu3SnS比表面积、孔容和孔径变小,酸性增强。Bu3SnS对苯甲醚Friedel-Crafts酰基化反应具有优异的催化性能,当反应温度为130℃,n(苯甲醚)∶n(苯甲酰氯)=1.0∶2.0,w(cat)=6%(相对于苯甲醚用量),反应时间为5 h,苯甲醚的转化率达到76.0%,对甲氧基二苯酮(p-MBP)选择性达到97.8%。The organotin inorganic complexes （C4H9）3Sn-O-SBA-15[Bu3SnS] were successfully synthesized by grafting tributyltin on SBA-15 mesoporous molecular sieves in a nitrogen atmosphere. The composition, structure and properties of the samples were characterized by X-ray diffraction（XRD）, transmittance electron microscopy（TEM）, Hammett indicator method, N2 adsorption-desorption, solid nuclear magnetic resonance（NMR） , in-situ pyridine infrared spectroscopy（Py-IR） and so on. The results show that the hexagonal P6mm mesostructure of parent siliceous SBA-15 is maintained in Bu3SnS. The surface areas, proe size and volume of Bu3SnS are all deceased with the increase of acidity, compared to those of SBA-15. Friedel-Crafts acylation of anisole and benzoyl chloride can be efficiently catalyzed in the presence of Bu3SnS. The reaction conversion of anisole and the selectivity of p-benzoylanisole are 76.0% and 97.8%, respectively, when the molar ratio of anisole to benzoyl chloride is 0.5∶1.0, the amount of catalyst is 6%, the reaction temperature is 130 ℃ and the reaction time is 5 h.

关 键 词：三丁基锡 SBA-15 功能配合物 FRIEDEL-CRAFTS反应 选择性催化 

分 类 号：O643[理学—物理化学]