Au/MOF-5催化剂在三组分偶联反应中的催化性能  

Supported Au/MOF-5: a highly active catalyst for three-component coupling reactions

作　　者：刘丽丽[1] 台夕市[1] 刘美芳[1] 李玉峰[1] 冯一民[1] 孙晓日[1] 

机构地区：[1]潍坊学院化学化工与环境工程学院,山东潍坊261061

出　　处：《化工学报》2015年第5期1738-1747,共10页CIESC Journal

基　　金：国家自然科学基金项目(21171132);山东省优秀中青年科学家科研奖励基金项目(2014BSB01061);潍坊市科学技术发展计划项目(201301035)~~

摘　　要：采用浸渍法制备了Au/MOF-5催化剂,用X射线衍射(XRD)、N2物理吸附、红外光谱(IR)、热重分析(TG-DTA)、电感耦合等离子体原子发射光谱(ICP-AES)和透射电镜(TEM)对催化剂进行表征,并探索其在醛、炔和胺三组分(A3)偶联反应中的催化性能。实验结果表明:Au/MOF-5对醛、炔和胺三组分偶联反应具有较好的催化活性,而且对产物炔丙基胺的选择性为100%。Au/MOF-5对反应底物具有较宽的适用范围,对于芳香醛和脂肪醛、二级胺和N-烷基取代苯胺、芳香炔和脂肪炔均具有较好的催化活性,而且对于吸电子芳香醛的催化活性大于供电子芳香醛。Au/MOF-5可以循环使用至少3次,催化活性变化不大。Gold was supported on a functionalized MOF-5 by impregnation method. The catalyst Au/MOF-5 was characterized by powder X-ray diffraction （XRD）, N2 adsorption-desorption, infrared spectra （IR）, thermogravimetric analysis and differential thermal analyses （TG-DTA）, transmission electro microscopy （TEM）, and inductivity coupled plasma （ICP）. Its catalytic performance was examined in one-pot synthesis of structurally divergent propargylaminesvia three component coupling of aldehyde, alkyne, and amine （A3） in 1,4-dioxane. The results showed that the Au/MOF-5 catalyst displayed high activity （high aldehyde consumption rate and turn-over number at 120℃： 18.7 mmol·（g Au）-1·h-1and 14.7, based on total gold content） and 100% selectivity for propargylamines. Various aromatic and aliphatic aldehydes were also able to undergo the A3 coupling on the catalyst Au/MOF-5. It was also found that the conversion of benzaldehyde was higher on the catalyst for aryl aldehydes with electron-withdrawing group bonded on benzene ring than for those with an electron-donating group. There was good conversion of benzaldehyde for secondary amines andN-alkyl aniline such as piperidine, pyrrolidine, morpholine, diethylamine, andN-methylaniline. It was also found that the conversion of benzaldehyde decreased with increasing chain length of straight-chain alkyl substituted phenylacetylene. Au/MOF-5 catalyst could be recycled at least three times, and the activity only decreased slightly.

关 键 词：配合物 催化剂 化学反应 活性 

分 类 号：O643[理学—物理化学]