共缩聚法制备TEA-MCM-41介孔材料及其催化性能研究  

Study on the preparation of TEA-MCM-41 mesoporous material by co-condensation method and its catalytic performance

作　　者：张卫红[1] 陆明珠 邹凯 刘平[1] 陈小萱 Zhang Weihong;Lu Mingzhu;Zou Kai;Liu Ping;Chen Xiaoxuan(School of Petrochemical Engineering,Changzhou University,Changzhou 213164)

机构地区：[1]常州大学石油化工学院,常州213164

出　　处：《化工新型材料》2024年第3期203-208,213,共7页New Chemical Materials

基　　金：江苏省绿色催化材料与技术实验室开放课题(BM2012110);江苏省高等学校基础科学(自然科学)研究重大项目(23KJA530001)。

摘　　要：采用共缩聚“一锅法”合成出一系列硅基三乙胺离子液体固体碱性材料TEA-MCM-41(x)。通过傅里叶变换红外光谱仪、X射线衍射仪、热重分析仪、氮气吸附-脱附、X射线光电子能谱仪和Hammett指示剂等技术对TEA-MCM-41(x)的理化性质进行了表征。结果表明,正硅酸乙酯与硅基三乙胺离子液体发生了共缩聚反应,在模板剂十六烷基三甲基溴化铵作用下制备的材料具有典型的介孔结构、较大的比表面积和较窄的孔径分布。在茴香醛与丙二腈的Knoevenagel缩合反应中,离子液体负载量为10%(摩尔分数)的TEA-MCM-41(10)催化活性最高。以乙醇为溶剂,在TEA-MCM-41(10)用量为0.08mmol,茴香醛与丙二腈摩尔比为1∶1.25,反应温度为30℃、反应时间1h条件下,茴香醛可以定量转化成目标产物(4-甲氧基苯亚甲基)丙二腈,催化剂重复使用5次未发现明显失活。Through a co-condensation method,a series of silicon-based triethylamine(TEA)ionic liquid solid base materials[TEA-MCM-41(x)]were synthesized in a one-pot process.The physicochemical properties of the materials were characterized by Fourier transform infrared spectrometer,X-ray diffractometer,thermogravimetric analyzer,N 2 adsorption-desorption technique,X-ray photoelectron spectrometer and Hammett indicator.The analytic results indicated the material owned a typical mesoporous structure with large surface areas and narrow pore size distribution via co-condensation between ethyl orthosilicate and silicon-based triethylamine ionic liquid under the guidance of template agent CTAB.These TEA-MCM-41(x)materials were evaluated as catalysts in Knoevenagel condensation of anisaldehyde and malonitrile,in which TEA-MCM-41(10)with 10%TEA ionic liquid loading exhibited the superior catalytic activity.Under the optimum conditions:catalyst dosage of 0.08mmol,molar ratio of anisaldehyde to malonitrile of 1∶1.25,reaction temperature of 30℃and reaction time of 1h,anisaldehyde could be quantitatively converted into the target product(4-methoxybenzylidene)malononitrile.After five repeated uses,there was no obvious decline in catalytic activity.

关 键 词：介孔材料 三乙胺离子液体 功能化 共缩聚 KNOEVENAGEL缩合 

分 类 号：TQ032.4[化学工程]