固载Pd配合物的二元Smectite介孔材料的合成及催化Heck反应的性能研究  

Preparation of Mesoporous M^(2+)-Smectite-Pd Materials and Catalytic Performance for Heck Reaction

作　　者：王元瑞[1,2] 李亚丰[1] 贺岩峰[1] 赵旭[2] 

机构地区：[1]长春工业大学化学工程学院,长春130012 [2]吉林大学化学学院,长春130012

出　　处：《分子催化》2009年第6期517-522,共6页Journal of Molecular Catalysis(China)

基　　金：吉林省科学技术厅资助项目(批准号:20070509)

摘　　要：水热条件下合成了含M2+离子(Mg2+、Co2+、Ni2+和Zn2+)的介孔Smectite材料.经X射线粉末衍射和比表面积与孔隙率测定,确定了其晶体结构和孔性质.以配位体交换法固载金属Pd配合物———Pd(PhCH2CN)2Cl2,制备固载Pd配合物的Smectite介孔材料催化剂———SM(M)Pd.负载后平均孔径的测定结果表明,SM(M)Pd平均孔径均高于H-Mont-Pd平均孔径(3.70 nm),说明固载的Pd(PhCH2CN)2Cl2能够扩大H-Mont-Pd孔径.不同SM(M)Pd催化Heck偶联反应结果表明,SM(Co)Pd催化剂活性最好,这一方面与SM(Co)Pd具有最大的比表面积和孔容一致,另外也与Co2+电子结构有关.在该催化剂下,碘苯与丙烯酸甲酯的Heck偶联反应的适宜溶剂是N,N-二甲基乙酰胺(NMAC),反应温度为80℃,反应时间1 h,催化剂用量5 mg/mmol碘苯,5次重复使用催化剂活性没有下降,碘苯转化率接近100%.The mesoporous Smectite materials containing M^2＋ ion （ Co^2＋ , Ni^2 ＋ , Mg^2＋ and Zn^2 ＋ ） are successfully synthesized via hydrothermal method. The results of XRD indicate that they are crystallized on typic Smeetite structure. Then, the PdCl2 complex is immobilized on the these mesoporous Smectite materials by ligand exchange methods to get a kind of novel catalysis materials denoted as SM （M） Pd. Their catalytic performances for the Heck reaction between iodobenzene and methacrylate are investigated. The SM（Co） Pd exhibits the best catalytic activity, in consistence with its larger surface area and pore volume as well as Co^2＋ property. This prepared method has two features ： one is to embody the property of metal ion ; the other is that the immobilization improves the textural property of catalyst and prolongs the life of catalyst. The optimal reaction condition ： the proper solvent is N, N-dimethyl acetamide, the reaction temperature is at 80 ℃, reaction time is for 1 h and the quantity is 5mg catalyst per l mmol iodobenzene. The catalyst could be recovered after 5 times use without significant loss of its catalytic activity.

关 键 词：SMECTITE 固载 PD配合物 催化 HECK反应 

分 类 号：O643.32[理学—物理化学]