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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 M2+-Smectite-Pd Materials and Catalytic Performance for Heck Reaction

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【作者】 王元瑞李亚丰贺岩峰赵旭

【Author】 WANG Yuan-rui1*,2,LI Ya-Feng1,HE Yan-feng1,ZHAO Xu2*(1.School of Chemical Engineering,Chang Chun University of Technology,Chang Chun 130012 China;2.College of Chemistry,Ji Lin University,Chang Chun 130012 China)

【机构】 长春工业大学化学工程学院吉林大学化学学院

【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%.

【Abstract】 The mesoporous Smectite materials containing M2+ ion(Co2+,Ni2+,Mg2+and Zn2+) are successfully synthesized via hydrothermal method.The results of XRD indicate that they are crystallized on typic Smectite 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 Co2+ 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 1h and the quantity is 5mg catalyst per 1mmol 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
【Key words】 SyntheticSmectiteImmobilizationPd complexCatalystHeck reaction
【基金】 吉林省科学技术厅资助项目(批准号:20070509)
  • 【文献出处】 分子催化 ,Journal of Molecular Catalysis , 编辑部邮箱 ,2009年06期
  • 【分类号】O643.32
  • 【被引频次】4
  • 【下载频次】145
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