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气相法二氧化硅负载胺-钯配合物的制备及对Heck反应催化性能的研究
引用本文:胡国辉,周健民,杨育林,李校堃,周仁贤,郑小明.气相法二氧化硅负载胺-钯配合物的制备及对Heck反应催化性能的研究[J].浙江大学学报(理学版),2009,36(5):561-565.
作者姓名:胡国辉  周健民  杨育林  李校堃  周仁贤  郑小明
作者单位:1. 温州医学院,药学院,浙江,温州,325035
2. 浙江大学,催化研究所,浙江,杭州,310028
基金项目:浙江省自然科学基金资助项目 
摘    要:以气相法二氧化硅为载体,链状胺和环胺为功能化试剂,制得一系列二氧化硅-胺基复合载体,通过配位反应得到二氧化硅负载胺-钯(Ⅱ)配合物,进一步还原得到二氧化硅负载胺-钯(0)配合物.采用IR、XRD、XPS、ICP技术对配合物进行表征,并研究了配合物的制备、反应条件以及配体差异对其催化碘苯与丙烯酸的Heck反应的性能.结果表明,该类催化剂在较低的温度下(70~90℃)即可较好地催化该反应,生成反式产物;还原后催化剂具有更好的催化活性和良好的重复使用性能;具有链状胺基配体的催化剂随着N原子数目的增加,催化活性呈上升趋势,而具有环状胺基配体的催化剂活性明显低于前者.

关 键 词:气相法二氧化硅  胺基配体  钯配合物  负载型催化剂  Heck反应

Synthesis of fumed silica supported amino-Pd complexes and their catalytic performance for Heck reaction
HU Guo-hui,ZHOU Jian-min,YANG Yu-lin,LI Xiao-kun,ZHOU Ren-xian,ZHENG Xiao-ming.Synthesis of fumed silica supported amino-Pd complexes and their catalytic performance for Heck reaction[J].Journal of Zhejiang University(Sciences Edition),2009,36(5):561-565.
Authors:HU Guo-hui  ZHOU Jian-min  YANG Yu-lin  LI Xiao-kun  ZHOU Ren-xian  ZHENG Xiao-ming
Institution:HU Guo-hui, ZHOU Jian-min, YANG Yu-lin, LI Xiao-kun, ZHOU Ren-xian, ZHENG Xiao-ming (1. School of Pharmacy, Wenzhou Medical College, Wenzhou 325035, Zhejiang Province, China ; 2. Institute of Catalysis, Zhejiang University, Hangzhou 310028, China)
Abstract:Using fumed silica as supporter, chain amino and cyclic amino as functional reagents, a series of fumed silica supported amino-palladium( Ⅱ ) complexes were prepared by coordination reaction followed by reduction. The catalysts were characterized by IR, XRD, XPS, ICP. The effect of the preparation condition and difference of ligand on the catalytic performance was studied. Its catalytic performance for Heck reaction of iodobenzene with acrylic acid showed that the catalyst has high activity at 70-90 ℃. The product takes E form. The catalyst after reduction had high catalytic activity and good recycling performance. With the increase of number of N atoms, there was a rising trend of catalytic activity for those catalysts which contain chain amino ligand. And the catalytic activity was much lower for those catalysts which contain cyclic amino ligand.
Keywords:fumed silica  amino ligand  Pd complex  supported catalyst  Heck reaction
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