新型有机介孔材料FDU-15负载卡宾配体络合醋酸钯催化剂FDU-NHC/Pd(Ⅱ)的制备方法简单,通过三步反应即可制得,采用X射线衍射、N2吸附-脱附和透射电镜等手段对催化剂进行了表征,并考察了它在Sonogashira偶联反应中的催化性能.结果表明,功能化不影响FDU-15的有序介孔结构,仅其孔径、孔体积和BET比表面积有所减小.另外,该催化剂在Sonogashira偶联反应中表现出较高的催化活性,底物普适性好,无论足带有吸电r取代基还是供电子取代基的碘苯都能够得到较高的分离产率,且该催化剂分离简单,重复使用10次以上时,其催化性能基本保持不变.
Palladium catalyst systems are the most widely used for the formation of C-C and C-N bonds.Environmentally friendly heterogeneous palladium catalysts have strongly stimulated growth in this research area.Herein,a FDU (Fudan University)-15 mesopolymer with p6mm mesostructures that combine the advantages of organic polymers and mesoporous materials was investigated as a new solid support for Pd complexes.The FDU-15 mesopolymer-supported N-heterocyclic carbine (NHC) precursor was developed by a simple chemical functionalization approach.It has been used as a phosphine-free ligand to prepare the novel heterogeneous palladium catalyst FDU-NHC/Pd(Ⅱ),which efficiently catalyzes Sonogashira reactions between aryl halides and terminal alkynes to afford the corresponding products in good yields.Various techniques such as X-ray diffraction,N2 adsorption-desorption isotherms,high resolution transmission electron microscopy,and X-ray photoelectron spectroscopy have been used to characterize the catalyst.The results indicate that the mesoporous structure of FDU-15 was not affected by immobilization,however,the pore diameter,pore volume,and BET surface area decrease.The stability of the heterogeneous catalyst was also studied.The FDU-NHC/Pd(II) complex catalyst was easily separated from the reaction system by a simple filtration of the reaction mixture and it has been shown to be robust without a significant loss of catalytic activity after recycling and reuse in 10 times.
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