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首页> 中文期刊> 《应用化学》 >胺化聚(苯乙烯-异丙烯膦酸)-磷酸氢锆轴向负载手性salen Mn(Ⅲ)的制备及其对α-甲基苯乙烯不对称环氧化反应的催化

胺化聚(苯乙烯-异丙烯膦酸)-磷酸氢锆轴向负载手性salen Mn(Ⅲ)的制备及其对α-甲基苯乙烯不对称环氧化反应的催化

         
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以聚(苯乙烯-异丙烯膦酸)-磷酸氢锆(ZPS-IPPA)为载体,通过对载体进行氯甲基化、胺化修饰后与手性Salen Mn(Ⅲ)轴向配位,合成了一种新的固载型手性Salen Mn(Ⅲ)催化剂. 采用FTIR、DR UV-Vis、XPS、SEM、TEM等测试技术对催化剂进行表征. 以次氯酸钠和间氯过氧苯甲酸为氧化剂,考察了固载催化剂对α-甲基苯乙烯不对称环氧化反应的催化性能. 结果表明,固载型催化剂的催化活性比相应均相催化剂略低,但对映体选择性明显提高. 在NaClO/PPNO氧化剂体系中0 ℃反应24 h,α-甲基苯乙烯环氧化反应的转化率达68%,对映选择性e.e.值达99%,循环使用8次后催化效果无明显降低.%Chiral Salen Mn(Ⅲ) complex was axially coordinated on diamine or polyamines modified Zirconium poly(styrene-isopropenyl phosphonate)-phosphates(ZPS-IPPA) by a covalent grafting method. All the supported heterogeneous chiral Salen Mn(Ⅲ) complexes prepared were characterized by FT-IR, diffusion reflection UV-Vis, XPS, SEM and TEM. The supported catalyst was applied to the enantioselective epoxidation of α-methylstyrene with NaClO and m-CPBA as oxidants. The results confirm that the activity of the supported catalyst was lower than that of the homogeneous chiral Salen Mn( Ⅲ). However, its enantioselecti-vity was higher than that of the homogeneous one. A conversion of 68% and an e.e. of 99% of epoxide were obtained when α-methylstyrene was oxidized by NaClO for 24 h at 0 ℃ in the presence of 4-PPNO. The catalysts were easily recovered by filtration and could be reused for at least eight times with little loss of activity and enantioselectivity.

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