连续流动状态下纤维负载Pd(Ⅱ)催化Suzuki偶联反应的研究.pdfVIP

连续流动状态下纤维负载 （Ⅱ）催化 Pd Suzuki 偶联反应的研究 ［摘要］以偕胺肟化聚丙烯腈纤维（AOFs ）为载体，制备了纤维负载Pd （Ⅱ）催化剂AOFs-Pd （Ⅱ）。利用FTIR ，SEM ， EDS ，XPS ，ICP-OES 等方法对AOFs-Pd （Ⅱ）进行结构表征；研究了连续流动状态下AOFs-Pd （Ⅱ）催化卤代芳烃与苯硼 酸Suzuki 偶联反应的性能，考察了反应温度、反应物流量、卤代芳烃浓度及不同取代基的卤代芳烃对偶联产物收率与产量的 影响。实验结果表明，在连续流动状态下，AOFs-Pd （Ⅱ）具有良好的催化活性。偶联反应的最佳条件为：温度70 ℃、反应 物流量3 mL/min （即最佳停留时间6.67 min ）、卤代芳烃浓度60.0 mmol/L、乙醇-水（乙醇与水体积比为2 ∶1 ）为溶剂。在 此条件下，AOFs-Pd （Ⅱ）催化碘苯与苯硼酸Suzuki 偶联反应，碘苯的转化率高达97%，偶联产物的选择性为99%。催化剂 表现出良好的稳定性，连续反应20 h ，催化剂活性为694.29 mmol/ （g ·h ）；连续流动状态下，AOFs-Pd （Ⅱ）的催化效率 是间歇式反应的2.6 倍。 ［关键词］纤维负载Pd （Ⅱ）催化剂；连续流动；Suzuki 偶联反应 - ( Ⅱ) Research on fiber supported Pd catalyst for Suzuki coupling reaction under continuous flow conditions ［ ］Pd ( Ⅱ) complex supported by amidoxime polyacrylonitrile fibers(AOFs)(AOFs-Pd ( Ⅱ)) Abstract was synthesized. The structure of AOFs-Pd ( Ⅱ) was characterized by FTIR ，SEM ，EDS ，XPS and ICP-OES. The Suzuki coupling reaction of aryl halides and phenylboronic acid catalyzed by the AOFs- Pd ( Ⅱ) was investigated under continuous flow conditions. The effects of reaction temperature ， flow rate ，concentration and scope of substrate on yield and production of coupling product were investigated. Under the optimal reaction conditions ，namely flow rate of 3 mL/min(residence time is 6.67 min) ，aryl halides concentration of 60.0 mmol/L in a of co-solvent of EtOH/water(volume ratio 2 ∶1) at 70 ℃，the conversion of iodobenzene was up to 97% and the selectivity to the corresponding cross-coupling product can reach 99%. AOFs-Pd ( Ⅱ) catalyst showed good stability after a continuous operation time of 20 h ，and the catalytic efficiency of Pd was 694.29 mmol/(g·h) ，which was 2.6 times of that obtained with traditional batch reaction. ［ ］fiber supported-Pd ( Ⅱ) catalyst ；continuous flow ；Suzuki coup