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高活性氨基胍树脂负载Pd(0)配合物的催化性能研究

Catalytic Characteristics of Highly Active Amino-guanidine-resin Supported Pd(0) Complex

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【作者】 杨元法卢茂玲曾朝霞刘卫东周凤羽罗孟飞

【Author】 YANG, Yuan-Fa* LU, Mao-Ling ZENG, Zhao-Xia LIU, Wei-Dong ZHOU, Feng-Yu LUO, Meng-Fei (Institute of Physical Chemistry, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Zhejiang Normal University, Jinhua 321004)

【机构】 浙江师范大学物理化学研究所浙江省固体表面反应化学重点实验室浙江师范大学物理化学研究所浙江省固体表面反应化学重点实验室 金华321004金华321004

【摘要】 以氨基碳酸胍改性氯球为载体,与氯化钯溶液反应并还原制备氨基胍树脂负载钯(0)催化剂.对催化剂进行了FT-IR,XRD,BET,TG-DTA表征.研究了该催化剂对各种取代卤代苯与丙烯酸、苯乙烯的Heck芳基化反应催化性能.实验结果表明,该催化剂对活性(吸电子基)溴代苯和碘苯具有良好的催化活性,对含活性吸电子基的溴代苯(4-溴苯甲醛和4-溴硝基苯)于140℃时能在22min内完成Heck芳基化反应;催化剂具有较好的重复使用性能,在90℃下催化碘苯与丙烯酸的反应循环21次时仍能保持良好的催化活性.反应机理研究表明:催化反应的活性组分是可溶性钯物种;可溶性钯是由卤代苯与催化剂表面上的钯氧化加成所致.

【Abstract】 Amino-guanidine-resin supported Pd(0) was prepared by the reaction of amino-guanidine modi- fied chloromethyl polystyrene resin with PdCl2, followed by reduction. The catalyst was characterized by FT-IR, XRD, BET, TG-DTA. The catalytic performance for the Heck reactions of various substituted aryl halides with acrylic acid or styrene was studied. Experiments indicated that the catalyst had excellent activ- ity and recycling. Aryl bromides with electron-withdrawing were converted completely within very short time (140 ℃ , 22 min). At 90 ℃ in the reaction of iodobenzene with acrylic acid, the catalyst could kept high activity at 21th run. The study on mechanism disclosed that the reaction was homogeneous catalytic reac- tion, and the palladium leaching was caused by the interaction of iodobenzene with the metal Pd(0) on sup- ported.

【基金】 浙江省自然科学基金(No.M203146)资助项目.
  • 【文献出处】 有机化学 ,Chinese Journal of Organic Chemistry , 编辑部邮箱 ,2007年02期
  • 【分类号】O643.32
  • 【被引频次】8
  • 【下载频次】213
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