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苯乙烯-甲基丙烯酸羟基乙酯共聚物微球固载金属卟啉催化剂的制备及其催化性能

Metalloporphyrins Supported on Styrene-Hydroxyethyl Methacrylate Copolymer Microspheres:Preparation and Catalytic Performance for Hydroxylation of Cyclohexane

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【作者】 叶元坚黄锦汪蔡金华吴文海余汉城周贤太纪红兵计亮年

【Author】 YE Yuanjian,HUANG Jinwang,CAI Jinhua,WU Wenhai,YU Hancheng,ZHOU Xiantai, JI Hongbing,JI Liangnian MOE Key Laboratory of Bioinorganic and Synthetic Chemistry,School of Chemistry and Chemical Engineering, Sun Yat-Sen University,Guangzhou 510275,Guangdong,China

【机构】 中山大学生物无机与合成化学教育部重点实验室化学与化学工程学院

【摘要】 将酰氯化的羧基金属卟啉(MP)与表面含羟基的苯乙烯-甲基丙烯酸羟基乙酯共聚物微球(P(St-co-HEMA))进行酯化反应,制备了共聚物微球固载的金属卟啉催化剂(P(St-co-HEMA)MP).采用扫描电镜、紫外-可见光谱、红外光谱和热重等手段对微球进行了表征,并考察了它在"金属卟啉-抗坏血酸-分子氧"体系中催化环己烷羟化反应性能.结果表明,共聚物微球固载的金属卟啉比非固载的金属卟啉具有更高的催化活性,催化剂重复使用4次,仍保持较高催化活性.各共聚物微球固载的金属卟啉催化活性顺序为P(St-co-HEMA)FeP>P(St-co-HEMA)MnP>P(St-co-HEMA)CoP.

【Abstract】 A series of styrene-hydroxyethyl methacrylate copolymer (P(St-co-HEMA)) microsphere-immobilized metalloporphyrin (MP) were prepared by the esterification of a hydroxyl in copolymer microsphere surface with a carboxyl chloride in the porphyrin ring,and were characterized by scanning electron microscopy,UV-Vis spectroscopy,Fourier transformation infrared spectroscopy and thermal gravimetric analysis. The catalytic performance of these catalysts for cyclohexane hydroxylation in the metalloporphyrin-O2-ascorbic acid system was measured. The results indicated that the supported metalloporphyrins are more efficient than the non-supported ones and can retain their high turnover numbers after being reused four times. The catalytic activity of the immobilized catalysts follows the order of P(St-co-HEMA)FeP > P(St-co-HEMA)MnP > P(St-co-HEMA)CoP.

【关键词】 金属卟啉共聚物微球环己烷羟化
【Key words】 metalloporphyrincopolymer microspherecyclohexanehydroxylationironmanganesecobalt
【基金】 国家自然科学基金(29771034);广州市科技计划项目(2007J1-C0361)
  • 【文献出处】 催化学报 ,Chinese Journal of Catalysis , 编辑部邮箱 ,2010年12期
  • 【分类号】O643.32
  • 【被引频次】7
  • 【下载频次】348
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