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碳纳米管上分子印迹微反应器的构建及催化Diels-Alder反应研究
Construction and Catalytic Properties of Molecular Imprinting Microreactor on Multiwalled Carbon Nanotubes for Diels-Alder Reaction

作  者: ; ; ; ; ; (文戈);

机构地区: 衡阳师范学院化学与材料科学系功能金属有机材料湖南省普通高等学校重点实验室

出  处: 《高等学校化学学报》 2011年第5期1157-1162,共6页

摘  要: 通过多壁碳纳米管(MWCNTs)上羟基的酯化反应在碳纳米管表面接枝双键,以蒽和马来酸的加成反应产物为模板分子,甲基丙烯酸(MAA)为功能单体,乙二醇二甲基丙烯酸酯(EDMA)为交联剂,通过微波辐射聚合在碳纳米管表面接枝一层厚度约为30 nm的分子印迹催化剂.该催化剂对蒽和马来酸的加成反应具有明显的催化作用,反应开始后的180 min内,催化反应速率是不加催化剂反应速率的1.77倍.该催化反应的催化动力学遵守Michaelis-Menten方程,最大速率(vmax)为0.713μmol/(L.s),米氏常数(KM)为17735.24μmol/L. The applications of molecularly imprinted polymers(MIPs) in synthesis and catalysis are being increasingly investigated.Conventional bulk polymerization often produces the polymer materials exhibiting low binding capacity,binding sites heterogeneity,and poor site accessibility.The use of nano-sized MIPs is expected to overcome these problems because nano-sized materials have a small dimension with high surface-to-volume ratio.The objective of this study is to construct molecular imprinting microreactor(MIM) in nanomaterials.In the first step,alkenyl multiwalled carbon nanotubes(MWCNTs) were prepared by esterification reaction of hydroxyl group of MWCNTs and methacryloyl chloride.Then,the molecular imprinted catalyst for Diels-Alder cycloaddition was fabricated on MWCNTs using alkenyl-MWCNTs as matrix,Diels-Alder cycloaddition product of anthracene and maleic acid as template molecule,methacrylic acid(MAA) and ethylene glycol dimethacrylate(EDMA) as functional monomer and cross-linker,respectively.The molecular imprinted catalyst exhibited catalytic activity for the cycloaddition reaction of anthracene and maleic acid.Compared with the uncatalyzed reaction,a rate enhancement of 1.77 fold was obtained.Plots of initial velocities of the cycloaddition versus substrate concentration showed typical Michaelis-Menten kinetics.In addition,the Michaelis constant(KM) and maximal rate(vmax) were calculated from Lineweaver-Burk plots to be 17735.24 μmol/L and 0.713 μmol/(L·s),respectively.

关 键 词: 分子印迹微反应器 多壁碳纳米管 环加成 催化

领  域: [理学] [理学]

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