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一种用于在二氧化硅纳米颗粒表面对TNT进行高密度印迹的表面功能单体导向策略。

A surface functional monomer-directing strategy for highly dense imprinting of TNT at surface of silica nanoparticles.

作者信息

Gao Daming, Zhang Zhongping, Wu Minghong, Xie Chenggen, Guan Guijian, Wang Dapeng

机构信息

Institute of Intelligent Machines, Chinese Academy of Sciences, Hefei, Anhui 230031, China.

出版信息

J Am Chem Soc. 2007 Jun 27;129(25):7859-66. doi: 10.1021/ja070975k. Epub 2007 Jun 6.

Abstract

This paper reports a surface functional monomer-directing strategy for the highly dense imprinting of 2,4,6-trinitrotoluene (TNT) molecules at the surface of silica nanoparticles. It has been demonstrated that the vinyl functional monomer layer of the silica surface can not only direct the selective occurrence of imprinting polymerization at the surface of silica through the copolymerization of vinyl end groups with functional monomers, but also drive TNT templates into the formed polymer shells through the charge-transfer complexing interactions between TNT and the functional monomer layer. The two basic processes lead to the formation of uniform core-shell TNT-imprinted nanoparticles with a controllable shell thickness and a high density of effective recognition sites. The high capacity and fast kinetics to uptake TNT molecules show that the density of effective imprinted sites in the nanoshells is nearly 5 times that of traditional imprinted particles. A critical value of shell thickness for the maximum rebinding capacity was determined by testing the evolution of rebinding capacity with shell thickness, which provides new insights into the effectiveness of molecular imprinting and the form of imprinted materials. These results reported here not only can find many applications in molecularly imprinting techniques but also can form the basis of a new strategy for preparing various polymer-coating layers on silica support.

摘要

本文报道了一种表面功能单体导向策略,用于在二氧化硅纳米颗粒表面对2,4,6-三硝基甲苯(TNT)分子进行高密度印迹。结果表明,二氧化硅表面的乙烯基功能单体层不仅可以通过乙烯基端基与功能单体的共聚作用,引导印迹聚合在二氧化硅表面选择性发生,还能通过TNT与功能单体层之间的电荷转移络合相互作用,将TNT模板驱入形成的聚合物壳层中。这两个基本过程导致形成具有可控壳层厚度和高密度有效识别位点的均匀核壳型TNT印迹纳米颗粒。对TNT分子的高吸附容量和快速动力学表明,纳米壳层中有效印迹位点的密度几乎是传统印迹颗粒的5倍。通过测试吸附容量随壳层厚度的变化,确定了最大再结合容量时壳层厚度的临界值,这为分子印迹的有效性和印迹材料的形式提供了新的见解。本文报道的这些结果不仅在分子印迹技术中有许多应用,而且可以构成在二氧化硅载体上制备各种聚合物涂层的新策略的基础。

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