A surface functional monomer-directing strategy for highly dense imprinting of TNT at surface of silica nanoparticles
A surface functional monomer-directing strategy for highly dense imprinting of TNT at surface of silica nanoparticles
复制标题
二氧化硅纳米粒子表面高密度 TNT 印迹的表面功能单体导向策略
DOI：
10.1021/ja070975k
复制
发表时间：
2007-06-27
影响因子：
15
通讯作者：
Wang, Dapeng
中科院分区：
文献类型：
--
作者：
Gao, Daming;Zhang, Zhongping;Wang, Dapeng
本文报道了一种表面功能单体导向策略，用于2，4，6-三硝基甲苯(TNT)分子在二氧化硅纳米颗粒表面的高密度印迹。研究表明，二氧化硅表面的乙烯基官能单体层不仅可以通过乙烯基端基与功能单体的共聚反应在二氧化硅表面选择性地进行印迹聚合，而且可以通过TNT与功能单体层之间的电荷转移络合作用将TNT模板驱动到形成的聚合物壳层中。这两个基本过程导致了均匀的核壳TNT印迹纳米颗粒的形成，具有可控的壳层厚度和高密度的有效识别位点。吸附TNT分子的高容量和快速动力学表明，纳米壳层中的有效印迹位置密度是传统印迹粒子的近5倍。通过测试结合能力随壳厚度的变化，确定了最大结合能力的壳层厚度临界值，为分子印迹的有效性和印迹材料的形式提供了新的见解。这些结果不仅可以在分子印迹技术中得到广泛的应用，而且可以作为在二氧化硅载体上制备各种聚合物涂层的新策略的基础。
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.