|Place of Conferral||北京|
|Keyword||分子印迹技术 溶胶-凝胶法 洛克沙砷 硅胶载体 分子印迹复杂性|
洛克沙砷(Roxarsone，ROX)是一种持久性有机砷污染物，慢性砷接触会造成严重的身体健康危害，分子印迹技术(MIT)是一种制备和模板分子在三维空间结构上高度匹配，具有高度亲和力和选择性的高分子聚合物材料的技术，广泛应用于固相萃取、模拟酶催化和化学生物传感等领域。表面分子印迹是近年来广泛研究的一种分子印迹的手段，它弥补了传统印迹聚合物的缺点，将印迹位点暴露于载体材料的表面，可有效提高分子印迹聚合物(MIPs)的吸附容量和传质动力学性能，具有较好的应用前景。全文的主要工作包括以下四部分的内容：1) 第一章简要介绍了分子印迹技术的发展历程和现状，并对分子印迹技术的基本构成要素和基于分子印迹的新兴功能材料领域最新的研究成果做了简要综述。2) 第二章设计合成了对洛克沙砷(ROX)具有特异性识别作用的溶胶-凝胶表面分子印迹聚合物。通过在硅胶载体面接枝印迹有ROX的聚合物薄膜，得到对ROX具有特异性识别的功能材料MIP(ROX)。并对材料进行了扫描电镜(SEM)、傅里叶红外光谱(FT-IR)，静态吸附实验等表征。吸附性能测试显示：MIPs最大吸附容量和印迹因子分别达到70.9 mg/g和2.78，并且MIPs对ROX的选择性高于其结构类似物对羟基苯砷酸(OSA)和对氨基苯砷酸(ASA)。研究结果表明，所制备的MIPs对ROX具有较高的吸附容量和选择性，具有快的动力学吸附特性。并且，MIPs再生性能良好，经过5次循环重复利用后其对ROX的吸附容量仅降低了6.4%。所合成的分子印记聚合物对洛克沙砷的识别和吸附有较好的应用前景。3) 第三章采用与合成MIP(ROX)相同的策略合成了邻硝基苯砷酸分子印迹聚合物MIP(NAA)，对羟基苯砷酸分子印迹聚合物MIP(OSA)，并对MIP(ROX)、MIP(NAA)和MIP(OSA)三种材料的选择性识别性能做了详细的研究。发现目标分子结构以及溶剂的极性都会对分子印迹材料的识别能力造成影响。4) 第四章为对本文中工作的总结和展望。
Roxarsone (ROX) is one of the main persistent organic arsenic pollutants. Chronic arsenic exposure can cause serious health problems. Molecular imprinting technique (MIT) is a technique for preparing polymeric materials with high affinity and selectivity, which is well matched with template molecules in three-dimensional cavities. It is widely used in solid phase extraction, enzyme catalysis and chemical and biological sensing. Surface molecular imprinting technology has been developed in recent years, it is an alternative approach to solve issues of traditional imprinting polymer. In this process, the imprinting sites are exposed to the surface of the support materials, thus can effectively improve the adsorption capacity and mass transfer kinetics of the prepared molecular imprinting polymers (MIPs). The three main parts in this dissertation are as following:1) In chapter 1, the development and current status of molecular imprinting technology are introduced briefly. The basic components of molecular imprinting and the latest research progress in the field of functional materials design based on molecular imprinting are reviewed.2) In chapter 2, a sol-gel surface molecularly imprinted polymer with specific recognition of roxarone (ROX) was designed and synthesized. The molecularly imprinted polymers MIP (ROX) was prepared by grafting a polymer film imprinted with ROX on the surface of silica gel support. The prepared MIPs were characterized by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR) and static adsorption experiments. The maximum adsorption capacity and imprinting factor were obtained as 70.9 mg g-1 and 2.78, respectively. The MIPs had higher selectivity for ROX compared with its structurally analogues oxarsanilic acid (OSA) and arsanilic acid (ASA). Binding results indicated that the prepared MIPs exhibited high adsorption capacity and selectivity, and a fast binding kinetics for ROX. MIPs also showed a good regeneration performance. The adsorption capacity for ROX only decreased by 6.4% after 5 reused cycles showing good application potential for the recognition and adsorption of Roxarsone.3) In chapter 3, the molecularly imprinted polymers MIP (2-nitrophenylarsenic acid, NAA) and MIP (OSA) were synthesized by the same strategy as MIP (ROX), and the selective recognition properties of MIP (ROX), MIP (NAA) and MIP (OSA) were studied in detail. It is found that the target molecular structure and the polarity of the solvent will affect the recognition ability of the molecularly imprinted materials.4) Chapter 4 is a brief summary of this dissertation and outlook of the related work in the field.
|徐鲁. 溶胶-凝胶和表面印迹制备洛克沙砷分子印记聚合物及其性能研究[D]. 北京. 中国科学院大学,2018.|
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