磁性强化分子印迹纳米材料应用于去除垃圾渗滤液中环境激素的效能与机理研究

Environmental hormone can induce harmful biological effects on human body. The leak out of leachate from landfill is an important way for the invading of environmental hormone to aquatic environment, and the improper handling would lead to threaten the health of human beings. In this research project, we study on magnetic molecular imprinted nanomaterials (MMINs) based adsorption-enrichment process, which is promising in specifically removing environmental hormone from landfill leachate, recycling the MMINs efficiently, and investigating the process control as well as mechanism explore. This work mainly includes that, (1) the selection of imprinting system and polymerization process, and its influence on the efficiency of MMINs, (2) process control and optimization of operation parameters in specifically removal of environmental hormone in landfill leachate, (3) adsorption behavior of MMINs on environmental hormone, (4) MMINs regeneration and its efficiency. In addition, aim at the polar environment, in which the principal component such as high concentration soluble organics and xenobiotics are coexistence, several key scientific issues such as the design and screening of imprinting system, which could influence the efficiency of MMINs, will be deeply studied. The mechanism of regeneration of MMINs will be analyzed profoundly. It will provide theoretical and applied foundation for research and development of specifically removal of environmental hormone in landfill leachate by MMINs, which offers a good guider in practical application. Therefore, it has important theoretical and practical application prospects.

环境激素可对人体产生有害的生物学效应，垃圾填埋场的渗滤液渗出是环境激素进入水环境的一个重要途径，若处理不当将会对人类健康造成威胁。本项目采用磁性强化分子印迹纳米材料（MMINs）处理垃圾渗滤液中的环境激素，并进行工艺控制过程的研究与作用机理的探讨，以期实现对环境激素的特异性高效富集去除与材料的循环使用。主要内容包括：（1）印迹体系与聚合方法的选择及其对MMINs的效能影响研究；（2）特异性去除垃圾渗滤液中环境激素的过程控制和条件优化；（3）MMINs对环境激素的吸附行为研究；（4）MMINs的再生方法及效能研究。针对垃圾渗滤液的高浓度溶解性有机物、异型生物质等主成分共存的复杂极性环境，进行印迹体系的设计、筛选等影响MMINs效能的关键问题的深入探讨，分析MMINs再生过程机制，可为MMINs在垃圾渗滤液深度处理方面提供科学理论依据和应用基础，具有重要的理论意义和实际应用前景。

项目通过合成制备对目标环境激素具有高效选择性的分子印迹复合材料，达到安全、高效地富集分离目标环境激素的目的，具有重要的研究价值。项目围绕磁性氧化石墨烯/分子印迹复合材料、β-环糊精修饰的磁性壳聚糖分子印迹复合材料、表面分子印迹型TiO2/GR复合材料、巯基功能化的二氧化钛分子印迹复合材料进行了优化制备过程的研究及作用机理的探讨。研究结果表明以磁性氧化石墨烯为载体、双酚A为模板分子合成磁性氧化石墨烯/分子印迹复合材料双酚A的吸附效果可达到472.68 mg/g。以双酚A为模板分子，β-环糊精修饰的磁性壳聚糖为印迹载体制得分子印迹复合材料对双酚A具有良好的识别和选择性，当初始pH为6.0，离子强度为20 mg/g时，MMIP的吸附容量能达到105.5 mg/g。同时材料的磁性达到5.938 emu g-1，良好的磁性使其在混合液中能够实现快速的固液分离。以二氧化钛/石墨烯复合材料为载体，双酚A为模板分子，邻苯二胺为功能单体，紫外光进行引发合成二氧化钛/石墨烯分子印迹复合材料对双酚A具有良好的催化降解性能和选择性，对降解机理进行研究结果发现：电子空穴对是催化反应产生的根本原因，羟基自由基是主要活性物质。以活化的二氧化钛-硫醇为印迹载体，2, 4-二硝基苯酚为模板分子，邻苯二胺为功能单体和交联单体，在过硫酸铵引发下于水相中进行聚合形成的分子印迹聚合物，相比于4-硝基苯酚为非目标污染物，对2, 4-二硝基苯酚有更高的催化选择性。本项目为优化调控分子印迹复合材料处理废水中的环境激素提供了科学理论依据。