共价有机骨架材料分离富集新型污染物及其作用机理研究

Environmental pollution has become one of the most important problems that affect the survival and health of human being. One of the most effective ways to eliminate environmental pollution is the use of adsorbents with high adsorption performance. Covalent organic frameworks (COFs) are novel porous adsorbents with the largest specific surface area, which not only have high specific surface area and porosity, but also have high thermal stability and chemical stability. New COFs, such as covalent triazine based frameworks, have hydrophobic and aromatic rigid skeleton and long chain polymer containing polar functional groups. Hydrophobic, π-π or hydrogen bonding interaction occurs between COFs and emerging contaminants..In order to overcome the disadvantages of traditional adsorbents (such as thermal instability and low extraction efficiency towards polar pollutants), based on the structural characteristics of emerging contaminants (polybrominated diphenyl ethers, perfluorinated compounds and alkyl phenols), this project is to prepare, find and use COFs with high adsorption performance as adsorbents for the separation, preconcentration and determination of emerging contaminants. In addition, the mechanism of using COFs as adsorbents for separation and preconcentration of emerging contaminants will be further clarified through investigating their structure characteristics and adsorption performance in detail. This project is not only searching novel functions of COFs, but also seeking new adsorbent materials with high adsorption performance, which is important for removal, rapid sample pretreatment and determination of emerging contaminants.

环境污染问题已成为影响人类生存与健康的重大问题之一，而消除环境污染最有效的方法之一是使用高效吸附剂。共价有机骨架材料(COFs)是迄今为止比表面积最大的新颖多孔吸附剂之一，这种材料不但具有较高的比表面积和多孔性，而且还具有较高的热稳定性和化学稳定性。以三嗪基COFs材料等为代表的新型COFs材料具有疏水和芳香的刚性骨架且聚合物长链中含极性官能团，可以与新型污染物发生疏水、π-π 或氢键作用等。本项目拟根据典型新型污染物的结构特征，制备并筛选出具有高效吸附性能的COFs材料作为吸附剂用于新型污染物的分离富集和分析，以克服传统吸附剂不耐高温和对极性污染物萃取效率低的缺点；还将详细研究COFs材料的结构特征和吸附性能，阐明COFs材料对典型新型污染物的作用机理。本项目是对COFs材料新功能的一次重要探索，也是寻找新型高效吸附剂的一条新途径，这对新型污染物的控制、快速前处理和分析有十分重要的意义。

项目制备并筛选出了一系列吸附性能强稳定性高的共价有机骨架材料（COFs）作为固相微萃取或固相萃取吸附剂，建立了全氟烷基酸类污染物、多溴联苯醚、酚类污染物、农药、抗生素和消毒副产物等新型污染物的快速样品前处理和分析的新方法，并成功应用于实际环境样品的分析；阐明了COFs对这些新型污染物的吸附作用机理主要是疏水作用、多孔结构，卤键作用、氢键作用、静电作用或π-π共轭作用等等。项目的完成对于新型污染物的分析和控制具有十分重要的意义。项目在Top期刊上共发表论文25篇，其中3篇入选ESI高被引论文，获山东省科技进步一等奖和中国分析测试协会科学技术一等奖各1项。在项目执行期间，项目负责人先后获批国际先进材料学会会士、国务院政府特殊津贴、国家百千万人才工程、国家有突出贡献中青年专家、环境领域全球2%顶尖科学家和泰山学者特聘专家等荣誉和奖励。