基于磁性有序微孔材料的全氟化合物选择性分析研究

Perfluorinated compounds (PFCs) are a new class of organic pollutants that attract worldwide concerns. The efficient detection and monitoring of PFCs in natural settings is a major challenge facing the environment scientists. Pretreatment is the key step in the analysis of environmental samples, which determines the analytical accuracy, speed, and sensitive. However, current pretreatment methods for PFCs have major disadvantages such as long extraction time, low sensitivity, and low selectivity. In this proposal, we plan to apply ordered microporous magnetic materials in the magnetic solid phase extraction (MSPE) of PFCs. With the assistant of micropores and active functional groups, the resulting materials could adsorb PFCs selectively over the macromolecular impurities in environmental samples. Additionally, the materials can be quickly separated from the sample matrix simply by a magnet field, which would effectively shorten the extraction time. The structure of ordered microporous magnetic materials will be manipulated by direct synthesis or post-modification. The extraction performance of PFCs of the materials will be studied by batch extraction experiments and spectroscopic techniques. The mechanisms for the selective extraction as well as the correlations between material structures and extraction performance will be illustrated. A rapid, sensitive and selective detection method for PFCs will be developed based on ordered microporous magnetic materials coupled with HPLC/MS/MS. Our research aims to provide reliable detection methods for PFCs in the environmental samples, supporting the research regarding the environmental behavior and risk of PFCs.

全氟化合物（PFCs）是一类新型的全球性有机污染物，对环境介质中PFCs的分析和监控已成为环境领域的重要课题。环境样品的前处理是PFCs分析的关键环节。然而，目前常用的PFCs分析前处理方法操作较繁琐、分析灵敏度有限，且易受可溶性有机质等基质干扰。本项目拟将有序微孔材料引入磁性固相萃取技术（MSPE），利用孔道的分子筛效应和表面活性基团的特殊作用高效识别PFCs，同时借助材料的磁响应性实现固液相快速分离，建立复杂环境介质中痕量PFCs的准确、快捷、选择性分析新方法。通过直接合成或后修饰手段，调控磁性有序微孔材料的结构性质；采用宏观萃取实验和微观观测技术相结合的方法，研究材料对PFCs的萃取特性，探明其选择性萃取机理，剖析材料结构性质对萃取特性的影响机制；结合HPLC/MS/MS技术，建立PFCs的MSPE-HPLC/MS/MS检测方法，为PFCs的环境监测、环境行为和效应研究提供技术支持。

本项目围绕全氟化合物（PFCs）的准确、快捷、选择性分析新方法开展研究，设计、制备了包括三嗪基有机骨架材料（CTF）、改性生物炭、金属有机骨架（MOFs）衍生磁性微孔碳在内的多种微孔材料；研究了这些材料对六种典型PFCs的吸附和萃取行为，考察了材料孔道结构和表面官能团性质，以及溶液pH值和共存可溶性有机质等环境因子对材料吸附PFCs的影响，剖析了材料对PFCs的吸附机制；以项目所构建的材料为基础，结合液质联用技术，建立了模型PFCs的选择性检测方法。主要结论如下：（1）材料表面疏水性和含氮官能团性质是决定其PFCs吸附性能的关键结构因素；（2）材料吸附PFCs的主要机制包括疏水作用、静电作用以及“脱溶剂损耗”效应；（3）基于CTF的模型PFCs固相萃取-液质联用分析方法具有线性范围宽、检出限低、精密度好等优点，且分析效果几乎不受共存可溶性有机质干扰，在PFCs的检测分析中具有一定的应用前景。

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