水体中痕量有机污染物系统分析方法学研究

In last few years, there is increasing concern over the presence of emerging contaminants in global aquatic ecosystems, since the number of potentially hazardous chemicals that can reach the environment is continuously increasing and new chemical substances are constantly being synthesized and released. Due to the potential adverse effect of human health or ecosystem safety, the comprehensive and objective study of organic pollutants in aquatic environment becomes a major concern..In this study, a systematic study strategy on the multiclass analysis of trace organic pollutants will be established to obtain a realistic and more complete overview of the organic pollution present in water. Because of the complexity of the aquatic system, the large variety of organic contaminants, the low analyte levels, with quite different physicochemical characteristics, a series of pretreatment procedures using solid-phase extraction (SPE) will be investigated to concentrate the analytes prior to instrument analysis. To simultaneously realize target, post-target, and non-target organic contaminants screening, an complementary analytical strategy will be applied by combining two powerful techniques, gas chromatography(GC) and liquid chromatography(LC), both hyphenated with triple-quadrupole analyzers (MS-MS) and time-of-flight mass spectrometry (TOFMS), and gas chromatography or multidimensional gas chromatography coupled with mass spectrometry can also be used. At the same time, the powerful softwares such as AMDIS, Targetlynx and ChromaLynx Application Manager will be used to analyze the huge amount of information for reliable screening of organic compounds..The established systematic multi-residue analytical method will be applied to the drinking water of Liaoning province, Dahuofang reservoir and its three main joint rivers, and the screening, identification, and quantification of the target, post-target, and non-target organic contaminants will be accomplished. The performance and potential of this method will be confirmed by the comprehensive and objective organic pollution levels obtained. By this study, we can not only build a systematic multi-residue analytical method of trace organic contaminants, but also make a great improvement in the analysis technology for organic pollutants in water.

随着全球水资源状况迅速恶化，水污染问题成为人们关注的焦点。对水体中复合污染的深入了解有赖于分析检测技术的发展与进步。项目以建立水体中复杂有机污染物系统检测程序、非目标污染物筛查和半定量技术等系统分析方法为目标，旨在通过样品前处理方法研究、多种检测手段联合运用，以及海量数据分析处理等系列工作相结合，形成系统的痕量有机污染物分析方法，以实现准确可靠地对水体中种类繁多、结构与性质各异的有机污染物进行目标化合物定性确认和定量分析，以及后目标、非目标化合物筛查。该项研究不仅可以建立水体有机污染物的系统分析方法、为更全面地认识区域水体有机污染程度提供技术基础，还能够推动复杂有机污染物分析检测技术的深入发展。

本项目针对水体中痕量、多种类有机污染物展开系统分析方法学研究。首先，以饮用水中痕量挥发性有机污染物（VOCs）非目标筛查为目的，构建了一种新型的大体积水样高倍富集装置。并将该装置与吹扫捕集-气相色谱/质谱（P&T-GC/MS）联合使用，对大辽河流域的VOCs进行综合筛查。另外，针对饮用水中弱极性消毒副产物卤代乙腈（HANs），建立了一种盐辅助分散液－液微萃取（SADLLME）富集方法，应用该方法联合程序升温－气相色谱/质谱法（PTV-GC/MS），并将该方法应用于饮用水消毒副产物筛查。其次，为解决液相色谱/质谱法基质效应的问题，制备了具有高度类选择性的分子印迹聚合物材料。针对替代模板筛选盲目、费时的问题，提出并验证了一种基于非印迹色谱柱的聚合物组成和替代模板快速筛选方法，并将其应用于双酚类高效替代模板的筛选，筛选出了1,1,1-三（4-羟基苯基）乙烷（THPE）和酚酞（PP）两种不属于双酚类化合物的超高类选择性替代模板，克服了双酚S（BPS）替代模板的不足。制备了双酚A（BPA）印迹海绵状介孔硅（MISMS）及二苯甲酮类化合物的分子印迹材料，并将这些材料应用于痕量有机污染物的富集。. 联合使用固相萃取、超声波辅助提取、分散液液微萃取等前处理方法，以及气相色谱/质谱法、液相色谱/串联质谱法、高效液相色谱-高分辨飞行时间质谱法等，建立了水体和沉积物非极性、中极性、极性和挥发性有机污染物的分析方法。利用自动解卷积技术和标准谱库，实现样品中非极性和弱极性有机污染物的高通量靶标筛查和非靶标筛查，利用MassHunter数据解析软件和AIQS-DB及500种毒、药物两种标准谱库，建立了环境样品中中极性和极性污染物基于精确分子量的高通量非靶标筛查方法，并将所建立的分析方法应用于环境水体中痕量有机污染物的综合筛查。