饮用水中新型极性碘代消毒副产物的检测鉴定和生成机理研究

As emerging pollutants in drinking water, iodinated disinfection byproducts (I-DBPs) have been drawing a lot of concerns in recent years as a result of their high carcinogenicity and mutagenicity. However, limited by current analytical techniques, almost all previously studies have focused on commonly known I-DBPs, with little study on new I-DBPs. This project was designed to study the detection, identification, and formation of new polar I-DBPs in drinking water. With the aid of ultra performance liquid chromatography/electrospray ionization-triple quadrupole mass spectrometry and liquid chromatography-ion trap-time of flight mass spectrometry, structure/formula identification methods will be developed for new polar I-DBPs based on precursor ion scan, multiple reaction monitoring, selected ion recording, product ion scan, and synthesis of standard compounds. Formation of new polar I-DBPs under various conditions will be investigated to elucidate precursors and formation mechanisms of new polar I-DBPs. Moreover, with the development of pretreatment method for real drinking water samples, concentration profiles of new polar I-DBPs in drinking water samples from five major cities of Yangtze River delta region will be revealed. This project will provide new methods and basis for analysis and control of new polar I-DBPs in drinking water.

碘代消毒副产物作为饮用水中的新兴污染物，因其极强的致癌和致突变特性而备受关注。由于受现有检测技术的局限，国内外相关研究尚集中在常见碘代消毒副产物上，缺乏对新型碘代消毒副产物的研究。本项目拟重点研究饮用水中新型极性碘代消毒副产物的检测鉴定和生成机理。结合极性碘代消毒副产物的特性，采用超效液相色谱/电喷雾三重四极杆质谱技术和液相色谱-离子阱-飞行时间质谱技术，建立基于前体离子扫描、多反应监测、选择性离子扫描、子离子扫描和标准品合成的新型极性碘代消毒副产物结构式/分子式鉴定方法；进而研究新型极性碘代消毒副产物的生成条件、辨识前驱物、探讨生成机理；并以长江三角洲地区五个主要城市的饮用水为研究对象，构建实际饮用水样的预处理方法，研究新型极性碘代消毒副产物的浓度分布情况。本项目的工作将为饮用水中新型极性碘代消毒副产物的研究提供新的科学方法和技术，并为控制饮用水中新型极性碘代消毒副产物的污染提供依据。

本研究围绕饮用水中的新型极性卤代消毒副产物（尤其是碘代和苯酚类消毒副产物）展开了检测鉴定方法开发、生成机理探索以及浓度分布调研等一系列工作。基于超效液相色谱/电喷雾电离三重四极杆质谱和高分辨质谱平台,建立了饮用水中痕量新型极性卤代消毒副产物的高效选择性检测鉴定方法；采用该方法，在饮用水中首次鉴定出11种新型极性碘代消毒副产物、25种新型极性苯酚类消毒副产物以及4种三卤代-羟基环戊烯二酮类消毒副产物。优化了超效液相色谱/电喷雾电离三重四极杆质谱对于新型消毒副产物定量方法，大幅降低了这些新型消毒副产物的定量限。研究发现这些新型消毒副产物的生成量受到水源水水质、饮用水处理工艺和消毒方式的共同影响，其前驱物为多羟基取代苯环类物质（如没食子酸），分析了这些新型极性卤代消毒副产物在不同消毒方式下的生成降解路径。通过浓度分布调研，证明这些新型消毒副产物在长三角地区主要城市的自来水中普遍存在。本研究建立的检测鉴定方法具有重要的理论和实际意义，为探索饮用水中其他新型极性卤代消毒副产物提供了新思路。