Nontarget Screening Reveals Time Trends of Polar Micropollutants in a Riverbank Filtration System
Nontarget Screening Reveals Time Trends of Polar Micropollutants in a Riverbank Filtration System
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DOI：
10.1021/acs.est.9b01750
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发表时间：
2019-07-02
影响因子：
11.4
通讯作者：
de Voogt, Pim
中科院分区：
文献类型：
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作者：
Albergamo, Vittorio;Schollee, Jennifer E.;de Voogt, Pim
采用高分辨率质谱和开放式化学信息学工具，通过非靶标筛选，研究了天然饮用水源中极性微污染物的历史排放量。研究区包括一个河岸过滤样带喂养的Lek河，下莱茵河的分支，并表现出长达60年的旅行时间。检测到18，000多个配置文件。层次聚类显示，43%的15个人口最多的集群的特点是强度趋势与最大值在20世纪90年代，反映了人类活动的加剧，污水处理厂升级和监管在莱茵河沿岸国家。使用自动计算机片段化进行初步结构注释。基于计算机模拟片段与实验串联质谱的拟合度、与可公开访问的准确质谱的相似性、相关元数据以及可疑列表中的存在，对从ChemSpider检索到的候选结构进行评分。初步鉴定了67种独特的结构（两种电离模式下有72种），其中25种已得到确认，包括迄今为止在银行滤液或天然沃茨中未知的污染物，如四甲基磺酰胺。这项研究表明，许多类别的亲水性有机物进入河岸过滤系统，坚持和迁移几十年，如果生态地球化学条件是稳定的。
The historic emissions of polar micropollutants in a natural drinking water source were investigated by nontarget screening with high-resolution mass spectrometry and open cheminformatics tools. The study area consisted of a riverbank filtration transect fed by the river Lek, a branch of the lower Rhine, and exhibiting up to 60-year travel time. More than 18,000 profiles were detected. Hierarchical clustering revealed that 43% of the 15 most populated clusters were characterized by intensity trends with maxima in the 1990s, reflecting intensified human activities, wastewater treatment plant upgrades and regulation in the Rhine riparian countries. Tentative structure annotation was performed using automated in silico fragmentation. Candidate structures retrieved from ChemSpider were scored based on the fit of the in silico fragments to the experimental tandem mass spectra, similarity to openly accessible accurate mass spectra, associated metadata, and presence in a suspect list. Sixty-seven unique structures (72 over both ionization modes) were tentatively identified, 25 of which were confirmed and included contaminants so far unknown to occur in bank filtrate or in natural waters at all, such as tetramethylsulfamide. This study demonstrates that many classes of hydrophilic organics enter riverbank filtration systems, persisting and migrating for decades if biogeochemical conditions are stable.