Sport fish fillets and human sera (fish consumers) were collected in the Lake Superior and Lake Michigan basin and screened for novel contaminants using the isotopic profile deconvoluted chromatogram (IPDC) algorithm. The IPDC algorithm was extended beyond traditional Cl/Br filters to detect additional potential bioaccumulative and toxic (PBT) such as perfluoroalkyl substances (PFAS). The IPDC algorithm screened for approximately 13.5 million theoretical molecular formulas. Additional algorithm modules were developed to detect data independent MS/MS fragmentation products and a retention time index calculator using a series of ¹³C-labeled perfluoroalkyl carboxylic acids (¹³C-PFCAs). Ten potential compound classes were isolated including six untargeted PFAS, six homologue groups of polyfluorinated carboxylic acids, polyfluorinated telomer alcohols (PoFTOHs), two hydroxylated polychlorobiphenyls, pesticides, herbicides, antifungals, pharmaceuticals, artificial sweeteners, and personal care products with minimal postprocessing efforts. The algorithm isolated 48 ubiquitous PoFTOHs in both fish fillet and serum of fish consumers suggesting a region wide distribution of this class of compounds. The 3, 4, and 7 fluorine substituted PoFTOH were the most abundant congeners in both biological matrices.

中文翻译：

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大湖地区新型污染物的非针对性发现：鱼片和鱼类消费者的比较

在苏必利尔湖和密歇根湖流域收集了运动鱼片和人类血清（鱼类食用者），并使用同位素轮廓反褶积色谱法（IPDC）筛选了新型污染物。IPDC算法已扩展到传统的Cl / Br过滤器之外，以检测其他潜在的生物累积性和有毒性（PBT），例如全氟烷基物质（PFAS）。IPDC算法筛选出约1350万个理论分子式。开发了其他算法模块以检测数据独立的MS / MS碎片产物和使用一系列¹³ C标记的全氟烷基羧酸的保留时间指数计算器（¹³C-PFCA）。分离出十种潜在的化合物类别，包括六种未靶向的PFAS，六种同族的多氟羧酸，多氟端粒醇（PoFTOH），两种羟基化的多氯联苯，农药，除草剂，抗真菌剂，药品，人工甜味剂和个人护理产品，而这些方法所需的后处理工作量很小。该算法在鱼片和鱼消费者的血清中分离出48个普遍存在的PoFTOH，这表明这类化合物在整个地区范围内分布。3、4和7个氟取代的PoFTOH是两种生物基质中最丰富的同类物。