Comprehensive Emerging Chemical Discovery: Novel Polyfluorinated Compounds in Lake Michigan Trout
Comprehensive Emerging Chemical Discovery: Novel Polyfluorinated Compounds in Lake Michigan Trout
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DOI：
10.1021/acs.est.6b01349
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发表时间：
2016-09-06
影响因子：
11.4
通讯作者：
Holsen, Thomas M.
中科院分区：
文献类型：
--
作者：
Baygi, Sadjad Fakouri;Crimmins, Bernard S.;Holsen, Thomas M.
一个通用的筛选算法，能够有效地搜索未知化合物的液相色谱/质谱数据已经开发出使用开源和通用计算软件包的组合。该脚本被用来搜索选择新的多氟污染物在五大湖鱼。然而，每当收集全扫描、高分辨率质谱和色谱数据时，该框架都适用。确定目标化合物类别，并生成候选物矩阵，其中包括质谱图和可能的裂解途径。使用已知的直链全氟烷基酸的标准溶液进行初始校准。一旦验证，密歇根湖鳟鱼的数据文件进行了分析，多氟烷基酸使用的算法参考3570可能的化合物，包括C-4-C-10全氟和多氟烷基，多氟氯烷基酸和磺酸盐，和潜在的醚形式。结果表明，存在30多氟化的化学式，以前没有在文献中报道。所确定的候选物包括单-至六氟烷基羧酸、单-和三氟烷基羧酸醚以及新型多氟烷基磺酸盐。湖鳟中确定的候选物种进行了资格使用理论同位素配置文件匹配，已知的线性全氟烷基酸（PFAA）的碎片的基础上的特征碎片模式，并在重复提取和注射之间的保留时间再现性。此外，根据理论辛醇/水分配系数比较了化合物类别内多个物质的相对保留时间。
A versatile screening algorithm capable of efficiently searching liquid chromatographic/mass spectrometric data for unknown compounds has been developed using a combination of open source and generic computing software packages. The script was used to search for select novel polyfluorinated contaminants in Great Lakes fish. However, the framework is applicable whenever full-scan, high-resolution mass spectral and chromatographic data are collected. Target compound classes are defined and a matrix of candidates is generated that includes mass spectral profiles and likely fragmentation pathways. The initial calibration was performed using a standard solution of known linear perfluoroalkyl acids. Once validated, Lake Michigan trout data files were analyzed for polyfluoroalkyl acids using the algorithm referencing 3570 possible compounds including C-4-C-10 perfluoro- and polyfluoroalkyl, polyfluorochloroalkyl acids and sulfonates, and potential ether forms. The results suggest the presence of 30 polyfluorinated chemical formulas which have not been previously reported in the literature. The identified candidates included mono- to hexafluoroalkyl carboxylic acids, mono- and trifluoroalkyl carboxylic acid ethers, and novel polyfluoroalkyl sulfonates. Candidate species identified in lake trout were qualified using theoretical isotopic profile matching, characteristic fragmentation patterns based on known linear perfluoroalkyl acid (PFAA) fragmentation, and retention time reproducibility among replicate extractions and injections. In addition, the relative retention times of multiple species within a compound class were compared based on theoretical octanol water partition coefficients.