Suspect screening is a valuable tool for characterizing per- and polyfluoroalkyl substances (PFASs) in environmental media. Although a variety of data mining tools have been developed and applied for suspect screening of PFAS, few suspect screening workflows have undergone a comprehensive performance evaluation or optimization. The goals of this research were to: (1) evaluate and optimize three independent suspect screening workflows for the detection of PFASs in water samples; and (2) apply the optimized suspect screening workflows to an environmental sample to determine the extent to which suspect screening results converge. We evaluated and optimized suspect screening workflows using Compound Discoverer v3.2, enviMass v4.2, and FluoroMatch v2.4 using test samples containing 33 target PFASs. The average sensitivity (Sen) and selectivity (Sel) for each workflow across the test samples was: Compound Discoverer Sen = 71%, Sel = 85%; enviMass Sen = 89%, Sel = 80%; FluoroMatch Sen = 51%, Sel = 82%. We then applied the optimized workflows to a contaminated groundwater sample containing an unknown number of PFASs. Each workflow managed to annotate unique PFASs that were not annotated by the other workflows including 2 by Compound Discoverer and 19 each by enviMass and FluoroMatch. Thirty-two enviMass hits and 28 of the Compound Discoverer and FluoroMatch hits were annotated by at least one of the other workflows. Sixteen PFASs were annotated by all three of the optimized workflows. This work provides a basis for conducting suspect screening for PFASs that will lead to more consistent reporting of suspect screening data.

中文翻译：

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用于表征水中全氟和多氟烷基物质的三个独立的可疑筛查工作流程的评估、优化和应用

可疑筛查是表征环境介质中全氟和多氟烷基物质 (PFAS) 的宝贵工具。尽管已经开发并应用了多种数据挖掘工具来对 PFAS 进行可疑筛选，但很少有可疑筛选工作流程经过全面的性能评估或优化。本研究的目标是：(1) 评估和优化用于检测水样中 PFAS 的三个独立的可疑筛查工作流程；(2) 将优化的可疑筛选工作流程应用于环境样本，以确定可疑筛选结果的收敛程度。我们使用Compound Discoverer v3.2、enviMass v4.2和FluoroMatch v2.4评估和优化了可疑筛选工作流程使用包含 33 种目标 PFAS 的测试样本。测试样品中每个工作流程的平均灵敏度 (Sen) 和选择性 (Sel) 为：Compound Discoverer Sen = 71%，Sel = 85%；环境质量森 = 89%，塞尔 = 80%；FluoroMatch Sen = 51%，Sel = 82%。然后，我们将优化的工作流程应用于含有未知数量 PFAS 的受污染地下水样本。每个工作流程都设法注释了其他工作流程未注释的独特 PFAS，其中包括Compound Discoverer 的2 个和enviMass和FluoroMatch各 19 个。Compound Discoverer和FluoroMatch 中的32 个enviMass命中和 28 个至少有一个其他工作流程对命中进行了注释。所有三个优化的工作流程都对 16 个 PFAS 进行了注释。这项工作为对 PFAS 进行可疑筛查提供了基础，这将导致对可疑筛查数据的报告更加一致。