Per- and polyfluoroalkyl substances (PFAS) are a group of anthropogenic pollutants that are found ubiquitously in surface and drinking water supplies. Due to their persistent nature, bioaccumulative potential, and significant adverse health effects associated with low concentrations, they pose a concern for human and environmental exposure. With the advances in high-resolution mass spectrometry (HRMS) methods, there has been an increasing number of non-targeted analysis (NTA) approaches that allow for a more comprehensive characterization of total PFAS present in environmental samples. In this study, we have developed and compared NTA workflows based on an online solid phase extraction- liquid chromatography high resolution mass spectrometry (online SPE-LC-HRMS) method followed by data processing using Compound Discoverer and FluoroMatch for the screening of PFAS in drinking waters from populated counties in South Florida, as well as in surface waters from Biscayne Bay, Key west, and Everglades canals. Tap water showed the highest number of PFAS features, indicating a poor removal of these chemicals by water treatment or perhaps the breakdown of PFAS precursors. The high number of PFAS features identified only by CD and FluoroMatch emphasizes the complementary aspects of these data processing methods. A Semi-quantitation method for NTA (qNTA) was proposed using a global calibration curve based on existing native standards and internal standards, in which concentration estimates were determined by a regression-based model and internal standard (IS) response factors. NTA play a crucial role in the identification and prioritization of non-traditionally monitored PFAS, needed for the understanding of the toxicological and environmental impact, which are largely underestimated due to the lack of such information for many PFAS.

全氟和多氟烷基物质 (PFAS) 是一组人为污染物，普遍存在于地表水和饮用水供应中。由于它们的持久性、生物蓄积潜力和与低浓度相关的显着不良健康影响，它们引起了人类和环境暴露的担忧。随着高分辨率质谱 (HRMS) 方法的进步，越来越多的非靶向分析 (NTA) 方法可以对环境样品中存在的总 PFAS 进行更全面的表征。在这项研究中，我们开发并比较了基于在线固相萃取-液相色谱高分辨率质谱（在线 SPE-LC-HRMS）方法的 NTA 工作流程，然后使用 Compound Discoverer 和 FluoroMatch 进行数据处理以筛查人口稠密县饮用水中的 PFAS在南佛罗里达州，以及比斯坎湾、基韦斯特和大沼泽地运河的地表水中。自来水显示出最多的 PFAS 特征，表明通过水处理或 PFAS 前体的分解可能无法去除这些化学物质。仅由 CD 和 FluoroMatch 识别的大量 PFAS 特征强调了这些数据处理方法的互补性。使用基于现有本地标准和内部标准的全局校准曲线提出了 NTA (qNTA) 的半定量方法，其中浓度估计由基于回归的模型和内部标准 (IS) 响应因子确定。NTA 在非传统监测的 PFAS 的识别和优先排序方面发挥着至关重要的作用，这是了解毒理学和环境影响所必需的，由于许多 PFAS 缺乏此类信息，这些影响在很大程度上被低估了。