Novel perfluoroalkyl substances (PFAS) discovered in whole blood using automated non-targeted analysis of dried blood spots.
Novel perfluoroalkyl substances (PFAS) discovered in whole blood using automated non-targeted analysis of dried blood spots.
复制标题
通过对干血斑进行自动非靶向分析，在全血中发现了新型全氟烷基物质 (PFAS)。
DOI：
10.1016/j.scitotenv.2023.163579
复制
发表时间：
2023
期刊：
影响因子：
--
通讯作者：
GodriPollitt,KrystalJ
中科院分区：
文献类型：
--
作者：
Koelmel,JeremyP;Lin,ElizabethZ;Parry,Emily;Stelben,Paul;Rennie,EmmaE;GodriPollitt,KrystalJ
在人类血液中常规筛查一小部分全氟烷基和多氟烷基物质（PFAS）。这些化合物通常占人体血液中总PFAS的<50%。随着替代PFAS和更复杂的PFAS化学品被引入市场，人体血液中已知PFAS的百分比一直在下降。这些新的PFAS中的大多数以前没有被发现。需要非靶向方法来表征这种“暗物质”PFAS。我们的目标是将非靶向PFAS分析应用于人体血液，以了解这些化合物的来源，浓度和毒性。高分辨率串联质谱（HRMS）和软件工作流程的PFAS特性在干血斑的报告。与静脉抽血相比，干血点是一种侵入性较小的采集技术，可以从弱势人群中采集。国际上可从新生儿获得存档干血斑的生物储存库，并提供研究产前PFAS暴露的机会。在本研究中，使用液相色谱HRMS的迭代MS/MS分析干燥血斑卡。使用FluoroMatch Suite进行数据处理，该套件包括一个可视化工具，可显示同源系列、保留时间vsm/zplots、MS/MS光谱、特征表、注释和片段，用于片段筛选。进行数据处理和注释的研究人员对标准品加标这一事实不知情，并且能够注释95%的干血斑样本上加标的标准品，这表明使用FluoroMatch Suite的假阴性率较低。在Schymanski 2级置信度下，在5个同源系列中共检测到28种PFAS（20种标准品和4种外源性化合物）。在这4种物质中，3种是全氟烷基醚羧酸（PFECA），这是PFAS的一种化学类别，在环境和生物基质中越来越多地被检测到，但目前在大多数目标分析中尚未筛选。使用片段筛选检测到另外86个潜在的PFAS。PFAS是非常持久和广泛的，但仍然在很大程度上不受管制。我们的研究结果将有助于提高对暴露的理解。这些方法在环境流行病学研究中的应用有可能为PFAS监测，监管和个人层面的缓解策略提供信息。
A small subset ofper- and polyfluoroalkyl substances (PFAS) are routinely screened in human blood. These compounds generally explain <50 % of the total PFAS in human blood. The percentage of known PFAS in human blood has been decreasing as replacement PFAS and more complex PFAS chemistries are introduced to the market. Most of these novel PFAS have not been previously identified. Non-targeted methods are required to characterize this “dark matter” PFAS. Our objective was to apply non-targeted PFAS analysis to human blood to gain an understanding about the sources, concentrations, and toxicity of these compounds. A high-resolution tandem mass spectrometry (HRMS) and software workflow for PFAS characterization in dried blood spots is reported. Dried blood spots are a less invasive collection technique compared to venous blood draws, allowing collection from vulnerable populations. Biorepositories of archived dried blood spots are available internationally from newborns and present opportunities to study prenatal exposure to PFAS. In this study, dried blood spot cards were analyzed using iterative MS/MS by liquid chromatography HRMS. Data processing was conducted using FluoroMatch Suite including a visualizer tool that presents homologous series, retention time vsm/zplots, MS/MS spectra, feature tables, annotations, and fragments for fragment screening. The researcher performing data-processing and annotation was blinded to the fact that standards were spiked in, and was able to annotate 95 % of standards spiked on dried blood spot samples, signifying a low false negative rate using FluoroMatch Suite. A total of 28 PFAS (20 standards and 4 exogenous compounds) were detected across five homologous series with Schymanski Level 2 confidence. Of these 4, 3 were perfluoroalkyl ether carboxylic acids (PFECA), a chemical class of PFAS which is increasingly being detected in environmental and biological matrices but is not currently screened in most targeted analysese. A further 86 potential PFAS were detected using fragment screening. PFAS are extremely persistent and widespread yet remain largely unregulated. Our findings will contribute to an improved an understanding of exposures. Application of these methods in environmental epidemiology studies have the potential to inform policy with regards to PFAS monitoring, regulation, and individual-level mitigation strategies.