High-Throughput UHPLC-MS/MS Measurement of Per- and Poly-Fluorinated Alkyl Substances in Human Serum
High-Throughput UHPLC-MS/MS Measurement of Per- and Poly-Fluorinated Alkyl Substances in Human Serum
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DOI：
10.1093/jat/bkz097
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发表时间：
2020-05-01
影响因子：
2.5
通讯作者：
Morris, Andrew J.
中科院分区：
文献类型：
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作者：
Mottaleb, M. Abdul;Petriello, Michael C.;Morris, Andrew J.
全氟烷基和多氟烷基物质（PFAS）是一大类合成表面活性剂化学品，广泛用于食品包装和纺织品制造，并作为水性成膜消防泡沫的主要成分。PFASs在环境中具有高度持久性，人类接触广泛，几乎所有成年美国人的血液中都可检测到这些化学物质。PFAS在临床前模型中表现出一系列毒性作用。在人类中，PFAS暴露与出生体重降低、免疫反应降低、癌症和生育能力受损以及循环胆固醇水平升高有关。我们已经开发了一种灵敏的高通量方法，用于定量人体血清和血浆中的代表性PFAS，用于PFAS暴露对人体健康影响的生物监测和流行病学研究。该方法结合了稳健和可重现的96孔板格式样品制备与超高效液相色谱-串联质谱。该方法的开发，验证和用于有针对性的测量8个短链/长链PFAS分析物在人血清中。使用质量标记的内标物在50微升样品中测量目标分析物。三级质量控制（QC-低、QC-中、QC-高）样品中目标分析物的平均加标回收率（n = 10）范围为70 - 127%，相对标准偏差（RSD）为2-14%。替代物的平均加标回收率（n = 10）为79-115%（QC-低），RSD为8-12%（QC-中），90-123%（RSD为7-12%），82-114%（QC-高），RSD为9-15%。目标化合物的检测限为0.05-0.04 ng/mL。该方法用于揭示在肯塔基州大学医院接受治疗的肯塔基州居民PFAS暴露的区域差异。
Per- and poly-fluorinated alkyl substances (PFASs) are a large group of synthetic surfactant chemicals with widespread uses in food packaging and textile manufacturing and as the main constituent of aqueous film-forming firefighting foams. PFASs are highly persistent in the environment, and human exposures are extensive with these chemicals detectable in the blood of almost all adult Americans. PFASs exhibit a range of toxic effects in preclinical models. In humans, PFAS exposure has been associated with lower birth weights, decreased immune responses, cancer and impaired fertility and elevated circulating cholesterol levels. We have developed a sensitive high-throughput method for quantification of representative PFAS in human serum and plasma for biomonitoring and epidemiological studies of human health effects of PFAS exposure. The method combines robust and reproducible 96-well plate format sample preparation with ultra-performance liquid chromatography-tandem mass spectrometry. The method was developed, validated and used for targeted measurements of eight short-/long-chain PFAS analytes in human serum. Targeted analytes were measured in 50 microliters of sample using mass-labeled internal standards. Mean spiked recoveries (n = 10) of target analytes for three tiers quality control (QC-low, QC-medium, QC-high) samples ranged from 70 to 127% with 2-14% relative standard deviation (RSD). The average spiked recoveries (n = 10) of surrogates were 79-115% with 8-12% RSD for QC-low, 90-123% with 7-12% RSD for QC-medium and 82-114% with 9-15% RSD for QC-high. The limit of detection for the target compounds was 0.05-0.04 ng/mL. The method was used to reveal regional differences in PFAS exposures in Kentucky residents receiving care at the University of Kentucky Hospitals.