An integrated method for simultaneously determining 10 classes of per- and polyfluoroalkyl substances in one drop of human serum

An integrated method for simultaneously determining 10 classes of per- and polyfluoroalkyl substances in one drop of human serum
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一滴人血清中同时测定10类全氟烷基和多氟烷基物质的综合方法

DOI:
10.1016/j.aca.2017.10.038
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发表时间:
2018-01-25
影响因子:
6.2
通讯作者:
Jiang, Guibin
Jiang, Guibin
中科院分区:
化学1区
文献类型:
--
作者:
Gao, Ke;Fu, Jianjie;Jiang, Guibin

文献摘要

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全氟烷基物质和多氟烷基物质(PFAS)是一组合成的化学物质,它们的物理化学性质有很大的不同,这导致了一次注射同时测定它们的困难。建立了一种灵敏、可靠、全自动化的在线Turboflow固相萃取-超高效液相色谱-MS/MS同时检测人血清中10类(共43种)PFASs的方法。该方法具有良好的线性关系(R&gT;0.99)和良好的方法检出限(0.013-0.089 ng mL(-1))。满意的基质加标回收率(84.3-109%)和相对标准偏差(日内RSD:1.3-12.6%,日间RSD:1.7-13.8%,周间RSD:1.8-13.5%,月间RSD:3.1-12.4%),分析时间短(19min/样),样本量少(L 25亩),适合大规模流行病学研究。此外,该方法为实时监测PFASs前体在体内和体外的降解动力学提供了可行性。通过对标准参考物质(SRM 1957)的重复分析,进一步验证了本方法的质量,目标PFAS浓度的检测值和参考值之间的偏差在1.9%~14.2%(n=5)之间。本研究还首次确定了除证书上的那些外,SRM 1957中的几种全氟辛烷磺酸的值,如N-乙酸甲酯、6:2氯-全氟辛烷磺酸和全氟辛烷磺酸。最后,应用所建立的方法对15名普通人群和15名职业工人血清中的PFASs进行了检测,发现6:2 FTSA是主要的前体物。(C)2017爱思唯尔B.V.保留所有权利。
Per- and polyfluoroalkyl substances (PFASs) represent a group of synthetic chemicals, and they have quite different physicochemical properties, which result in difficulties of their simultaneous determination in a single injection. A sensitive, reliable, and fully automated method was developed for simultaneously detecting 10 classes of PFASs (total of 43) in human serum using online Turboflow SPE-UHPLC-MS/MS. This method provided high linearity of matrix-matched calibration standards (R > 0.99), excellent method limits of detection (MLODs) (0.013-0.089 ng mL(-1)). satisfactory matrix spiked recoveries (84.3-109%) and relative standard deviations (RSDs) (intra-day RSDs: 1.3-12.6%, inter-day RSDs: 1.7-13.8%, inter-week RSDs: 1.8-13.5%, inter-month RSDs: 3.1-12.4%), short analysis time (19 min per sample) and small sample amount requirement (25 mu L), which were suitable for large-scale epidemiologic studies. Moreover, the method provided the feasibility of real-time monitoring for the degradation kinetics of PFASs precursors both in vitro and in vivo. The quality of the present method was further verified by repetitive analysis of a standard reference material (SRM 1957), with the deviations of the targeted PFAS concentrations ranging from 1.9% to 14.2% (n = 5) between the detected and reference values. The present study also determined values for several PFASs in SRM 1957 other than those on the certificate, for the first time, such as N-EtFOSA, 6:2 Cl-PFESA, and PFBA. Finally, the established method was applied to detect PFASs in serum samples of 15 ordinary people and 15 occupational workers, and 6:2 FTSA was found as the dominant precursor. (C) 2017 Elsevier B.V. All rights reserved.