血清中53种全氟和多氟烷基化合物的高通量液质联用检测方法的建立OA北大核心CSTPCD

[Background]Per-and polyfluoroalkyl substances(PFAS)are a class of persistent organic pollu-tants that possess potential toxicity to the human body.The production and utilization of diverse emerging PFAS have resulted in widespread human exposure.Therefore,it is imperative to es-tablish a quantitative methodology encompassing a wide range of PFAS for a comprehensive as-sessment of human exposure to these compounds. [Objective]To establish a high-throughput quantitative method for the simultaneous determina-tion of 53 PFAS in human serum based on ultra-high-performance liquid chromatography-Q Ex-active high resolution mass spectrometry(UPLC-Q Exactive HRMS). [Methods]The extraction recoveries of hydrophilic-lipophilic balance(HLB)column,weak anion exchange(WAX)column,and 96-well WAX μElution plate were compared to select the SPE column with the highest recovery.The retention time and peak shape of the target compounds were compared between ACQUITY UPLC BEH C18 column and Accucore aQ column,and the more cost-effective column was chosen.The effects of adding different levels of ammonium formate(0,2,5 and 10 mmol·L-1)in mobile phase on peak shape and target response were compared to determine the optimal buffer salt concentration.The optimal spray voltage was obtained by comparing-2 kV and-4 kV.The proposed method was validated from the aspects of selectivity,standard curve,limits of detection,precision,accuracy,and matrix effect.The method was applied to 142 umbilical serum samples. [Results]The best recovery rate(64%-118%)was achieved by using 96-well WAX μElution plate.The optimal separation and peak shape were obtained by utilizing Accucore aQ column with H2O-methanol(containing 5 mmol·L-1 ammonium formate)as the mobile phase.Less in-source collision and better target response were observed when the spray voltage was set to-2 kV.All target analytes had a good linearity,with R2>0.99.The limits of detection ranged from 0.01 to 0.50 μg·L-1,and the recovery ranged from 69%to 127%with the precision less than 26%.A total of 31 PFAS were detected in the 142 actual samples,among which 14 PFAS had a detection frequency over 50%.Perfluorooctanoic acid showed the highest median concentration of 4.16 μg·L-1,followed by 6:2 chlorinated polyfluorinated ether sulfonate and perfluorooctane sulfonates(3.50 μg·L-1 and 1.59 μg·L-1,respectively). [Conclusion]In this study,we establish a UPLC-Q Excative HRMS method for simutanious determination of 53 PFAS concentrations in serum.This method has the advantages of wide coverage of PFAS,good selectivity,and easy operation,and is suitable for biological de-tection with a large sample size.