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    超高效液相色谱-串联质谱法测定人体血清中49种全氟及多氟物质的含量

    Determination of 49 Perfluorinated and Polyfluorinated Substances in Human Serum by Ultra-High Performance Liquid Chromatography-Tandem Mass Spectrometry

    • 摘要: 提出了超高效液相色谱-串联质谱法(UHPLC-MS/MS)同时测定人体血清中49种全氟及多氟物质(PFASs)含量的方法。取50 μL健康人血清样品置于1.5 mL离心管中,加入3.125 μg·L−1混合内标使用液200 μL,涡旋60 s,于4 ℃超声10 min,于−20 ℃冷冻保存1 h,于4 ℃以转速12 000 r·min−1离心15 min,取100 μL上清液置于含150 μL水的1.5 mL离心管中,涡旋60 s,于4 ℃超声5 min,于4 ℃以转速12 000 r·min−1离心10 min,上清液上机测定。以Poroshell 120 EC-C18色谱柱为固定相,以不同体积比的4 mmol·L−1甲酸铵溶液-乙腈混合液为流动相进行梯度洗脱,质谱分析采用电喷雾离子(ESI)源,在负离子(ESI)扫描模式下采用多反应监测(MRM)模式检测。结果表明,49种PFASs质量浓度和内标的质量浓度比值与其峰面积比值均在一定范围内呈线性关系,检出限(3S/N)为0.000 2~0.166 7 μg·L−1;按照标准加入法进行回收试验,回收率为80.5%~118%,测定值的相对标准偏差(n=6)为0.80%~12%;方法用于200份健康人血清样品的分析,49种PFASs均有检出,其中检出量中位数排在前五的PFASs依次为全氟辛烷磺酸,9-氯全氟三氧代壬烷磺酸,全氟己烷磺酸,全氟辛酸,全氟癸酸,检出量中位数分别为107.188,68.838,51.810,44.381,12.507 μg·L−1

       

      Abstract: A method for determination of 49 perfluorinated and polyfluorinated substances (PFASs) in human serum by ultra-high performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS) was proposed. 50 μL of healthy human serum sample was taken and placed in a 1.5 mL-centrifuge tube. 200 μL of 3.125 μg·L−1 mixed internal standard solution was added, the solution was vortexed for 60 s and sonicated at 4 ℃ for 10 min. The mixture was frozen at −20 ℃ for 1 h and centrifuged at a rotational speed of 12 000 r·min−1 for 15 min at 4 ℃. 100 μL of supernatant was taken and placed in a 1.5 mL-centrifuge tube which containing 150 μL of water, the solution was vortexed for 60 s, and sonicated at 4 ℃ for 5 min. The mixture was centrifuged at a rotational speed of 12 000 r·min−1 for 10 min at 4 ℃, and the supernatant was determined by the instrument. Poroshell 120 EC-C18 column was used as the stationary phase and the mixed solution composed of 4 mmol·L−1 ammonium formate solution and acetonitrile at different volume ratios was used as the mobile phase for gradient elution. Electrospray ion (ESI) source was used for mass spectrometry. The targets were analyzed by multiple reaction monitoring (MRM) mode in negative ion (ESI) scanning mode. As shown by the results, linear relationships between values of the mass concentration ratio and the peak area ratio of the target to internal standard were kept in definite ranges, with detection limits (3S/N) in the range of 0.000 2‒0.166 7 μg·L−1. Test for recovery was made by the standard addition method, giving results in the range of 80.5%‒118%, with RSDs (n=6) of the determined values in the range of 0.80%‒12%. This method was used for the analysis of 200 healthy human serum samples, and 49 PFASs were detected. Among them, the top five PFASs with median detection amounts were perfluorooctane sulfonic acid, 9-chloroperfluorotrioxynonanesulfonic acid, perfluorohexane sulfonic acid, perfluorooctanoic acid, and perfluorodecanoic acid, with median detection amounts of 107.188, 68.838, 51.810, 44.381, and 12.507 μg·L−1, respectively.

       

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