Assessing the performance of a targeted absolute quantification isotope dilution liquid chromatograhy tandem mass spectrometry assay versus a commercial nontargeted relative quantification assay for detection of three major perfluoroalkyls in human blood

IF 1.9 3区 化学 Q3 BIOCHEMICAL RESEARCH METHODS
Samira Salihovic, Linda Dunder, Monica Lind, Lars Lind
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引用次数: 0

Abstract

Isotope dilution ultrahigh-performance liquid chromatography coupled to tandem mass spectrometry (UHPLC–MS/MS) is commonly used for trace analysis of polyfluoroalkyl and perfluoroalkyl substances (PFAS) in difficult matrices. Commercial nontargeted analysis of major PFAS where relative concentrations are obtained cost effectively is rapidly emerging and is claimed to provide comparable results to that of absolute quantification using matrix matched calibration and isotope dilution UHPLC–MS/MS. However, this remains to be demonstrated on a large scale. We aimed to assess the performance of a targeted absolute quantification isotope dilution LC–MS/MS assay versus a commercial nontargeted relative quantification assay for detection of three major PFAS in human blood. We evaluated a population-based cohort of 503 individuals. Correlations were assessed using Spearman's rank correlation coefficients (rho). Precision and bias were assessed using Bland–Altman plots. For perfluorooctane sulfonic acid, the median concentrations were 5.10 ng/mL (interquartile range [IQR] 3.50–7.24 ng/mL), the two assays correlated with rho 0.83. For perfluorooctanoic acid, the median concentrations were 2.14 ng/mL (IQR 1.60–3.0 ng/mL), the two assays correlated with rho 0.92. For perfluorohexanesulfonate, the median concentrations were 5.5 ng/mL (IQR 2.50–11.61 ng/mL), the two assays correlated with rho 0.96. The Bland–Altman statistical test showed agreement of the mean difference for the majority of samples (97–98%) between the two assays. Absolute plasma concentrations of PFAS obtained using matrix matched calibration and isotope dilution UHPLC–MS/MS show agreement with relative plasma concentrations from a nontargeted commercial platform by Metabolon. We observed striking consistency between the two assays when examining the associations of the three PFAS with cholesterol, offering additional confidence in the validity of utilizing the nontargeted approach for correlations with various health phenotypes.

Abstract Image

评估定向绝对定量同位素稀释液相色谱串联质谱测定法与商用非定向相对定量测定法在检测人体血液中三种主要全氟烷基化合物方面的性能。
同位素稀释超高效液相色谱-串联质谱法(UHPLC-MS/MS)通常用于痕量分析困难基质中的多氟烷基和全氟烷基物质(PFAS)。对主要 PFAS 进行商业性非目标分析可获得具有成本效益的相对浓度,这种分析方法正在迅速兴起,据称其结果可与使用基质匹配校准和同位素稀释超高效液相色谱-质谱法进行绝对定量分析的结果相媲美。然而,这仍有待大规模验证。在检测人体血液中的三种主要全氟辛烷磺酸时,我们的目标是评估定向绝对定量同位素稀释 LC-MS/MS 检测法与商用非定向相对定量检测法的性能。我们对 503 人的人群进行了评估。相关性采用斯皮尔曼等级相关系数 (rho) 进行评估。精确度和偏差采用 Bland-Altman 图进行评估。全氟辛烷磺酸的中位浓度为 5.10 纳克/毫升(四分位数间距 [IQR] 3.50-7.24 纳克/毫升),两种检测方法的相关系数为 rho 0.83。全氟辛酸的中位浓度为 2.14 纳克/毫升(IQR 1.60-3.0 纳克/毫升),两种检测方法的相关性为 rho 0.92。全氟己烷磺酸的中位浓度为 5.5 纳克/毫升(IQR 2.50-11.61 纳克/毫升),两种检测方法的相关性为 rho 0.96。Bland-Altman 统计检验显示,两种检测方法在大多数样本(97%-98%)中的平均值差异一致。使用基质匹配校准和同位素稀释超高效液相色谱-质谱/多质谱获得的 PFAS 绝对血浆浓度与 Metabolon 公司非靶向商业平台获得的相对血浆浓度一致。在检测三种全氟辛烷磺酸与胆固醇的关系时,我们发现这两种检测方法具有惊人的一致性,这为利用非靶向方法检测各种健康表型的相关性提供了更多信心。
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来源期刊
Journal of Mass Spectrometry
Journal of Mass Spectrometry 化学-光谱学
CiteScore
5.10
自引率
0.00%
发文量
84
审稿时长
1.5 months
期刊介绍: The Journal of Mass Spectrometry publishes papers on a broad range of topics of interest to scientists working in both fundamental and applied areas involving the study of gaseous ions. The aim of JMS is to serve the scientific community with information provided and arranged to help senior investigators to better stay abreast of new discoveries and studies in their own field, to make them aware of events and developments in associated fields, and to provide students and newcomers the basic tools with which to learn fundamental and applied aspects of mass spectrometry.
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