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Combining the targeted and untargeted screening of environmental contaminants reveals associations between PFAS exposure and vitamin D metabolism in human plasma
Environmental Science: Processes & Impacts ( IF 4.3 ) Pub Date : 2023-05-11 , DOI: 10.1039/d3em00060e
Henrik Carlsson 1 , Akshai Parakkal Sreenivasan 1 , Ida Erngren 1 , Anders Larsson 1 , Kim Kultima 1
Affiliation  

We have developed, validated, and applied a method for the targeted and untargeted screening of environmental contaminants in human plasma using liquid chromatography high-resolution mass spectrometry (LC-HRMS). The method was optimized for several classes of environmental contaminants, including PFASs, OH-PCBs, HBCDs, and bisphenols. One-hundred plasma samples from blood donors (19–75 years, men n = 50, women n = 50, from Uppsala, Sweden) were analyzed. Nineteen targeted compounds were detected across the samples, with 18 being PFASs and the 19th being OH-PCB (4-OH-PCB-187). Ten compounds were positively associated with age (in order of increasing p-values: PFNA, PFOS, PFDA, 4-OH-PCB-187, FOSA, PFUdA, L-PFHpS, PFTrDA, PFDoA, and PFHpA; p-values ranging from 2.5 × 10−5 to 4.67 × 10−2). Three compounds were associated with sex (in order of increasing p-values: L-PFHpS, PFOS, and PFNA; p-values ranging from 1.71 × 10−2 to 3.88 × 10−2), all with higher concentrations in male subjects compared with female subjects. Strong correlations (0.56–0.93) were observed between long-chain PFAS compounds (PFNA, PFOS, PFDA, PFUdA, PFDoA, and PFTrDA). In the non-targeted data analysis, fourteen unknown features correlating with known PFASs were found (correlation coefficients 0.48–0.99). Five endogenous compounds were identified from these features, all correlating strongly with PFHxS (correlation coefficients 0.59–0.71). Three of the identified compounds were vitamin D3 metabolites, and two were diglyceride lipids (DG 24:6;O). The results demonstrate the potential of combining targeted and untargeted approaches to increase the coverage of compounds detected with a single method. This methodology is well suited for exposomics to detect previously unknown associations between environmental contaminants and endogenous compounds that may be important for human health.

中文翻译:

结合环境污染物的定向和非定向筛查揭示了 PFAS 暴露与人血浆中维生素 D 代谢之间的关联

我们开发、验证并应用了一种使用液相色谱高分辨率质谱 (LC-HRMS) 对人血浆中的环境污染物进行靶向和非靶向筛查的方法。该方法针对几类环境污染物进行了优化,包括 PFAS、OH-PCB、HBCD 和双酚。对来自献血者(19-75 岁,男性n = 50,女性n = 50,来自瑞典乌普萨拉)的 100 份血浆样本进行了分析。在样品中检测到 19 种目标化合物,其中 18 种是 PFAS,第 19 种是 OH-PCB (4-OH-PCB-187)。十种化合物与年龄呈正相关(按照p值递增的顺序:PFNA、PFOS、PFDA、4-OH-PCB-187、FOSA、PFUdA、L-PFHpS、PFTrDA、PFDoA 和 PFHpA;p-值范围为 2.5 × 10 -5至 4.67 × 10 -2)。三种化合物与性别相关(按照p值递增的顺序:L-PFHpS、PFOS 和 PFNA;p值范围从 1.71 × 10 -2到 3.88 × 10 -2),与女性受试者相比,男性受试者的浓度更高。长链 PFAS 化合物(PFNA、PFOS、PFDA、PFUdA、PFDoA 和 PFTrDA)之间观察到强相关性 (0.56–0.93)。在非针对性数据分析中,发现了 14 个与已知 PFAS 相关的未知特征(相关系数 0.48-0.99)。从这些特征中鉴定出五种内源性化合物,它们均与 PFHxS 密切相关(相关系数 0.59-0.71)。三种已鉴定的化合物是维生素 D 3代谢物,其中两种是甘油二酯脂质 (DG 24:6;O)。结果表明,结合靶向和非靶向方法可以提高单一方法检测到的化合物的覆盖范围。这种方法非常适合暴露组学,以检测环境污染物和内源性化合物之间以前未知的关联,这些关联可能对人类健康很重要。
更新日期:2023-05-11
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