Combining the targeted and untargeted screening of environmental contaminants reveals associations between PFAS exposure and vitamin D metabolism in human plasma
Published: 2023-05-24
Formatted citation
Carlsson H, Sreenivasan AP, Erngren I, Larsson A, Kultima K..
Combining the targeted and untargeted screening of environmental contaminants reveals associations between PFAS exposure and vitamin D metabolism in human plasma.
Environ Sci Process Impacts.
(2023).
DOI: 10.1039/d3em00060e
Abstract
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.