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Phospholipid removal for enhanced chemical exposomics in human plasma
Department of Environmental Science, Science for Life Laboratory, Stockholm University, Stockholm, Sweden.
Department of Environmental Science, Science for Life Laboratory, Stockholm University, Stockholm, Sweden.
Department of Environmental Science, Science for Life Laboratory, Stockholm University, Stockholm, Sweden; National Facility for Exposomics, Science for Life Laboratory, Stockholm University, Solna, Sweden.
Department of Environmental Science, Science for Life Laboratory, Stockholm University, Stockholm, Sweden; National Facility for Exposomics, Science for Life Laboratory, Stockholm University, Solna, Sweden.
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2023 (Engelska)Ingår i: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 57, nr 28, s. 10173-10184Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

The challenge of chemical exposomics in human plasma is the 1000-fold concentration gap between endogenous substances and environmental pollutants. Phospholipids are the major endogenous small molecules in plasma, thus we validated a chemical exposomics protocol with an optimized phospholipid-removal step prior to targeted and non-targeted liquid chromatography high-resolution mass spectrometry. Increased injection volume with negligible matrix effect permitted sensitive multiclass targeted analysis of 77 priority analytes; median MLOQ = 0.05 ng/mL for 200 μL plasma. In non-targeted acquisition, mean total signal intensities of non-phospholipids were enhanced 6-fold in positive (max 28-fold) and 4-fold in negative mode (max 58-fold) compared to a control method without phospholipid removal. Moreover, 109 and 28% more non-phospholipid molecular features were detected by exposomics in positive and negative mode, respectively, allowing new substances to be annotated that were non-detectable without phospholipid removal. In individual adult plasma (100 μL, n = 34), 28 analytes were detected and quantified among 10 chemical classes, and quantitation of per- and polyfluoroalkyl substances (PFAS) was externally validated by independent targeted analysis. Retrospective discovery and semi-quantification of PFAS-precursors was demonstrated, and widespread fenuron exposure is reported in plasma for the first time. The new exposomics method is complementary to metabolomics protocols, relies on open science resources, and can be scaled to support large studies of the exposome.

Ort, förlag, år, upplaga, sidor
American Chemical Society (ACS), 2023. Vol. 57, nr 28, s. 10173-10184
Nyckelord [en]
chemical exposome, high-resolution mass spectrometry, liquid chromatography, multiclass targeted, non-targeted, phospholipid, plasma
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URN: urn:nbn:se:umu:diva-212322DOI: 10.1021/acs.est.3c00663ISI: 001021461300001PubMedID: 37394749Scopus ID: 2-s2.0-85164670955OAI: oai:DiVA.org:umu-212322DiVA, id: diva2:1783871
Forskningsfinansiär
Vetenskapsrådet, 2018-03409Vetenskapsrådet, 2017-00650Tillgänglig från: 2023-07-25 Skapad: 2023-07-25 Senast uppdaterad: 2023-07-25Bibliografiskt granskad

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