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A large scale multi-laboratory suspect screening of pesticide metabolites in human biomonitoring: From tentative annotations to verified occurrences

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HUBER Carolin NIJSSEN Rosalie MOL Hans ANTIGNAC Jean Philippe KRAUSS Martin BRACK Werner WAGNER Kevin DEBRAUWER Laurent VITALE Chiara Maria PRICE Elliott James KLÁNOVÁ Jana MOLINA Borja Garlito LEON Nuria PARDO Olga FERNANDEZ Sandra F. SZIGETI Tamas KOZEPESY Szilvia ŠULC Libor ČUPR Pavel MARTINSONE Inese AKULOVA Lasma OTTENBROS Ilse VERMEULEN Roel VLAANDEREN Jelle LUIJTEN Mirjam LOMMEN Arjen

Rok publikování 2022
Druh Článek v odborném periodiku
Časopis / Zdroj Environment International
Fakulta / Pracoviště MU

Přírodovědecká fakulta

Citace
www https://www.sciencedirect.com/science/article/pii/S0160412022003798?via%3Dihub
Doi http://dx.doi.org/10.1016/j.envint.2022.107452
Klíčová slova Human biomonitoring; Exposomics; Pesticides; Suspect screening; Pesticide metabolites; LC-HAMS; HBM4EU
Přiložené soubory
Popis Within the Human Biomonitoring for Europe initiative (HBM4EU), a study to determine new biomarkers of exposure to pesticides and to assess exposure patterns was conducted. Human urine samples (N = 2,088) were collected from five European regions in two different seasons. The objective of the study was to identify pesticides and their metabolites in collected urine samples with a harmonized suspect screening approach based on liquid chromatography coupled to high resolution mass spectrometry (LC-HRMS) applied in five laboratories. A combined data processing workflow included comprehensive data reduction, correction of mass error and retention time (RT) drifts, isotopic pattern analysis, adduct and elemental composition annotation, finalized by a mining of the elemental compositions for possible annotations of pesticide metabolites. The obtained tentative annotations (n = 498) were used for acquiring representative data-dependent tandem mass spectra (MS2) and verified by spectral comparison to reference spectra generated from commercially available reference standards or produced through human liver S9 in vitro incubation experiments. 14 parent pesticides and 71 metabolites (including 16 glucumnide and 11 sulfate conjugates) were detected. Collectively these related to 46 unique pesticides. For the remaining tentative annotations either (i) no data-dependent MS2 spectra could be acquired, (ii) the spectral purity was too low for sufficient matching, or (iii) RTs indicated a wrong annotation, leaving potential for more pesticides and/or their metabolites being confirmed in further studies. Thus, the reported results are reflecting only a part of the possible pesticide exposure.
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