What is in the fish? Collaborative trial in suspect and non-target screening of organic micropollutants using LC- and GC-HRMS

Wiebke Dürig; Sofia Lindblad; Oksana Golovko; Georgios Gkotsis; Reza Aalizadeh; Maria-Christina Nika; Nikolaos Thomaidis; Nikiforos A Alygizakis; Merle Plassmann; Peter Haglund; Qiuguo Fu; Juliane Hollender; Jade Chaker; Arthur David; Uwe Kunkel; André Macherius; Lidia Belova; Giulia Poma; Hugues Preud'Homme; Catherine Munschy; Yann Aminot; Carsten Jaeger; Jan Lisec; Martin Hansen; Katrin Vorkamp; Linyan Zhu; Francesca Cappelli; Claudio Roscioli; Sara Valsecchi; Renzo Bagnati; Belén González; Ailette Prieto; Olatz Zuloaga; Ruben Gil-Solsona; Pablo Gago-Ferrero; Sara Rodriguez-Mozaz; Hélène Budzinski; Marie-Helene Devier; Georg Dierkes; Lise Boulard; Griet Jacobs; Stefan Voorspoels; Heinz Rüdel; Lutz Ahrens

doi:10.1016/j.envint.2023.108288

What is in the fish? Collaborative trial in suspect and non-target screening of organic micropollutants using LC- and GC-HRMS

Environ Int. 2023 Nov:181:108288. doi: 10.1016/j.envint.2023.108288. Epub 2023 Oct 25.

Authors

Wiebke Dürig¹, Sofia Lindblad², Oksana Golovko³, Georgios Gkotsis⁴, Reza Aalizadeh⁵, Maria-Christina Nika⁶, Nikolaos Thomaidis⁷, Nikiforos A Alygizakis⁸, Merle Plassmann⁹, Peter Haglund¹⁰, Qiuguo Fu¹¹, Juliane Hollender¹², Jade Chaker¹³, Arthur David¹⁴, Uwe Kunkel¹⁵, André Macherius¹⁶, Lidia Belova¹⁷, Giulia Poma¹⁸, Hugues Preud'Homme¹⁹, Catherine Munschy²⁰, Yann Aminot²¹, Carsten Jaeger²², Jan Lisec²³, Martin Hansen²⁴, Katrin Vorkamp²⁵, Linyan Zhu²⁶, Francesca Cappelli²⁷, Claudio Roscioli²⁸, Sara Valsecchi²⁹, Renzo Bagnati³⁰, Belén González³¹, Ailette Prieto³², Olatz Zuloaga³³, Ruben Gil-Solsona³⁴, Pablo Gago-Ferrero³⁵, Sara Rodriguez-Mozaz³⁶, Hélène Budzinski³⁷, Marie-Helene Devier³⁸, Georg Dierkes³⁹, Lise Boulard⁴⁰, Griet Jacobs⁴¹, Stefan Voorspoels⁴², Heinz Rüdel⁴³, Lutz Ahrens⁴⁴

Affiliations

¹ Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), Box 7050, 75007 Uppsala, Sweden. Electronic address: wiebke.durig@slu.se.
² Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), Box 7050, 75007 Uppsala, Sweden. Electronic address: sofia.lindblad@slu.se.
³ Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), Box 7050, 75007 Uppsala, Sweden. Electronic address: Oksana.Golovko@slu.se.
⁴ Department of Chemistry, National and Kapodistrian University of Athens, 15771 Athens, Greece. Electronic address: geogkotsis@chem.uoa.gr.
⁵ Department of Chemistry, National and Kapodistrian University of Athens, 15771 Athens, Greece. Electronic address: raalizadeh@chem.uoa.gr.
⁶ Department of Chemistry, National and Kapodistrian University of Athens, 15771 Athens, Greece. Electronic address: nikamar@chem.uoa.gr.
⁷ Department of Chemistry, National and Kapodistrian University of Athens, 15771 Athens, Greece. Electronic address: ntho@chem.uoa.gr.
⁸ Department of Chemistry, National and Kapodistrian University of Athens, 15771 Athens, Greece; Environmental Institute, Okružná 784/42, 97241 Koš, Slovakia. Electronic address: alygizakis@ei.sk.
⁹ Department of Environmental Science, Stockholm University, 10691 Stockholm, Sweden. Electronic address: merle.plassmann@aces.su.se.
¹⁰ Department of Chemistry, Chemical Biological Centre (KBC), Umeå University, Linnaeus väg 6, 90187 Umeå, Sweden. Electronic address: peter.haglund@umu.se.
¹¹ Eawag: Swiss Federal Institute of Aquatic Science and Technology, Überlandstrasse 133, 8600 Dübendorf, Switzerland; Helmholtz Centre for Environmental Research - UFZ, Permoserstraße 15, 04318 Leipzig, Germany. Electronic address: qiuguo.fu@ufz.de.
¹² Eawag: Swiss Federal Institute of Aquatic Science and Technology, Überlandstrasse 133, 8600 Dübendorf, Switzerland; Institute of Biogeochemistry and Pollutant Dynamics, ETH Zürich, Universitätstrasse 16, 8092 Zürich, Switzerland. Electronic address: juliane.hollender@eawag.ch.
¹³ Université de Rennes, Inserm, EHESP, Irset - UMR_S, 1085 Rennes, France. Electronic address: jade.chaker@ehesp.fr.
¹⁴ Université de Rennes, Inserm, EHESP, Irset - UMR_S, 1085 Rennes, France. Electronic address: arthur.david@ehesp.fr.
¹⁵ Bavarian Environment Agency, Bürgermeister-Ulrich-Straße 160, 86179 Augsburg, Germany. Electronic address: uwe.kunkel@lfu.bayern.de.
¹⁶ Bavarian Environment Agency, Bürgermeister-Ulrich-Straße 160, 86179 Augsburg, Germany. Electronic address: andre.macherius@lfu.bayern.de.
¹⁷ Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610 Wilrijk, Belgium. Electronic address: lidia.belova@uantwerpen.be.
¹⁸ Toxicological Centre, University of Antwerp, Universiteitsplein 1, 2610 Wilrijk, Belgium. Electronic address: giulia.poma@uantwerpen.be.
¹⁹ IPREM-UMR5254, E2S UPPA, CNRS, 2 avenue Angot, 64053 Pau cedex, France. Electronic address: hugues.preudhomme@univ-pau.fr.
²⁰ Ifremer, CCEM Contamination Chimique des Écosystèmes Marins, 44000 Nantes, France. Electronic address: catherine.munschy@ifremer.fr.
²¹ Ifremer, CCEM Contamination Chimique des Écosystèmes Marins, 44000 Nantes, France. Electronic address: yann.aminot@ifremer.fr.
²² Bundesanstalt für Materialforschung und -prüfung (BAM), Analytical Chemistry, Richard-Willstätter-Straße 11, 12489 Berlin, Germany. Electronic address: carsten.jaeger@bam.de.
²³ Bundesanstalt für Materialforschung und -prüfung (BAM), Analytical Chemistry, Richard-Willstätter-Straße 11, 12489 Berlin, Germany. Electronic address: jan.lisec@bam.de.
²⁴ Department of Environmental Science, Aarhus University, Frederiksborgvej 399, 4000 Roskilde, Denmark. Electronic address: martin.hansen@envs.au.dk.
²⁵ Department of Environmental Science, Aarhus University, Frederiksborgvej 399, 4000 Roskilde, Denmark. Electronic address: kvo@envs.au.dk.
²⁶ Department of Environmental Science, Aarhus University, Frederiksborgvej 399, 4000 Roskilde, Denmark. Electronic address: lzhu@envs.au.dk.
²⁷ Water Research Institute, National Research Council of Italy, Via del Mulino 19, 20861 Brugherio MB, Italy. Electronic address: cappelli@irsa.cnr.it.
²⁸ Water Research Institute, National Research Council of Italy, Via del Mulino 19, 20861 Brugherio MB, Italy. Electronic address: roscioli@irsa.cnr.it.
²⁹ Water Research Institute, National Research Council of Italy, Via del Mulino 19, 20861 Brugherio MB, Italy. Electronic address: valsecchi@irsa.cnr.it.
³⁰ Department of Environmental Health Sciences, Istituto di Ricerche Farmacologiche Mario Negri IRCCS, Via Mario Negri 2, 20156 Milan, Italy. Electronic address: renzo.bagnati@marionegri.it.
³¹ Department of Analytical Chemistry, Faculty of Science and Technology, University of the Basque Country (UPV/EHU), Barrio Sarriena s/n, 48940 Leioa, Spain; Research Centre for Experimental Marine Biology and Biotechnology (PIE), University of the Basque Country (UPV/EHU), Areatza Pasealekua 47, 48620 Plentzia, Spain. Electronic address: belen.gonzalez@ehu.eus.
³² Department of Analytical Chemistry, Faculty of Science and Technology, University of the Basque Country (UPV/EHU), Barrio Sarriena s/n, 48940 Leioa, Spain; Research Centre for Experimental Marine Biology and Biotechnology (PIE), University of the Basque Country (UPV/EHU), Areatza Pasealekua 47, 48620 Plentzia, Spain. Electronic address: ailette.prieto@ehu.eus.
³³ Department of Analytical Chemistry, Faculty of Science and Technology, University of the Basque Country (UPV/EHU), Barrio Sarriena s/n, 48940 Leioa, Spain; Research Centre for Experimental Marine Biology and Biotechnology (PIE), University of the Basque Country (UPV/EHU), Areatza Pasealekua 47, 48620 Plentzia, Spain. Electronic address: olatz.zuloaga@ehu.eus.
³⁴ Catalan Institute for Water Research (ICRA), Carrer Emili Grahit 101, 17003 Girona, Spain; Universitat de Girona, Girona, Spain; Institute of Environmental Assessment and Water Research - Severo Ochoa Excellence Center (IDAEA), Spanish Council of Scientific Research (CSIC), Barcelona 08034, Spain. Electronic address: ruben.gil.solsona@csic.es.
³⁵ Catalan Institute for Water Research (ICRA), Carrer Emili Grahit 101, 17003 Girona, Spain; Institute of Environmental Assessment and Water Research - Severo Ochoa Excellence Center (IDAEA), Spanish Council of Scientific Research (CSIC), Barcelona 08034, Spain. Electronic address: pablo.gago@idaea.csic.es.
³⁶ Catalan Institute for Water Research (ICRA), Carrer Emili Grahit 101, 17003 Girona, Spain; Universitat de Girona, Girona, Spain. Electronic address: srodriguez@icra.cat.
³⁷ University Bordeaux, CNRS, Bordeaux INP, EPOC, UMR 5805, 33600 Pessac, France. Electronic address: helene.budzinski@u-bordeaux.fr.
³⁸ University Bordeaux, CNRS, Bordeaux INP, EPOC, UMR 5805, 33600 Pessac, France. Electronic address: marie-helene.devier@u-bordeaux.fr.
³⁹ Federal Institute of Hydrology, Am Mainzer Tor 1, 56068 Koblenz, Germany. Electronic address: Dierkes@bafg.de.
⁴⁰ Federal Institute of Hydrology, Am Mainzer Tor 1, 56068 Koblenz, Germany; Metabolomics Core Facility, Centre de Ressources et Recherches Technologiques (C2RT), Institut Pasteur, 25-28 Rue du Dr Roux, 75015 Paris, France. Electronic address: lise.boulard@pasteur.fr.
⁴¹ Flemish Institute for Technological Research (VITO), Unit Separation and Conversion Technology, Boeretang 200, 2400 Mol, Belgium. Electronic address: griet.jacobs@vito.be.
⁴² Flemish Institute for Technological Research (VITO), Unit Separation and Conversion Technology, Boeretang 200, 2400 Mol, Belgium. Electronic address: stefan.voorspoels@vito.be.
⁴³ Fraunhofer Institute for Molecular Biology and Applied Ecology (Fraunhofer IME), Auf dem Aberg 1, 57392 Schmallenberg, Germany. Electronic address: heinz.ruedel@ime.fraunhofer.de.
⁴⁴ Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), Box 7050, 75007 Uppsala, Sweden. Electronic address: lutz.ahrens@slu.se.

PMID: 37918065
DOI: 10.1016/j.envint.2023.108288

Abstract

A collaborative trial involving 16 participants from nine European countries was conducted within the NORMAN network in efforts to harmonise suspect and non-target screening of environmental contaminants in whole fish samples of bream (Abramis brama). Participants were provided with freeze-dried, homogenised fish samples from a contaminated and a reference site, extracts (spiked and non-spiked) and reference sample preparation protocols for liquid chromatography (LC) and gas chromatography (GC) coupled to high resolution mass spectrometry (HRMS). Participants extracted fish samples using their in-house sample preparation method and/or the protocol provided. Participants correctly identified 9-69 % of spiked compounds using LC-HRMS and 20-60 % of spiked compounds using GC-HRMS. From the contaminated site, suspect screening with participants' own suspect lists led to putative identification of on average ∼145 and ∼20 unique features per participant using LC-HRMS and GC-HRMS, respectively, while non-target screening identified on average ∼42 and ∼56 unique features per participant using LC-HRMS and GC-HRMS, respectively. Within the same sub-group of sample preparation method, only a few features were identified by at least two participants in suspect screening (16 features using LC-HRMS, 0 features using GC-HRMS) and non-target screening (0 features using LC-HRMS, 2 features using GC-HRMS). The compounds identified had log octanol/water partition coefficient (K_OW) values from -9.9 to 16 and mass-to-charge ratios (m/z) of 68 to 761 (LC-HRMS and GC-HRMS). A significant linear trend was found between log K_OW and m/z for the GC-HRMS data. Overall, these findings indicate that differences in screening results are mainly due to the data analysis workflows used by different participants. Further work is needed to harmonise the results obtained when applying suspect and non-target screening approaches to environmental biota samples.

Keywords: Biota; Collaborative trial; Exposome; GC-HRMS; LC-HRMS; Suspect and non-target analysis.

MeSH terms

Animals
Chromatography, Liquid / methods
Environmental Monitoring* / methods
Fishes*
Gas Chromatography-Mass Spectrometry
Humans
Mass Spectrometry / methods