[en] Identification of bioaccumulating contaminants of emerging concern (CECs) via suspect and non-target screening remains a challenging task. In this study, ion mobility separation with high-resolution mass spectrometry (IM-HRMS) was used to investigate the effects of drift time (DT) alignment on spectrum quality and peak annotation for screening of CECs in complex sample matrices using data independent acquisition (DIA). Data treatment approaches (Binary Sample Comparison) and prioritisation strategies (Halogen Match, co-occurrence of features in biota and the water phase) were explored in a case study on zebra mussel (Dreissena polymorpha) in Lake Mälaren, Sweden’s largest drinking water reservoir. DT alignment evidently improved the fragment spectrum quality by increasing the similarity score to reference spectra from on average (±standard deviation) 0.33 ± 0.31 to 0.64 ± 0.30 points, thus positively influencing structure elucidation efforts. Thirty-two features were tentatively identified at confidence level 3 or higher using MetFrag coupled with the new PubChemLite database, which included predicted collision cross-section values from CCSbase. The implementation of predicted mobility data was found to support compound annotation. This study illustrates a quantitative assessment of the benefits of IM-HRMS on spectral quality, which will enhance the performance of future screening studies of CECs in complex environmental matrices.
Disciplines :
Sciences de l’environnement & écologie
Auteur, co-auteur :
Menger, Frank
Celma, Alberto
SCHYMANSKI, Emma ; University of Luxembourg > Luxembourg Centre for Systems Biomedicine (LCSB)
Lai, Foon Yin
Bijlsma, Lubertus
Wiberg, Karin
Hernández, Félix
Sancho, Juan V.
Ahrens, Lutz
Co-auteurs externes :
yes
Langue du document :
Anglais
Titre :
Enhancing spectral quality in complex environmental matrices: Supporting suspect and non-target screening in zebra mussels with ion mobility
Ahrens, L., Daneshvar, A., Lau, A.E., Kreuger, J., Characterization of five passive sampling devices for monitoring of pesticides in water. J. Chromatogr. A. 1405 (2015), 1–11, 10.1016/j.chroma.2015.05.044.
Badea, S.-L., Geana, E.-I., Niculescu, V.-C., Ionete, R.-E., Recent progresses in analytical GC and LC mass spectrometric based-methods for the detection of emerging chlorinated and brominated contaminants and their transformation products in aquatic environment. Sci. Total Environ., 722, 2020, 137914, 10.1016/j.scitotenv.2020.137914.
Baduel, C., Mueller, J.F., Tsai, H., Gomez Ramos, M.J., Development of sample extraction and clean-up strategies for target and non-target analysis of environmental contaminants in biological matrices. J. Chromatogr. A. 1426 (2015), 33–47, 10.1016/j.chroma.2015.11.040.
Barbosa, M.O., Moreira, N.F.F., Ribeiro, A.R., Pereira, M.F.R., Silva, A.M.T., Occurrence and removal of organic micropollutants: An overview of the watch list of EU Decision 2015/495. Water Res. 94 (2016), 257–279, 10.1016/j.watres.2016.02.047.
Barrett, H., Du, X., Houde, M., Lair, S., Verreault, J., Peng, H., Suspect and nontarget screening revealed class-specific temporal trends (2000–2017) of poly- and perfluoroalkyl substances in St. Lawrence Beluga Whales. Environ. Sci. Technol. 55 (2021), 1659–1671, 10.1021/acs.est.0c05957.
Baygi, S.F., Fernando, S., Hopke, P.K., Holsen, T.M., Crimmins, B.S., Nontargeted discovery of novel contaminants in the great lakes region: a comparison of fish fillets and fish consumers. Environ. Sci. Technol. 55 (2021), 3765–3774, 10.1021/acs.est.0c08507.
Belova, L., Caballero-Casero, N., van Nuijs, A.L.N., Covaci, A., Ion mobility-high-resolution mass spectrometry (IM-HRMS) for the analysis of contaminants of emerging concern (CECs): database compilation and application to urine samples. Anal. Chem. 93 (2021), 6428–6436, 10.1021/acs.analchem.1c00142.
Bervoets, L., Voets, J., Chu, S., Covaci, A., Schepens, P., Blust, R., Comparison of accumulation of micropollutants between indigenous and transplanted zebra mussels (dreissena polymorpha). Environ. Toxicol. Chem., 23, 2004, 1973, 10.1897/03-365.
Bervoets, L., Voets, J., Covaci, A., Chu, S., Qadah, D., Smolders, R., Schepens, P., Blust, R., Use of transplanted zebra mussels (Dreissena polymorpha) to assess the bioavailability of microcontaminants in flemish surface waters. Environ. Sci. Technol. 39 (2005), 1492–1505, 10.1021/es049048t.
Bijlsma, L., Bade, R., Celma, A., Mullin, L., Cleland, G., Stead, S., Hernandez, F., Sancho, J.V., Prediction of collision cross-section values for small molecules: application to pesticide residue analysis. Anal. Chem. 89 (2017), 6583–6589, 10.1021/acs.analchem.7b00741.
Bijlsma, L., Berntssen, M.H.G., Merel, S., A refined nontarget workflow for the investigation of metabolites through the prioritization by in silico prediction tools. Anal. Chem. 91 (2019), 6321–6328, 10.1021/acs.analchem.9b01218.
Binelli, A., Cogni, D., Parolini, M., Riva, C., Provini, A., In vivo experiments for the evaluation of genotoxic and cytotoxic effects of Triclosan in Zebra mussel hemocytes. Aquat. Toxicol. 91 (2009), 238–244, 10.1016/j.aquatox.2008.11.008.
Celma, A., Fabregat-Safont, D., Ibàñez, M., Bijlsma, L., Hernandez, F., Sancho, J.V., 2019. S61 | UJICCSLIB | Collision Cross Section (CCS) Library from UJI, http://doi.org/10.5281/zenodo.3966751.
Celma, A., Sancho, J.V., Schymanski, E.L., Fabregat-Safont, D., Ibáñez, M., Goshawk, J., Barknowitz, G., Hernández, F., Bijlsma, L., Improving target and suspect screening high-resolution mass spectrometry workflows in environmental analysis by ion mobility separation. Environ. Sci. Technol. 54 (2020), 15120–15131, 10.1021/acs.est.0c05713.
Celma, A., Ahrens, L., Gago-Ferrero, P., Hernández, F., López, F., Lundqvist, J., Pitarch, E., Sancho, J.V., Wiberg, K., Bijlsma, L., The relevant role of ion mobility separation in LC-HRMS based screening strategies for contaminants of emerging concern in the aquatic environment. Chemosphere, 280, 2021, 130799, 10.1016/j.chemosphere.2021.130799.
Chen, C., Wohlfarth, A., Xu, H., Su, D., Wang, X., Jiang, H., Feng, Y., Zhu, M., Untargeted screening of unknown xenobiotics and potential toxins in plasma of poisoned patients using high-resolution mass spectrometry: Generation of xenobiotic fingerprint using background subtraction. Anal. Chim. Acta. 944 (2016), 37–43, 10.1016/j.aca.2016.09.034.
D'Atri, V., Causon, T., Hernandez-Alba, O., Mutabazi, A., Veuthey, J.-L., Cianferani, S., Guillarme, D., Adding a new separation dimension to MS and LC–MS: What is the utility of ion mobility spectrometry?. J. Sep. Sci. 41 (2018), 20–67, 10.1002/jssc.201700919.
Dom, I., Biré, R., Hort, V., Lavison-Bompard, G., Nicolas, M., Guérin, T., Extended targeted and non-targeted strategies for the analysis of marine toxins in mussels and oysters by (LC-HRMS). Toxins., 10, 2018, 375, 10.3390/toxins10090375.
Du, B., Lofton, J.M., Peter, K.T., Gipe, A.D., James, C.A., McIntyre, J.K., Scholz, N.L., Baker, J.E., Kolodziej, E.P., Development of suspect and non-target screening methods for detection of organic contaminants in highway runoff and fish tissue with high-resolution time-of-flight mass spectrometry. Environ. Sci. Process. Impacts. 19 (2017), 1185–1196, 10.1039/c7em00243b.
Dürig, W., Kintzi, A., Golovko, O., Wiberg, K., Ahrens, L., New extraction method prior to screening of organic micropollutants in various biota matrices using liquid chromatography coupled to high-resolution time-of-flight mass spectrometry. Talanta, 219, 2020, 121294, 10.1016/j.talanta.2020.121294.
Dürig, W., Alygizakis, N.A., Menger, F., Golovko, O., Wiberg, K., Ahrens, L., Novel prioritisation strategies for evaluation of temporal trends in archived white-tailed sea eagle muscle tissue in non-target screening. J. Hazard. Mater., 424, 2022, 127331, 10.1016/j.jhazmat.2021.127331.
Fabregat-Safont, D., Ibáñez, M., Bijlsma, L., Hernández, F., Waichman, A.V., de Oliveira, R., Rico, A., Wide-scope screening of pharmaceuticals, illicit drugs and their metabolites in the Amazon River. Water Res., 200, 2021, 117251, 10.1016/j.watres.2021.117251.
Fernando, S., Renaguli, A., Milligan, M.S., Pagano, J.J., Hopke, P.K., Holsen, T.M., Crimmins, B.S., Comprehensive analysis of the great lakes top predator fish for novel halogenated organic contaminants by GC×GC-HR-ToF mass spectrometry. Environ. Sci. Technol. 52 (2018), 2909–2917, 10.1021/acs.est.7b05999.
Gago-Ferrero, P., Bletsou, A.A., Damalas, D.E., Aalizadeh, R., Alygizakis, N.A., Singer, H.P., Hollender, J., Thomaidis, N.S., Wide-scope target screening of >2000 emerging contaminants in wastewater samples with UPLC-Q-ToF-HRMS/MS and smart evaluation of its performance through the validation of 195 selected representative analytes. J. Hazard. Mater., 387, 2020, 121712, 10.1016/j.jhazmat.2019.121712.
Goto, A., Tue, N.M., Isobe, T., Takahashi, S., Tanabe, S., Kunisue, T., Nontarget and target screening of organohalogen compounds in mussels and sediment from Hiroshima Bay, Japan: occurrence of novel bioaccumulative substances. Environ. Sci. Technol. 54 (2020), 5480–5488, 10.1021/acs.est.9b06998.
Grabicova, K., Vojs Staňová, A., Koba Ucun, O., Borik, A., Randak, T., Grabic, R., Development of a robust extraction procedure for the HPLC-ESI-HRPS determination of multi-residual pharmaceuticals in biota samples. Anal. Chim. Acta. 1022 (2018), 53–60, 10.1016/j.aca.2018.04.011.
Hallstan, S., Grandin, U., Goedkoop, W., Current and modeled potential distribution of the zebra mussel (Dreissena polymorpha) in Sweden. Biol. Invasions. 12 (2010), 285–296, 10.1007/s10530-009-9449-9.
Heffernan, A.L., Gómez-Ramos, M.M., Gaus, C., Vijayasarathy, S., Bell, I., Hof, C., Mueller, J.F., Gómez-Ramos, M.J., Non-targeted, high resolution mass spectrometry strategy for simultaneous monitoring of xenobiotics and endogenous compounds in green sea turtles on the Great Barrier Reef. Sci. Total Environ. 599–600 (2017), 1251–1262, 10.1016/j.scitotenv.2017.05.016.
Hernández, F., Bakker, J., Bijlsma, L., de Boer, J., Botero-Coy, A.M., Bruinen de Bruin, Y., Fischer, S., Hollender, J., Kasprzyk-Hordern, B., Lamoree, M., López, F.J., ter Laak, T.L., van Leerdam, J.A., Sancho, J.V., Schymanski, E.L., de Voogt, P., Hogendoorn, E.A., The role of analytical chemistry in exposure science: Focus on the aquatic environment. Chemosphere 222 (2019), 564–583, 10.1016/j.chemosphere.2019.01.118.
Hinnenkamp, V., Klein, J., Meckelmann, S.W., Balsaa, P., Schmidt, T.C., Schmitz, O.J., Comparison of CCS values determined by traveling wave ion mobility mass spectrometry and drift tube ion mobility mass spectrometry. Anal. Chem. 90 (2018), 12042–12050, 10.1021/acs.analchem.8b02711.
Hollender, J., Schymanski, E.L., Singer, H.P., Ferguson, P.L., Nontarget screening with high resolution mass spectrometry in the environment: ready to go?. Environ. Sci. Technol. 51 (2017), 11505–11512, 10.1021/acs.est.7b02184.
Jacob, P., Barzen-Hanson, K.A., Helbling, D.E., Target and nontarget analysis of per- and polyfluoralkyl substances in wastewater from electronics fabrication facilities. Environ. Sci. Technol. 55 (2021), 2346–2356, 10.1021/acs.est.0c06690.
Kannan, K., Tao, L., Sinclair, E., Pastva, S.D., Jude, D.J., Giesy, J.P., Perfluorinated compounds in aquatic organisms at various trophic levels in a great lakes food chain. Arch. Environ. Contam. Toxicol. 48 (2005), 559–566, 10.1007/s00244-004-0133-x.
Kaufmann, A., Butcher, P., Maden, K., Walker, S., Widmer, M., Does the ion mobility resolving power as provided by commercially available ion mobility quadrupole time-of-flight mass spectrometry instruments permit the unambiguous identification of small molecules in complex matrices?. Anal. Chim. Acta. 1107 (2020), 113–126, 10.1016/j.aca.2020.02.032.
Kiefer, K., Müller, A., Singer, H., Hollender, J., New relevant pesticide transformation products in groundwater detected using target and suspect screening for agricultural and urban micropollutants with LC-HRMS. Water Res., 165, 2019, 114972, 10.1016/j.watres.2019.114972.
Lai, A., Singh, R.R., Kovalova, L., Jaeggi, O., Kondić, T., Schymanski, E.L., Retrospective non-target analysis to support regulatory water monitoring: from masses of interest to recommendations via in silico workflows. Environ. Sci. Eur., 33, 2021, 43, 10.1186/s12302-021-00475-1.
LCSB-ECI, Schymanski, Emma, Kondic, Todor, PubChem Team, Bolton, Evan, Thiessen, Paul, Zhang, Jeff, CCSbase Team, Krinsky, Ally, Ross, David H., Xu, Libin, PubChemLite for Exposomics (1 Jan 2021) + predicted CCS from CCSbase, (2021). http://doi.org/10.5281/zenodo.4456208.
Madgett, A.S., Yates, K., Webster, L., McKenzie, C., Brownlow, A., Moffat, C.F., The concentration and biomagnification of PCBs and PBDEs across four trophic levels in a marine food web. Environ. Pollut., 309, 2022, 119752, 10.1016/j.envpol.2022.119752.
Menger, F., Gago-Ferrero, P., Wiberg, K., Ahrens, L., Wide-scope screening of polar contaminants of concern in water: A critical review of liquid chromatography-high resolution mass spectrometry-based strategies. Trends Environ. Anal. Chem., 28, 2020, e00102.
Menger, F., 2021. Re-structuring UNIFI data for use in MetFrag. https://github.com/MengerFrankC/UNIFI_SpectrumExport (accessed May 6, 2021).
Mollerup, C.B., Mardal, M., Dalsgaard, P.W., Linnet, K., Barron, L.P., Prediction of collision cross section and retention time for broad scope screening in gradient reversed-phase liquid chromatography-ion mobility-high resolution accurate mass spectrometry. J. Chromatogr. A. 1542 (2018), 82–88, 10.1016/j.chroma.2018.02.025.
Moschet, C., Wittmer, I., Simovic, J., Junghans, M., Piazzoli, A., Singer, H., Stamm, C., Leu, C., Hollender, J., How a complete pesticide screening changes the assessment of surface water quality. Environ. Sci. Technol. 48 (2014), 5423–5432, 10.1021/es500371t.
Mrema, E.J., Rubino, F.M., Brambilla, G., Moretto, A., Tsatsakis, A.M., Colosio, C., Persistent organochlorinated pesticides and mechanisms of their toxicity. Toxicology 307 (2013), 74–88, 10.1016/j.tox.2012.11.015.
Munoz, G., Mercier, L., Duy, S.V., Liu, J., Sauvé, S., Houde, M., Bioaccumulation and trophic magnification of emerging and legacy per- and polyfluoroalkyl substances (PFAS) in a St. Lawrence River food web. Environ. Pollut., 309, 2022, 119739, 10.1016/j.envpol.2022.119739.
Nilsen, E., Smalling, K.L., Ahrens, L., Gros, M., Miglioranza, K.S.B., Picó, Y., Schoenfuss, H.L., Critical review: Grand challenges in assessing the adverse effects of contaminants of emerging concern on aquatic food webs. Environ. Toxicol. Chem. 38 (2019), 46–60, 10.1002/etc.4290.
Parolini, M., Magni, S., Castiglioni, S., Zuccato, E., Binelli, A., Realistic mixture of illicit drugs impaired the oxidative status of the zebra mussel (Dreissena polymorpha). Chemosphere 128 (2015), 96–102, 10.1016/j.chemosphere.2014.12.092.
Peter, K.T., Tian, Z., Wu, C., Lin, P., White, S., Du, B., McIntyre, J.K., Scholz, N.L., Kolodziej, E.P., Using high-resolution mass spectrometry to identify organic contaminants linked to urban stormwater mortality syndrome in coho salmon. Environ. Sci. Technol. 52 (2018), 10317–10327, 10.1021/acs.est.8b03287.
Plassmann, M.M., Fischer, S., Benskin, J.P., Nontarget time trend screening in human blood. Environ. Sci. Technol. Lett. 5 (2018), 335–340, 10.1021/acs.estlett.8b00196.
Rebryk, A., Haglund, P., Non-targeted screening workflows for gas chromatography–high-resolution mass spectrometry analysis and identification of biomagnifying contaminants in biota samples. Anal. Bioanal. Chem. 413 (2021), 479–501, 10.1007/s00216-020-03018-4.
Regueiro, J., Negreira, N., Berntssen, M.H.G., Ion-mobility-derived collision cross section as an additional identification point for multiresidue screening of pesticides in fish feed. Anal. Chem. 88 (2016), 11169–11177, 10.1021/acs.analchem.6b03381.
Rehrl, A.-L., Golovko, O., Ahrens, L., Köhler, S., Spatial and seasonal trends of organic micropollutants in Sweden's most important drinking water reservoir. Chemosphere, 249, 2020, 126168, 10.1016/j.chemosphere.2020.126168.
Ross, D.H., Cho, J.H., Xu, L., Breaking down structural diversity for comprehensive prediction of ion-neutral collision cross sections. Anal. Chem. 92 (2020), 4548–4557, 10.1021/acs.analchem.9b05772.
Ruttkies, C., Neumann, S., Posch, S., Improving MetFrag with statistical learning of fragment annotations. BMC Bioinf., 20, 2019, 376, 10.1186/s12859-019-2954-7.
Schlüsener, M.P., Kunkel, U., Ternes, T.A., Quaternary triphenylphosphonium compounds: A new class of environmental pollutants. Environ. Sci. Technol. 49 (2015), 14282–14291, 10.1021/acs.est.5b03926.
Schymanski, E.L., Jeon, J., Gulde, R., Fenner, K., Ruff, M., Singer, H.P., Hollender, J., Identifying small molecules via high resolution mass spectrometry: communicating confidence. Environ. Sci. Technol. 48 (2014), 2097–2098, 10.1021/es5002105.
Schymanski, E.L., Ruttkies, C., Krauss, M., Brouard, C., Kind, T., Dührkop, K., Allen, F., Vaniya, A., Verdegem, D., Böcker, S., Rousu, J., Shen, H., Tsugawa, H., Sajed, T., Fiehn, O., Ghesquière, B., Neumann, S., Critical assessment of small molecule identification 2016: automated methods. J. Cheminformatics., 9, 2017, 22, 10.1186/s13321-017-0207-1.
Schymanski, E.L., Kondić, T., Neumann, S., Thiessen, P.A., Zhang, J., Bolton, E.E., Empowering large chemical knowledge bases for exposomics: PubChemLite meets MetFrag. J. Cheminformatics., 13, 2021, 19, 10.1186/s13321-021-00489-0.
Schymanski, E., 2021. schymane/ReSOLUTION, https://github.com/schymane/ReSOLUTION.
Stephan, S., Hippler, J., Köhler, T., Deeb, A.A., Schmidt, T.C., Schmitz, O.J., Contaminant screening of wastewater with HPLC-IM-qTOF-MS and LC+LC-IM-qTOF-MS using a CCS database. Anal. Bioanal. Chem. 408 (2016), 6545–6555, 10.1007/s00216-016-9820-5.
Tian, Z., Peter, K.T., Gipe, A.D., Zhao, H., Hou, F., Wark, D.A., Khangaonkar, T., Kolodziej, E.P., James, C.A., Suspect and nontarget screening for contaminants of emerging concern in an urban estuary. Environ. Sci. Technol. 54 (2020), 889–901, 10.1021/acs.est.9b06126.
Tian, Z., Zhao, H., Peter, K.T., Gonzalez, M., Wetzel, J., Wu, C., Hu, X., Prat, J., Mudrock, E., Hettinger, R., Cortina, A.E., Biswas, R.G., Kock, F.V.C., Soong, R., Jenne, A., Du, B., Hou, F., He, H., Lundeen, R., Gilbreath, A., Sutton, R., Scholz, N.L., Davis, J.W., Dodd, M.C., Simpson, A., McIntyre, J.K., Kolodziej, E.P., A ubiquitous tire rubber–derived chemical induces acute mortality in coho salmon. Science 371:6525 (2021), 185–189.
Wang, Y., Yu, N., Zhu, X., Guo, H., Jiang, J., Wang, X., Shi, W., Wu, J., Yu, H., Wei, S., Suspect and nontarget screening of per- and polyfluoroalkyl substances in wastewater from a fluorochemical manufacturing park. Environ. Sci. Technol. 52 (2018), 11007–11016, 10.1021/acs.est.8b03030.
Wang, X., Yu, N., Yang, J., Jin, L., Guo, H., Shi, W., Zhang, X., Yang, L., Yu, H., Wei, S., Suspect and non-target screening of pesticides and pharmaceuticals transformation products in wastewater using QTOF-MS. Environ. Int., 137, 2020, 105599, 10.1016/j.envint.2020.105599.
Wolf, S., Schmidt, S., Müller-Hannemann, M., Neumann, S., In silico fragmentation for computer assisted identification of metabolite mass spectra. BMC Bioinf., 11, 2010, 148, 10.1186/1471-2105-11-148.
Xing, J., Zang, M., Liu, H., The application of a novel high-resolution mass spectrometry-based analytical strategy to rapid metabolite profiling of a dual drug combination in humans. Anal. Chim. Acta. 993 (2017), 38–46, 10.1016/j.aca.2017.08.047.
Zhou, Z., Shen, X., Tu, J., Zhu, Z.-J., Large-scale prediction of collision cross-section values for metabolites in ion mobility-mass spectrometry. Anal. Chem. 88 (2016), 11084–11091, 10.1021/acs.analchem.6b03091.
