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Tracing Urban Wastewater Contaminants into the Atlantic Ocean by Nontarget Screening

  • Pablo A. Lara-Martín*
    Pablo A. Lara-Martín
    Physical Chemistry Department, Faculty of Marine and Environmental Sciences, University of Cadiz, Campus of International Excellence of the Sea (CEI·MAR), 11510 Puerto Real, Spain
    *Phone: +34 956 016159. Email: [email protected]
  • Aurea C. Chiaia-Hernández
    Aurea C. Chiaia-Hernández
    Eawag, Swiss Federal Institute of Aquatic Science and Technology, 8600 Dübendorf, Switzerland
    Institute of Geography and Oeschger Centre for Climate Change Research, University of Bern, 3012 Bern, Switzerland
  • Miriam Biel-Maeso
    Miriam Biel-Maeso
    Physical Chemistry Department, Faculty of Marine and Environmental Sciences, University of Cadiz, Campus of International Excellence of the Sea (CEI·MAR), 11510 Puerto Real, Spain
  • Rosa M. Baena-Nogueras
    Rosa M. Baena-Nogueras
    Physical Chemistry Department, Faculty of Marine and Environmental Sciences, University of Cadiz, Campus of International Excellence of the Sea (CEI·MAR), 11510 Puerto Real, Spain
  • , and 
  • Juliane Hollender
    Juliane Hollender
    Eawag, Swiss Federal Institute of Aquatic Science and Technology, 8600 Dübendorf, Switzerland
    Institute of Biogeochemistry and Pollutant Dynamics, IBP, ETH Zurich, 8092 Zurich, Switzerland
Cite this: Environ. Sci. Technol. 2020, 54, 7, 3996–4005
Publication Date (Web):March 2, 2020
https://doi.org/10.1021/acs.est.9b06114
Copyright © 2020 American Chemical Society

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    Abstract

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    Oceans are the ultimate sink for many of the over 100 million man-made substances. Until now, monitoring was limited to a reduced number of targeted persistent organic pollutants, reaching open waters mainly via atmospheric deposition. However, the composition and fate of the thousands of pollutants reaching the marine environment though wastewater discharges from coastal sources remain largely unexplored. By combining a newly developed nontarget screening (NTS) workflow and high-resolution mass spectrometry (HRMS), we have identified over 500 sewage-derived contaminants occurring in the ocean. Samples from the NE Atlantic contained this anthropogenic imprint at distances over 50 km from the coastline and >500 m depth, beyond the continental margin. The range of identified compounds spans from pharmaceuticals and personal care products to food additives and industrial chemicals, including several that have never been reported in the environment, as they escaped conventional targeted analytical methods. Predicting the effects of the continuous input of this chemical “cocktail” on marine ecosystems is a formidable challenge, since 40% of the detected compounds lack information regarding their use and ecotoxicity.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.9b06114.

    • Materials and Methods, principal component analysis of normalized signal intensities of all organic compounds, mass vs retention time plots for detected compounds corresponding to different sample types, number of sewage-derived compounds detected in water samples, examples of contaminants identified at confidence levels 1, 2, and 3, Kendrick mass defect plots showing the occurrence of homologous series for CHNOS sewage-derived contaminants, normalized signal intensities of potential sewage markers, and linear correlation between retention time (RT) and log P for all the standards (PDF)

    • List of reference standards for identification of contaminants and internal standards, list of tentative sewage-derived compounds detected by HPLC-ESI-HRMS, environmental and food safety and NORMAN network compound databases used in this work for suspect screening, and prioritized sewage-derived contaminants identified by HPLC-ESI-HRMS (ZIP)

    • MS and MS/MS spectra of sewage-derived compounds in selected wastewater effluent and coastal samples (ZIP)

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