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      Contaminants of emerging concern in tributaries to the Laurentian Great Lakes: I. Patterns of occurrence

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          Abstract

          Human activities introduce a variety of chemicals to the Laurentian Great Lakes including pesticides, pharmaceuticals, flame retardants, plasticizers, and solvents (collectively referred to as contaminants of emerging concern or CECs) potentially threatening the vitality of these valuable ecosystems. We conducted a basin-wide study to identify the presence of CECs and other chemicals of interest in 12 U.S. tributaries to the Laurentian Great Lakes during 2013 and 2014. A total of 292 surface-water and 80 sediment samples were collected and analyzed for approximately 200 chemicals. A total of 32 and 28 chemicals were detected in at least 30% of water and sediment samples, respectively. Concentrations ranged from 0.0284 (indole) to 72.2 (cholesterol) μg/L in water and 1.75 (diphenhydramine) to 20,800 μg/kg (fluoranthene) in sediment. Cluster analyses revealed chemicals that frequently co-occurred such as pharmaceuticals and flame retardants at sites receiving similar inputs such as wastewater treatment plant effluent. Comparison of environmental concentrations to water and sediment-quality benchmarks revealed that polycyclic aromatic hydrocarbon concentrations often exceeded benchmarks in both water and sediment. Additionally, bis(2-ethylhexyl) phthalate and dichlorvos concentrations exceeded water-quality benchmarks in several rivers. Results from this study can be used to understand organism exposure, prioritize river basins for future management efforts, and guide detailed assessments of factors influencing transport and fate of CECs in the Great Lakes Basin.

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          Most cited references38

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          EU-wide monitoring survey on emerging polar organic contaminants in wastewater treatment plant effluents.

          In the year 2010, effluents from 90 European wastewater treatment plants (WWTPs) were analyzed for 156 polar organic chemical contaminants. The analyses were complemented by effect-based monitoring approaches aiming at estrogenicity and dioxin-like toxicity analyzed by in vitro reporter gene bioassays, and yeast and diatom culture acute toxicity optical bioassays. Analyses of organic substances were performed by solid-phase extraction (SPE) or liquid-liquid extraction (LLE) followed by liquid chromatography tandem mass spectrometry (LC-MS-MS) or gas chromatography high-resolution mass spectrometry (GC-HRMS). Target microcontaminants were pharmaceuticals and personal care products (PPCPs), veterinary (antibiotic) drugs, perfluoroalkyl substances (PFASs), organophosphate ester flame retardants, pesticides (and some metabolites), industrial chemicals such as benzotriazoles (corrosion inhibitors), iodinated x-ray contrast agents, and gadolinium magnetic resonance imaging agents; in addition biological endpoints were measured. The obtained results show the presence of 125 substances (80% of the target compounds) in European wastewater effluents, in concentrations ranging from low nanograms to milligrams per liter. These results allow for an estimation to be made of a European median level for the chemicals investigated in WWTP effluents. The most relevant compounds in the effluent waters with the highest median concentration levels were the artificial sweeteners acesulfame and sucralose, benzotriazoles (corrosion inhibitors), several organophosphate ester flame retardants and plasticizers (e.g. tris(2-chloroisopropyl)phosphate; TCPP), pharmaceutical compounds such as carbamazepine, tramadol, telmisartan, venlafaxine, irbesartan, fluconazole, oxazepam, fexofenadine, diclofenac, citalopram, codeine, bisoprolol, eprosartan, the antibiotics trimethoprim, ciprofloxacine, sulfamethoxazole, and clindamycine, the insect repellent N,N'-diethyltoluamide (DEET), the pesticides MCPA and mecoprop, perfluoroalkyl substances (such as PFOS and PFOA), caffeine, and gadolinium. Copyright © 2013 Elsevier Ltd. All rights reserved.
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            Impacts of emerging organic contaminants on freshwater resources: review of recent occurrences, sources, fate and effects.

            Rapid urbanization and frequent disposal of wastewater to surface water cause widespread contamination of freshwater supplies with emerging contaminants, such as pharmaceuticals, insecticides, surfactants, endocrine disruptors, including hormones. Although these organic contaminants may be present at trace levels, their adverse effects on aquatic life, animals and even humans are a growing concern. Numerous studies have been published on the occurrence and fate of emerging organic contaminants in different parts of the world, spanning a wide range of sources and aquatic environments including freshwater catchments, effluent wastewater streams, lakes, rivers, reservoirs, estuaries and marine waters. This paper reviews recent studies on the occurrence and fate of frequently detected pharmaceuticals and hormones and identifies areas that merit further research. Copyright © 2010 Elsevier B.V. All rights reserved.
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              EU-wide survey of polar organic persistent pollutants in European river waters.

              This study provides the first EU-wide reconnaissance of the occurrence of polar organic persistent pollutants in European river waters. More than 100 individual water samples from over 100 European rivers from 27 European Countries were analysed for 35 selected compounds, comprising pharmaceuticals, pesticides, PFOS, PFOA, benzotriazoles, hormones, and endocrine disrupters. Around 40 laboratories participated in this sampling exercise. The most frequently and at the highest concentration levels detected compounds were benzotriazole, caffeine, carbamazepine, tolyltriazole, and nonylphenoxy acetic acid (NPE(1)C). Only about 10% of the river water samples analysed could be classified as "very clean" in terms of chemical pollution. The rivers responsible for the major aqueous emissions of PFOS and PFOA from the European Continent could be identified. For the target compounds chosen, we are proposing "indicative warning levels" in surface waters, which are (for most compounds) close to the 90th percentile of all water samples analysed.
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                Author and article information

                Contributors
                Role: Data curationRole: Formal analysisRole: Project administrationRole: ValidationRole: VisualizationRole: Writing – original draftRole: Writing – review & editing
                Role: Data curationRole: Formal analysisRole: Funding acquisitionRole: Project administrationRole: ValidationRole: Writing – review & editing
                Role: ConceptualizationRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: SupervisionRole: Writing – review & editing
                Role: ConceptualizationRole: InvestigationRole: ResourcesRole: Writing – review & editing
                Role: ConceptualizationRole: InvestigationRole: ResourcesRole: VisualizationRole: Writing – review & editing
                Role: ConceptualizationRole: InvestigationRole: ResourcesRole: Writing – review & editing
                Role: ConceptualizationRole: InvestigationRole: ResourcesRole: Writing – review & editing
                Role: ConceptualizationRole: InvestigationRole: ResourcesRole: Writing – review & editing
                Role: ConceptualizationRole: Formal analysisRole: InvestigationRole: Project administrationRole: ResourcesRole: SupervisionRole: ValidationRole: Writing – original draftRole: Writing – review & editing
                Role: Editor
                Journal
                PLoS One
                PLoS ONE
                plos
                plosone
                PLoS ONE
                Public Library of Science (San Francisco, CA USA )
                1932-6203
                27 September 2017
                2017
                : 12
                : 9
                : e0182868
                Affiliations
                [1 ] U.S. Geological Survey, Mounds View, Minnesota, United States of America
                [2 ] U.S. Geological Survey, Grand Rapids, Minnesota, United States of America
                [3 ] U.S. Fish and Wildlife Service, Columbus, Ohio, United States of America
                [4 ] U.S. Fish and Wildlife Service, Madison, Wisconsin, United States of America
                [5 ] U.S. Fish and Wildlife Service, Cortland, New York, United States of America
                [6 ] Metropolitan Water Reclamation District of Greater Chicago, Cicero, IL, United States of America
                [7 ] U.S. Fish and Wildlife Service, Chubbuck, Idaho, United States of America
                [8 ] Department of Biology, St. Cloud State University, St. Cloud, Minnesota, United States of America
                [9 ] U.S. Fish and Wildlife Service, Bloomington, Minnesota, United States of America
                Purdue University, UNITED STATES
                Author notes

                Competing Interests: The authors have declared that no competing interests exist.

                Author information
                http://orcid.org/0000-0002-1414-3024
                Article
                PONE-D-17-18203
                10.1371/journal.pone.0182868
                5617142
                28953889
                2c8a5fa0-ec0e-48ec-9625-32b96fecf0ec

                This is an open access article, free of all copyright, and may be freely reproduced, distributed, transmitted, modified, built upon, or otherwise used by anyone for any lawful purpose. The work is made available under the Creative Commons CC0 public domain dedication.

                History
                : 11 May 2017
                : 25 July 2017
                Page count
                Figures: 3, Tables: 3, Pages: 21
                Funding
                Funded by: Great Lakes Restoration Initiative
                Award Recipient :
                MEB and KEL (U.S. Geological Survey) received funding from the U.S. Fish and Wildlife Service for this project. Funding was provided from the Great Lakes Restoration Initiative through the U.S. Fish and Wildlife Service’s CEC Team. In-kind support from the Metropolitan Water Reclamation District of Greater Chicago is acknowledged.
                Categories
                Research Article
                Earth Sciences
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                Petrology
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                Geology
                Sedimentary Geology
                Sediment
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                Marine and Aquatic Sciences
                Bodies of Water
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                Ecology and Environmental Sciences
                Aquatic Environments
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                Biology and Life Sciences
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                Custom metadata
                All data are available online at doi.org/10.5066/F7TH8JS6 and doi.org/10.5066/F7DF6P9D.

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