Integrating Contaminant Source Indicators, Water Quality Measures, and Ecotoxicity to Characterize Contaminant Mixtures and Per- and Polyfluoroalkyl Substance (PFAS) Variability in an Urban Watershed

Jonathan R. Behrens; Abigail S. Joyce; P. Lee Ferguson; Dana W. Kolpin; Nishad Jayasundara; Nadia Barbo; Emily S. Bernhardt

doi:10.1021/acs.est.4c14607

Integrating Contaminant Source Indicators, Water Quality Measures, and Ecotoxicity to Characterize Contaminant Mixtures and Per- and Polyfluoroalkyl Substance (PFAS) Variability in an Urban Watershed

Jonathan R. Behrens, Abigail S. Joyce, P. Lee Ferguson, Dana W. Kolpin, Nishad Jayasundara, Nadia Barbo, Emily S. Bernhardt

Biogeochemical Dynamics

Research output: Contribution to journal › Article › peer-review

Abstract

Thousands of chemical contaminants threaten watersheds but are time and cost prohibitive to monitor. Identifying their sources, transport, and ecological risk is limited in heterogeneous urban watersheds. We present an integrative watershed approach using source-specific indicator compounds, common water quality measures, and ecotoxicity assays to examine the distribution of contaminant mixtures in an urbanized watershed. Indicator compound concentrations were temporally and spatially distributed for treated/untreated sewage (sucralose, artificial sweetener), road runoff (diphenyl-guanidine [DPG] and 6PPD-quinone [6PPD-Q], automobile tire additives), and lawncare runoff (aminomethanephosphonic acid (AMPA), major degradant of the herbicide glyphosate). Sucralose was predominately sourced from treated wastewater; measurable concentrations in tributaries indicated raw sewage inputs. DPG and 6PPD-Q concentrations correlated to road density during base flow and were elevated during stormflow. AMPA was measurable spring through fall, especially where lawns were dense. When specific sources dominated flow, water quality measures correlated with wastewater (sulfate, potassium, chloride, and sodium) and road runoff (chromium and lead) indicators. The limited behavioral toxicity observed in exposed zebrafish (Danio rerio) (18%) was not well explained by source-indicators. PFAS concentrations were highly variable spatially but not well explained by our source-specific indicator compounds. More costly compound-specific monitoring may be necessary when multiple sources exist or when unexpected toxicity trends occur.

Original language	English
Journal	Environmental Science and Technology
DOIs	https://doi.org/10.1021/acs.est.4c14607
State	Accepted/In press - 2025

Funding

Work was supported by the Duke Science and Technology Initiative Seed Grant, Bass Connections at Duke University (2021–2023), North Carolina Water Resources Research Institute Graduate Fellowship, Duke Forest, and the Duke University Superfund Research Center (National Institute of Environmental Health Sciences award number 5P42ES010356-21). Programmatic support was provided by the Environmental Health Program of the U.S. Geological Survey Ecosystems Mission Area. Limited support was provided by the Watershed Dynamics and Evolution Science Focus Area at Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. We thank Steve Anderson, Brooke Hassett, Nelson Rivera, and Melissa Chernick for analysis support and community collaborators Rickie White and Laura Stroud. Any use of trade, firm, or product names is for descriptive purposes only and does not imply endorsement by the U.S. Government or the authors.

Keywords

monitoring
pollutant
runoff
stormwater
surface water
wastewater

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10.1021/acs.est.4c14607

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Behrens, J. R., Joyce, A. S., Ferguson, P. L., Kolpin, D. W., Jayasundara, N., Barbo, N., & Bernhardt, E. S. (Accepted/In press). Integrating Contaminant Source Indicators, Water Quality Measures, and Ecotoxicity to Characterize Contaminant Mixtures and Per- and Polyfluoroalkyl Substance (PFAS) Variability in an Urban Watershed. Environmental Science and Technology. https://doi.org/10.1021/acs.est.4c14607

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abstract = "Thousands of chemical contaminants threaten watersheds but are time and cost prohibitive to monitor. Identifying their sources, transport, and ecological risk is limited in heterogeneous urban watersheds. We present an integrative watershed approach using source-specific indicator compounds, common water quality measures, and ecotoxicity assays to examine the distribution of contaminant mixtures in an urbanized watershed. Indicator compound concentrations were temporally and spatially distributed for treated/untreated sewage (sucralose, artificial sweetener), road runoff (diphenyl-guanidine [DPG] and 6PPD-quinone [6PPD-Q], automobile tire additives), and lawncare runoff (aminomethanephosphonic acid (AMPA), major degradant of the herbicide glyphosate). Sucralose was predominately sourced from treated wastewater; measurable concentrations in tributaries indicated raw sewage inputs. DPG and 6PPD-Q concentrations correlated to road density during base flow and were elevated during stormflow. AMPA was measurable spring through fall, especially where lawns were dense. When specific sources dominated flow, water quality measures correlated with wastewater (sulfate, potassium, chloride, and sodium) and road runoff (chromium and lead) indicators. The limited behavioral toxicity observed in exposed zebrafish (Danio rerio) (18\%) was not well explained by source-indicators. PFAS concentrations were highly variable spatially but not well explained by our source-specific indicator compounds. More costly compound-specific monitoring may be necessary when multiple sources exist or when unexpected toxicity trends occur.",

keywords = "monitoring, pollutant, runoff, stormwater, surface water, wastewater",

author = "Behrens, \{Jonathan R.\} and Joyce, \{Abigail S.\} and Ferguson, \{P. Lee\} and Kolpin, \{Dana W.\} and Nishad Jayasundara and Nadia Barbo and Bernhardt, \{Emily S.\}",

note = "Publisher Copyright: {\textcopyright} 2025 The Authors. Published by American Chemical Society.",

year = "2025",

doi = "10.1021/acs.est.4c14607",

language = "English",

journal = "Environmental Science and Technology",

issn = "0013-936X",

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Behrens, JR, Joyce, AS, Ferguson, PL, Kolpin, DW, Jayasundara, N, Barbo, N & Bernhardt, ES 2025, 'Integrating Contaminant Source Indicators, Water Quality Measures, and Ecotoxicity to Characterize Contaminant Mixtures and Per- and Polyfluoroalkyl Substance (PFAS) Variability in an Urban Watershed', Environmental Science and Technology. https://doi.org/10.1021/acs.est.4c14607

Integrating Contaminant Source Indicators, Water Quality Measures, and Ecotoxicity to Characterize Contaminant Mixtures and Per- and Polyfluoroalkyl Substance (PFAS) Variability in an Urban Watershed. / Behrens, Jonathan R.; Joyce, Abigail S.; Ferguson, P. Lee et al.
In: Environmental Science and Technology, 2025.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Integrating Contaminant Source Indicators, Water Quality Measures, and Ecotoxicity to Characterize Contaminant Mixtures and Per- and Polyfluoroalkyl Substance (PFAS) Variability in an Urban Watershed

AU - Behrens, Jonathan R.

AU - Joyce, Abigail S.

AU - Ferguson, P. Lee

AU - Kolpin, Dana W.

AU - Jayasundara, Nishad

AU - Barbo, Nadia

AU - Bernhardt, Emily S.

PY - 2025

Y1 - 2025

N2 - Thousands of chemical contaminants threaten watersheds but are time and cost prohibitive to monitor. Identifying their sources, transport, and ecological risk is limited in heterogeneous urban watersheds. We present an integrative watershed approach using source-specific indicator compounds, common water quality measures, and ecotoxicity assays to examine the distribution of contaminant mixtures in an urbanized watershed. Indicator compound concentrations were temporally and spatially distributed for treated/untreated sewage (sucralose, artificial sweetener), road runoff (diphenyl-guanidine [DPG] and 6PPD-quinone [6PPD-Q], automobile tire additives), and lawncare runoff (aminomethanephosphonic acid (AMPA), major degradant of the herbicide glyphosate). Sucralose was predominately sourced from treated wastewater; measurable concentrations in tributaries indicated raw sewage inputs. DPG and 6PPD-Q concentrations correlated to road density during base flow and were elevated during stormflow. AMPA was measurable spring through fall, especially where lawns were dense. When specific sources dominated flow, water quality measures correlated with wastewater (sulfate, potassium, chloride, and sodium) and road runoff (chromium and lead) indicators. The limited behavioral toxicity observed in exposed zebrafish (Danio rerio) (18%) was not well explained by source-indicators. PFAS concentrations were highly variable spatially but not well explained by our source-specific indicator compounds. More costly compound-specific monitoring may be necessary when multiple sources exist or when unexpected toxicity trends occur.

AB - Thousands of chemical contaminants threaten watersheds but are time and cost prohibitive to monitor. Identifying their sources, transport, and ecological risk is limited in heterogeneous urban watersheds. We present an integrative watershed approach using source-specific indicator compounds, common water quality measures, and ecotoxicity assays to examine the distribution of contaminant mixtures in an urbanized watershed. Indicator compound concentrations were temporally and spatially distributed for treated/untreated sewage (sucralose, artificial sweetener), road runoff (diphenyl-guanidine [DPG] and 6PPD-quinone [6PPD-Q], automobile tire additives), and lawncare runoff (aminomethanephosphonic acid (AMPA), major degradant of the herbicide glyphosate). Sucralose was predominately sourced from treated wastewater; measurable concentrations in tributaries indicated raw sewage inputs. DPG and 6PPD-Q concentrations correlated to road density during base flow and were elevated during stormflow. AMPA was measurable spring through fall, especially where lawns were dense. When specific sources dominated flow, water quality measures correlated with wastewater (sulfate, potassium, chloride, and sodium) and road runoff (chromium and lead) indicators. The limited behavioral toxicity observed in exposed zebrafish (Danio rerio) (18%) was not well explained by source-indicators. PFAS concentrations were highly variable spatially but not well explained by our source-specific indicator compounds. More costly compound-specific monitoring may be necessary when multiple sources exist or when unexpected toxicity trends occur.

KW - monitoring

KW - pollutant

KW - runoff

KW - stormwater

KW - surface water

KW - wastewater

UR - https://www.scopus.com/pages/publications/105009750462

U2 - 10.1021/acs.est.4c14607

DO - 10.1021/acs.est.4c14607

M3 - Article

C2 - 40609970

AN - SCOPUS:105009750462

SN - 0013-936X

JO - Environmental Science and Technology

JF - Environmental Science and Technology

ER -

Integrating Contaminant Source Indicators, Water Quality Measures, and Ecotoxicity to Characterize Contaminant Mixtures and Per- and Polyfluoroalkyl Substance (PFAS) Variability in an Urban Watershed

Abstract

Funding

Keywords

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