Dataset Information

Identifying and Managing Aqueous Film-Forming Foam-Derived Per- and Polyfluoroalkyl Substances in the Environment.

ABSTRACT: The use of aqueous film-forming foam (AFFF) has resulted in the widespread occurrence of per- and polyfluoroalkyl substances (PFAS) in groundwater, drinking water, soils, sediments, and receiving waters throughout the United States and other countries. We present the research and development efforts to date by the Strategic Environmental Research and Development Program (SERDP) and the Environmental Security Technology Certification Program (ESTCP) to measure PFAS in the environment, characterize AFFF-associated sources of PFAS, understand PFAS fate and behavior in the environment, assess the risk to ecological receptors, develop in situ and ex situ treatment technologies for groundwater, treat soils and investigation-derived wastes, and examine the ecotoxicity of PFAS-free fire suppression formulations. Environ Toxicol Chem 2021;40:24-36. © 2020 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC. This article has been contributed to by US Government employees and their work is in the public domain in the USA.

SUBMITTER: Leeson A

PROVIDER: S-EPMC7839684 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Identifying and Managing Aqueous Film-Forming Foam-Derived Per- and Polyfluoroalkyl Substances in the Environment.

Leeson Andrea A Thompson Timothy T Stroo Hans F HF Anderson Richard H RH Speicher Jason J Mills Marc A MA Willey Janice J Coyle Charles C Ghosh Rajat R Lebrón Carmen C Patton Cara C

Environmental toxicology and chemistry 20201209 1

The use of aqueous film-forming foam (AFFF) has resulted in the widespread occurrence of per- and polyfluoroalkyl substances (PFAS) in groundwater, drinking water, soils, sediments, and receiving waters throughout the United States and other countries. We present the research and development efforts to date by the Strategic Environmental Research and Development Program (SERDP) and the Environmental Security Technology Certification Program (ESTCP) to measure PFAS in the environment, characteriz ...[more]

PMID: 33026660

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Project description:Drinking water contaminated by fluorosurfactant-based aqueous film-forming foams (AFFF) is a source of human exposure to poly- and perfluoroalkyl substances (PFAS). However, assessment of bioaccumulation potentials of diverse PFAS in commercial products such as AFFF have been insufficient and challenging, especially due to a lack of analytical standards. Here we explore the value of suspect screening, equilibrium dialysis, and molecular-docking simulations to identify potentially bioaccumulative PFAS. We exposed human serum albumin (HSA) protein to dilutions of a legacy AFFF produced by 3M in 1999 using equilibrium dialysis and screened in-vitro protein-binding affinities using high-resolution mass spectrometry (HRMS). Through suspect screening, we identified 32 PFAS and 18 hydrocarbon surfactants in the AFFF that bound to HSA. Quantification of noncovalent association constants for 26 PFAS standards confirmed that many PFAS, including the short-chain perfluoropropane sulfonic acid (log Ka= 4.1 ± 0.2 M-1), exhibit strong binding affinities with HSA. At least five PFAS in AFFF (including three PFAS with less than five perfluorocarbons) remained bound to the precipitated HSA pellet after extensive solvent washing-an indication of high PFAS binding potential. Three PFAS (PFBS, PFOS, and PFOA) were confirmed in the protein pellet with analytical standards and quantified after acid digestion-this sample fraction accounted for 5 to 20% of each compound mass in the sample. We calculated pseudo-bioconcentration factors (BCFpseudo) for PFAS that suspect screening flagged as noncovalently bound or potentially covalently bound. Most PFAS exhibiting high BCFpseudo, especially those with seven perfluorocarbons, contained a carboxylic acid or a sulfonic acid. Finally, we used molecular docking to simulate HSA binding affinities for 62 ligands (26 PFAS targets, 18 PFAS qualified in AFFF, and 18 hydrocarbon surfactants qualified in AFFF). We found that molecular docking can effectively separate HSA-binding and -nonbinding compounds in AFFF. In-vitro and in-silico approaches described in this study provide replicable, high-throughput workflows for assessing bioaccumulation potentials of diverse PFAS in commercial products.

Project description:BackgroundPer- and polyfluoroalkyl substances (PFAS) are a chemical class widely used in industrial and commercial applications because of their unique physical and chemical properties. Between 2013 and 2016 PFAS were detected in public water systems and private wells in El Paso County, Colorado. The contamination was likely due to aqueous film forming foams used at a nearby Air Force base.ObjectiveTo cross-sectionally describe the serum concentrations of PFAS in a highly exposed community, estimate associations with drinking water source, and explore potential demographic and behavioral predictors.MethodsIn June 2018, serum PFAS concentrations were quantified and questionnaires administered in 213 non-smoking adult (ages 19-93) participants residing in three affected water districts. Twenty PFAS were quantified and those detected in >50% of participants were analyzed: perfluorohexane sulfonate (PFHxS), perfluorooctane sulfonate (PFOS), perfluorooctanoate (PFOA), perfluorononanoate (PFNA) and perfluoroheptane sulfonate (PFHpS). Unadjusted associations were estimated between serum PFAS concentrations and several predictors, including water consumption, demographics, personal behaviors and employment. A multiple linear regression model estimated adjusted associations with smoking history.ResultsStudy participants' median PFHxS serum concentration (14.8 ng/mL) was approximately 12 times as high as the U.S. national average. Median serum concentrations for PFOS, PFOA, PFNA and PFHpS were 9.7 ng/mL, 3.0 ng/mL, 0.4 ng/mL and 0.2 ng/mL, respectively. Determinants of PFHxS serum concentrations were water district of residence, frequency of bottled water consumption, age, race/ethnicity, and smoking history. Determinants of serum concentrations for the other four PFAS evaluated included: water district of residence, bottled water consumption, age, sex, race/ethnicity, smoking history, and firefighter or military employment.ConclusionsDeterminants of serum concentrations for multiple PFAS, including PFHxS, included water district of residence and frequency of bottled water consumption. Participants' dominant PFAS exposure route was likely consumption of PFAS-contaminated water, but certain demographic and behavioral characteristics also predicted serum concentrations.

Project description:PurposePer- and polyfluoroalkyl substances (PFAS) have been found to be widespread, extremely persistent and bioaccumulative with toxicity tendencies. Pre-synthesized nanocomposite-activated carbons, referred to, as physically activated maize tassel silver (PAMTAg) and chemically activated maize tassel silver (CAMTAg) were utilized in the present study. They were used for the removal of 10 PFAS from aqueous solutions.MethodsThe nanocomposite-activated carbons were characterized via scanning electron microscopy (SEM), Fourier transform infrared (FTIR) spectroscopy, Brunauer Emmett Teller (BET) and other techniques. Batch equilibrium experiments were conducted in order to investigate the effects of solution pH, adsorbent dosage, initial PFAS concentration and temperature on the removal of PFAS using PAMTAg and CAMTAg. Langmuir and Freundlich adsorption isotherm models were used to analyse the equilibrium data obtained.ResultsMaximum adsorption capacities of 454.1 mg/g (0.91 mmol/g) and 321.2 mg/g (0.78 mmol/g) were recorded for perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA), respectively using CAMTAg. The values recorded for the Gibbs' free energy (ΔG°) for the adsorption of PFOS and PFOA onto PAMTAg and CAMTAg were negative; PFOS (-9.61, -9.99 and - 10.39), PFOA (-8.77, -9.76 and - 10.21) using PAMTAg; and PFOS (-13.70, -12.70 and - 12.37), PFOA (-12.86, -12.21 and - 11.17) using CAMTAg. Therefore, the adsorption processes were spontaneous and feasible. The values recorded for enthalpy (ΔH°) (kJ/mol) for the adsorption of PFOS (-26.15) and PFOA (-35.86) onto CAMTAg were negative, indicating that the adsorption mechanism is exothermic in nature. Positive values were recorded for ΔH° for the adsorption of PFOS (2.32) and PFOA (12.69) onto PAMTAg, indicative of an endothermic adsorption mechanism. Positive entropy (ΔS°) values (0.04 and 0.07) were recorded for PFOS and PFOA using PAMTAg; whereas negative values (-0.04 and - 0.08) were recorded for ΔS° using CAMTAg. A positive ΔS° indicates an increase in randomness of the adsorbate at the solid-solution interface and the reverse is the case for a negative ΔS°.ConclusionThe interplay of electrostatic attraction and hydrophobic interactions enabled the removal of PFAS using PAMTAg and CAMTAg. Findings suggest that PAMTAg and CAMTAg are effective for the removal of PFAS from aqueous media and are good alternatives to commercially available activated carbons.Graphical abstractSupplementary informationThe online version contains supplementary material available at 10.1007/s40201-020-00597-3.

Project description:The deployment of aqueous film forming foams (AFFF) used for firefighting during emergencies and training often releases per- and polyfluoroalkyl substances (PFAS) into the environment. In October 2018, first responders in Providence, RI, USA applied an AFFF during a fuel spill. Due to the proximity of the incident to the upper reaches of Narragansett Bay (NB), an unknown quantity of gasoline and AFFF entered the estuary via surface runoff and stormwater drains. Water samples near the spill were collected approximately 15 h after the incident and analyzed for 24 PFAS. Minor increases in measured PFAS concentrations were observed relative to pre- and post-spill samples at monitoring sites near the incident, except 6:2-fluorotelomer sulfonate (6:2-FTS) that peaked post-spill (max 311 ng/L). After performing the total oxidizable precursor (TOP) assay on water samples and the AFFF concentrate, significant increases in perfluorocarboxylic acids (PFCAs) were observed. One compound, 6:2 fluorotelomer mercaptoalkylamido sulfonate (6:2-FTSAS), was identified as a major component of the AFFF used. Peak areas of 6:2-FTSAS and the degradation product 6:2-FTSAS-sulfoxide corresponded to observed increases in the TOP assay results and were useful as tracers of AFFF in surrounding waters. Elevated levels of PFAS at the time of sampling were limited to a confined area of the Providence River due to river flow and tidal action. Observed concentrations were also compared to hydrodynamic model results, and results confirmed rapid dissipation of AFFF components with distance from the spill. However, modeled results did not capture possible secondary releases of AFFF from local municipal stormwater and sewer infrastructure, as observational data suggest. The multiple lines of evidence of PFAS present in surface waters permitted a better assessment of the potential environmental impacts from products such as AFFF for which the chemical composition is largely unknown.

Dataset Information

Identifying and Managing Aqueous Film-Forming Foam-Derived Per- and Polyfluoroalkyl Substances in the Environment.

Publications

Identifying and Managing Aqueous Film-Forming Foam-Derived Per- and Polyfluoroalkyl Substances in the Environment.

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