The effect of drinking water contaminated with perfluoroalkyl substances on a 10-year longitudinal trend of plasma levels in an elderly Uppsala cohort.

BACKGROUND: In 2012, drinking water contaminated with per- and polyfluoroalkyl substances (PFASs), foremost perfluorooctanesulfonic acid (PFOS) and perfluorohexanesulfonic acid (PFHxS) at levels over 20ng/L and 40ng/L, respectively, was confirmed in Uppsala, Sweden. OBJECTIVES: We assessed how a longitudinally sampled cohort's temporal trend in PFAS plasma concentration was influenced by their residential location and determined the plausible association or disparity between the PFASs detected in the drinking water and the trend in the study cohort. METHODS: The Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) cohort provided plasma samples three times from 2001 to 2014. Individuals maintaining the same zip code throughout the study (n = 399) were divided into a reference (no known PFAS exposure), low, intermediate and high exposure area depending on the proportion of contaminated drinking water received. Eight PFASs detected in the majority (75%) of the cohort's plasma samples were evaluated for significant changes in temporal PFAS concentrations using a random effects (mixed) model. RESULTS: PFHxS plasma concentrations continued to significantly increase in individuals living in areas receiving the largest percentage of contaminated drinking water (p < 0.0001), while PFOS showed an overall decrease. The temporal trend of other PFAS plasma concentrations did not show an association to the quality of drinking water received. CONCLUSIONS: The distribution of contaminated drinking water had a direct effect on the trend in PFHxS plasma levels among the different exposure groups, resulting in increased concentrations over time, especially in the intermediate and high exposure areas. PFOS and the remaining PFASs did not show the same relationship, suggesting other sources of exposure influenced these PFAS plasma trends.

Influence of contaminated drinking water on perfluoroalkyl acid levels in human serum--A case study from Uppsala, Sweden.

In 2012 a contamination of drinking water with perfluoroalkyl acids (PFAAs) was uncovered in the City of Uppsala, Sweden. The aim of the present study was to determine how these substances have been distributed from the contamination source through the groundwater to the drinking water and how the drinking water exposure has influenced the levels of PFAAs in humans over time. The results show that PFAA levels in groundwater measured 2012-2014 decreased downstream from the point source, although high ΣPFAA levels (>100ng/L) were still found several kilometers from the point source in the Uppsala aquifer. The usage of aqueous film forming fire-fighting foams (AFFF) at a military airport in the north of the city is probably an important contamination source. Computer simulation of the distribution of PFAA-contaminated drinking water throughout the City using a hydraulic model of the pipeline network suggested that consumers in the western and southern parts of Uppsala have received most of the contaminated drinking water. PFAA levels in blood serum from 297 young women from Uppsala County, Sweden, sampled during 1996-1999 and 2008-2011 were analyzed. Significantly higher concentrations of perfluorobutane sulfonic acid (PFBS) and perfluorohexane sulfonic acid (PFHxS) were found among women who lived in districts modeled to have received contaminated drinking water compared to unaffected districts both in 1996-1999 and 2008-2011, indicating that the contamination was already present in the late 1990s. Isomer-specific analysis of PFHxS in serum showed that women in districts with contaminated drinking water also had an increased percentage of branched isomers. Our results further indicate that exposure via contaminated drinking water was the driving factor behind the earlier reported increasing temporal trends of PFBS and PFHxS in blood serum from young women in Uppsala.

Drinking water nanofiltration with concentrate foam fractionation-A novel approach for removal of per- and polyfluoroalkyl substances (PFAS).

Per- and polyfluoroalkyl substances (PFAS) are recognized as persistent pollutants that have been found in drinking water sources on a global scale. Semi-permeable membrane treatment processes such as reverse osmosis and nanofiltration (NF) have been shown effective at removing PFAS, however, disposal of PFAS laden concentrate is problematic. Without treatment of the concentrate, PFAS is released into the environment. The present work examined a novel PFAS removal scheme for drinking water using NF filtration with treatment of the resulting NF concentrate via foam fractionation (FF) with and without co-surfactants. The NF-pilot removed 98% of PFAS from AFFF contaminated groundwater producing permeate with 1.4 ng L-1 total PFAS. Using FF resulted in ∑PFAS removal efficiency of 90% from the NF concentrate and with improved removal of 94% with addition of cationic co-surfactant. The resulting foamate composed approximately 2% of the NF feedwater volume and contained greater than 3000 ng L-1 PFAS or 41 times greater than the NF feedwater. Addition of the cationic co-surfactant to the FF process resulted in increased removal efficiency of the shorter chain PFAS, specifically 37% for PFPeA, 9% for PFHxA, and 34% for PFBS thus attaining 59%, 99% and 96% removal efficiency, respectively. PFOA, PFPeS, PFHxS, PFOS each attained 99% FF removal with or without co-surfactant addition.

Electrochemical Oxidation for Treatment of PFAS in Contaminated Water and Fractionated Foam-A Pilot-Scale Study.

Per- and polyfluoroalkyl substances (PFAS) are persistent synthetic contaminants that are present globally in water and are exceptionally difficult to remove during conventional water treatment processes. Here, we demonstrate a practical treatment train that combines foam fractionation to concentrate PFAS from groundwater and landfill leachate, followed by an electrochemical oxidation (EO) step to degrade the PFAS. The study combined an up-scaled experimental approach with thorough characterization strategies, including target analysis, PFAS sum parameters, and toxicity testing. Additionally, the EO kinetics were successfully reproduced by a newly developed coupled numerical model. The mean total PFAS degradation over the designed treatment train reached 50%, with long- and short-chain PFAS degrading up to 86 and 31%, respectively. The treatment resulted in a decrease in the toxic potency of the water, as assessed by transthyretin binding and bacterial bioluminescence bioassays. Moreover, the extractable organofluorine concentration of the water decreased by up to 44%. Together, these findings provide an improved understanding of a promising and practical approach for on-site remediation of PFAS-contaminated water.

Pilot-Scale Continuous Foam Fractionation for the Removal of Per- and Polyfluoroalkyl Substances (PFAS) from Landfill Leachate.

Per- and polyfluoroalkyl substances (PFAS) are of concern for their ubiquity in the environment combined with their persistent, bioaccumulative, and toxic properties. Landfill leachate is often contaminated with these chemicals, and therefore, the development of cost-efficient water treatment technologies is urgently needed. The present study investigated the applicability of a pilot-scale foam fractionation setup for the removal of PFAS from natural landfill leachate in a novel continuous operating mode. A benchmark batch test was also performed to compare treatment efficiency. The ΣPFAS removal efficiency plateaued around 60% and was shown to decrease for the investigated process variables air flow rate (Q air), collected foam fraction (%foam) and contact time in the column (t c). For individual long-chain PFAS, removal efficiencies above 90% were obtained, whereas the removal for certain short-chain PFAS was low (<30%). Differences in treatment efficiency between enriching mode versus stripping mode as well as between continuous versus batch mode were negligible. Taken together, these findings suggest that continuous foam fractionation is a highly applicable treatment technology for PFAS contaminated water. Coupling the proposed cost- and energy-efficient foam fractionation pretreatment to an energy-intensive degradative technology for the concentrated foam establishes a promising strategy for on-site PFAS remediation.

Long-distance transport of per- and polyfluoroalkyl substances (PFAS) in a Swedish drinking water aquifer.

Use of per- and polyfluoroalkyl substance (PFAS)-containing aqueous film-forming foams (AFFF) at firefighting training sites (FFTS) has been linked to PFAS contamination of drinking water. This study investigated PFAS transport and distribution in an urban groundwater aquifer used for drinking water production that has been affected by PFAS-containing AFFF. Soil, sediment, surface water and drinking water were sampled. In soil (n = 12) at a FFTS with high perfluorooctane sulfonate (PFOS) content (87% of ∑PFAS), the ∑PFAS concentration (n = 26) ranged from below detection limit to 560 ng g-1 dry weight. In groundwater (n = 28), the ∑PFAS concentration near a military airbase FFTS reached 1000 ng L-1. Principal component analysis (PCA) identified the military FFTS as the main source of PFAS contamination in drinking water wellfields >10 km down-gradient. Groundwater samples taken close to the military FFTS site showed no ∑PFAS concentration change between 2013 and 2021, while a location further down-gradient showed a transitory 99.6% decrease. Correlation analysis on PFAS composition profile indicated that this decrease was likely caused by dilution from an adjacent conflating aquifer. ∑PFAS concentration reached 15 ng L-1 (PFOS 47% and PFHxS 41% of ∑PFAS) in surface river water (n = 6) and ranged between 1 ng L-1 and 8 ng L-1 (PFHxS 73% and PFBS 17% of ∑PFAS) in drinking water (n = 4). Drinking water had lower PFAS concentrations than the wellfields due to PFAS removal at the water treatment plant. This demonstrates the importance of monitoring PFAS concentrations throughout a groundwater aquifer, to better understand variations in transport from contamination sources and resulting impacts on PFAS concentrations in drinking water extraction areas.

Artificial infiltration in drinking water production: Addressing chemical hazards using effect-based methods.

Artificial infiltration is an established managed aquifer recharge method that is commonly incorporated into drinking water processes. However, groundwater sourced from this type of purification method is prone to contamination with chemical hazards. Such an instance was previously shown at a Swedish DWTP where the river water was contaminated by hazardous chemicals during artificial infiltration. Further, there remains a paucity of research studying the quality of drinking water following this type of treatment from an effect-based bioanalytical perspective. In the current study, an effect-based assessment for chemical hazards was conducted for a Swedish drinking water system comprised of two DWTPs fed artificially-infiltrated river water. In this system, artificial infiltration of the river water takes approximately six to eight months. A sampling event was conducted in the autumn season and the samples were enriched by solid phase extraction. A panel of cell-based reporter gene assays representing several toxicity pathways was selected: oxidative stress response (Nrf2 activity), aryl hydrocarbon receptor (AhR) activation, and hormone receptor-mediated effects (estrogen receptor [ER], androgen receptor [AR]). AhR and ER bioactivities were detected in samples collected from the river intake and in the open-air infiltration basins prior to artificial infiltration. However, the AhR activity decreased and ER activity was effectively removed following artificial infiltration. In the Nrf2 and AR assays, no bioactivities above cut-off levels were detected in any samples collected along the entire treatment process of the drinking water production from source to tap. Using a suite of bioassays, the current study highlighted the effectiveness of artificial infiltration in reducing bioactive compounds in this raw river water. Although artificial infiltration is a common purification method in drinking water production, the limited number of effect-based studies evaluating the effectiveness of this method emphasizes the need for further research to better understand the risks and benefits of this water treatment process.

Removal of per- and polyfluoroalkyl substances (PFASs) in a full-scale drinking water treatment plant: Long-term performance of granular activated carbon (GAC) and influence of flow-rate.

Per- and polyfluoroalkyl substances (PFASs) have been ubiquitously detected in drinking water which poses a risk for human exposure. In this study, the treatment efficiency for the removal of 15 PFASs was examined in a full-scale drinking water treatment plant (DWTP) in the City of Uppsala, Sweden, over a period of two years (2015-2017). Removal of the five frequently detected PFASs was influenced by the total operation time of granular activated carbon (GAC) filters, GAC type and surface loading rate. The average removal efficiency of PFASs ranged from 92 to 100% for "young" GAC filters and decreased to 7.0-100% for "old" GAC filters (up to 357 operation days, 29 300 bed volumes (BV) treated). Flow-rates were adjusted in two full-scale GAC filters of different operational age to examine the removal of PFAS and organic matter depending on GAC operational age and operating flow. The decrease in flow-rate by 10 L s-1 from 39 to 29 L s-1 led to an average increase of 14% and 6.5% in total PFAS removal efficiency for an "old" (264 operation days, 21 971 BV treated) and a "young" GAC filter (63 operation days, 5 725 BV treated), respectively. A cost-analysis for various operation scenarios illustrated the dominating effect of treatment goals and costs for GAC regeneration on overall GAC operation costs. The unit costs for GAC filters ranged from 0.08 to 0.10 € m-3 water treated and 0.020-0.025 € m-3 water treated for a treatment goal of 10 ng L-1 and 85 ng L-1, respectively, for ∑11PFAS. Furthermore, it was concluded that prolonging the GAC service life by lowering the flow-rates after reaching the treatment goal could lead to a 26% cost-deduction. The results and methods presented in this study give drinking water providers valuable tools for the operation of a full-scale treatment train for the removal of PFAS in contaminated raw water.

Removal efficiency of multiple poly- and perfluoroalkyl substances (PFASs) in drinking water using granular activated carbon (GAC) and anion exchange (AE) column tests.

Poly- and perfluoroalkyl substances (PFASs) have been detected in drinking water at relatively high concentrations throughout the world which has led to implementation of regulatory guidelines for specific PFASs in drinking water in several European countries and in the U.S. The Swedish National Food Agency has determined that the drinking water of over one third of the country's municipal consumers is at risk or already affected by PFAS contamination. The present study investigated the effects of perfluorocarbon chain length, functional group and isomer structure (branched or linear) on removal of multiple PFASs using granular activated carbon (GAC, Filtrasorb® 400) and anion exchange (AE, Purolite® A600) column experiments. The removal of 14 different PFASs, i.e. the C3C11, C14 perfluoroalkyl carboxylic acids (PFCAs) (PFBA, PFPeA, PFHxA, PFHpA, PFOA, PFNA, PFDA, PFUnDA, PFDoDA, PFTeDA), perfluorooctane sulfonamide (FOSA), and the C4, C6, C8 perfluoroalkyl sulfonic acids (PFSAs) (PFBS, PFHxS, PFOS), was monitored for a 217 day period. The results indicate the selective nature of PFAS removal as the absorbents are loaded with PFASs and dissolved organic carbon (DOC). A clear relationship between perfluorocarbon chain length and removal efficiency of PFASs using GAC and AE was found while PFASs with sulfonate functional groups displayed greater removal efficiency than those with carboxylate groups. Similarly, time to column breakthrough increased with increasing perfluorocarbon chain length and was greater for the PFSAs than the PFCAs for both GAC and AE. Shorter carbon chained PFASs such as PFBA, PFPeA, PFHxA showed desorption behavior and long-chained PFASs showed increased removal towards the end of the experiment indicating agglomeration or micelle development. Linear isomers of PFOS, PFHxS, and perfluorooctane sulfonamide (FOSA) had greater column removal efficiencies using GAC (and also for AE at greater bed volume throughput) than the branched and this difference increased at greater bed volume throughputs. The GAC and AE columns showed a poor correlation between DOC and PFAS removal efficiency. The results indicate that designers and operators of AE and GAC treatment processes must take into consideration the selective nature of PFAS removal and associated desorption of short-chain PFCAs during co-removal of multiple PFASs.