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James L. Gray

Publications and source records attributed to James L. Gray.

At least 19 recordsLinked to original sources

Tapwater contaminant mixtures and cumulative risk screening on the Crow (Apsáalooke) Reservation

Introduction: Water insecurity is a challenge for the Apsáalooke (Crow) Tribal Nation in south-central Montana, United States. Both private-well and public-supply tapwater (TW) are vulnerable to a range of contaminants, posing potential risks to community health and well-being. Ongoing community concerns about unrecognized inorganic, organic, and microbial contaminants underscore the need for continued comprehensive monitoring and improved water management strategies. Materials and methods: TW samples were collected from 26 private-well and 12 public-supply participant locations, selected and recruited by the Crow Water Quality Project. A total of 35 inorganic, 450 organic, and three microbial analytes were assessed in these samples. Public-Supply Maximum Contaminant Levels and Health benchmark-based screening levels were used to evaluate contaminant concentrations. Results: Sixty-one organic and 34 inorganic contaminants were detected. Screening levels were frequently exceeded, particularly due to multiple inorganic contaminants in private TW and both chlorine-based disinfection byproducts (DBPs) and inorganics in public TW. These findings highlight gaps in current source-water protection and water treatment practices. Conclusions: After reporting results to participants, anonymized data were shared at community events to inform risk management decisions. The study underscores the importance of broad monitoring and analysis throughout the upper Missouri River basin and across the United States to address Tribal concerns over water insecurity and mitigate potential unrecognized TW contaminant risks, particularly to vulnerable subpopulations.

Montana↗

Assessing pesticide application contributions of per- and polyfluoroalkyl substances (PFAS) in agricultural streams

Research has documented per-and polyfluoroalkyl substances (PFAS) to be prevalent in streams impacted by urban sources; less is known regarding PFAS contributions via pesticide applications: PFAS coming from pesticide containers and “inert” ingredients not listed on pesticide formulation labels. To better understand co-occurrence of pesticides and PFAS in agricultural streams, 10 streams were sampled in two agricultural valleys in northern California, USA during two periods of pesticide application (May and July of 2024). Water samples were analyzed for 183 pesticides and 57 PFAS. Sixty pesticides were detected: 23 herbicides, 18 insecticides, 18 fungicides, and 1 synergist. Overall detection frequencies (DF) ranged from 0 to 100%, and concentrations ranged from non-detect (ND) to 782 ng/L (fluxapyroxad). Fourteen PFAS were detected: 6 perfluoroalkyl carboxylates, 5 perfluoroalkyl sulfonates, 2 perfluoroalkyl acid precursors, and 1 perfluoroalkyl phosphinic acid with DFs ranging from 0 to 60% (PFOA) and concentrations ranging from ND to 20 ng/L (PFBA). Co-occurrence of PFAS and pesticides was observed in 80% of samples. Adopting the global definition of PFAS (includes fluorinated pesticides), pesticide applications are a likely source of instream PFAS. Examination of total organic fluorine and transformations to terminal and ultra-short PFAS could further elucidate pesticide contributions to environmental PFAS.

California↗

Per- and polyfluoroalkyl substances (PFAS) and other contaminants of concern in tribal waters of Montana

We assessed potential exposures to a broad suite of contaminants (inorganic, organic and microbial) in culturally important surface waters from three watersheds in a northern plains Native American community (Apsáalooke [Crow Tribe of Montana]) in south-central Montana, United States, with water insecurity concerns. Inorganic (37), organic (435) and microbial (3) constituents were assessed in 12 surface water sites from the Pryor Creek ( n = 2), Bighorn River ( n = 2) and Little Bighorn River ( n = 8) valleys. Twenty-six organics, 33 inorganics and Escherichia coli were detected. Despite relatively low concentrations in surface waters within the Crow Reservation, mixture toxicity indicated prevalent chronic ecological effects and human-health secondary contact (recreation) effects at multiple sites. Further, to address Tribal concerns over the prevalence and corresponding risks of per- and polyfluoroalkyl substances (PFAS), we sampled water, sediment, biofilms and fish at a limited number of locations in the Little Bighorn River. Results indicated that PFAS were prevalent in fish tissues, including whole blood and filets, and to a lesser extent in biofilms, despite few detections in water and sediment samples. This is the first attempt to document environmental PFAS contamination within the reservation and the potential human-health concerns for the general population from consumption of recreational/subsistence fish. Overall, this effort provided preliminary information on the contaminant mixtures present and their potential health implications, which can support the protection of community health and culturally meaningful resources across the Crow Reservation.

Montana↗

Bioaccumulation and transfer of per- and polyfluoroalkyl substances (PFAS) in a stream and riparian food web contaminated by food processing wastewater

We evaluated the bioaccumulation and transfer of per- and polyfluoroalkyl substances (PFAS) in a stream food web contaminated by a food processing facility. Abiotic (i.e., water, sediment, and foam) and biotic (i.e., algae, aquatic insect larvae and adults, fish, and riparian spiders) matrices were sampled upstream and downstream of the facility’s wastewater outfall. Compared with upstream, PFAS concentrations were 600-fold higher in downstream water (mean ∑ 40 PFAS 3.67 ng mL –1 ± 0.48 (standard error)) and reflected inputs from the outfall, with 6:2 fluorotelomer sulfonate (6:2 FTS) dominating the PFAS profile. Within the aquatic food web, perfluorooctanesulfonate (PFOS) was the most biomagnified, and 6:2 FTS was the most biodiluted. In contrast, insect-mediated transfer of PFAS to riparian spiders showed trophic enrichment of 6:2 FTS and dilution of PFOS. We observed significant positive associations between phospholipid membrane-water partition coefficient (log K MW ) and perfluoroalkyl carboxylate (PFCA) chain length on bioaccumulation across most biological matrices, demonstrating that these chemical parameters are predictive of PFAS bioaccumulation potential in the field. Our research reveals important differences in aquatic versus terrestrial exposure for certain PFAS and that biological processes (e.g., trophic interactions and metamorphosis) and chemical properties (e.g., chain length, log K MW , and concentration) control PFAS uptake, bioaccumulation, and transfer in linked freshwater and terrestrial ecosystems.

Environmental Science & Technology↗

Revealing organofluorine contamination in effluents and surface waters with complementary analytical approaches: Fluorine-19 nuclear magnetic resonance spectroscopy (19F-NMR) and liquid chromatography-tandem mass spectrometry (LC-MS/MS)

Fluorinated organic contaminants, including per- and polyfluoroalkyl substances (PFASs) and fluorinated pesticides and pharmaceuticals (FPPs), pose a persistent threat to environmental health. Widely used liquid chromatography-tandem mass spectrometry (LC-MS/MS) methods fail to capture large fractions of total organofluorine in environmental samples, confounding the assessment of fluorinated contamination. Fluorine-19 nuclear magnetic resonance spectroscopy ( 19 F-NMR) is an inclusive method for total and class-based organofluorine analysis. Here, we apply 19 F-NMR to 31 effluent, surface water, and foam samples collected at 13 potential organofluorine point sources or source regions and compare the results to targeted LC-MS/MS for 34 or 64 PFASs. LC-MS/MS detected a median of 11.4% of total organofluorine detected by 19 F-NMR (range: nondetect to 8190 nM F 19 F-NMR; nondetect to 8010 nM F LC-MS/MS). The highest 19 F-NMR total organofluorine concentrations, detected in wastewater treatment plant (WWTP)-associated foam and at a soy oil production facility, arose from resonances characteristic of per- and polyfluorinated alkyl chains. 19 F-NMR resonances from aryl CF 3 moieties were abundant in the WWTP-associated samples, consistent with prior reports of substantial contributions from pharmaceuticals to WWTP effluents. 19 F-NMR enables the quantitative assessment of total organofluorine and qualitative insight into fluorinated structures, providing complementary analysis of organofluorine compounds missed by targeted mass spectrometry-based protocols.

Environmental Science & Technology↗

Determination of per- and polyfluoroalkyl substances in water by direct injection of matrix-modified centrifuge supernatant and liquid chromatography/tandem mass spectrometry with isotope dilution

A direct-injection liquid chromatography/tandem mass spectrometry method was developed to determine 34 per- and polyfluoroalkyl substances (PFAS), including selected branched isomers, in centrifuge supernatant of matrix-modified (amended with approximately 50 percent methanol) water samples. The method has been validated in reagent water, surface water, groundwater, and wastewater effluent. Other water types (for example, drinking water, untreated wastewater, and landfill leachate) have been analyzed by the method but not systematically validated. Recovery of isotope-dilution standards, added to each sample, may be used to assess method performance in nonvalidated matrices on a sample-by-sample basis. Using this method, PFAS concentrations were determined in the range of 2–2,000 nanograms per liter in water samples. This range can be extended by diluting concentrated samples. At circumneutral pH, most compounds are present in the environment in their ionized form, and data are reported as such (for example, perfluorooctanoic acid is referred to as “perfluorooctanoate” [PFOA], perfluorooctane sulfonic acid is referred to as “perfluorooctane sulfonate” [PFOS]). Sample preparation procedures were designed without the use of filtration and with minimum sample handling steps to mitigate procedural losses of target compounds due to sorption to surfaces. Further, isotope-dilution quantification allowed for the correction of bias that may result from procedural losses, matrix-induced signal suppression or enhancement, and other factors. Validation experiments to characterize bias and variability, method detection level, and holding time were done in four distinct water matrices—reagent water, surface water, treated wastewater effluent, and groundwater—at multiple concentration levels. Mean PFAS recoveries met data quality objectives of bias and variability studies in all four validation matrices except for two compounds with low and variable recovery in the reagent water matrix only. Isotope-dilution standards, treated as surrogate compounds, were analyzed in more than 1,500 customer-submitted environmental samples with aggregate recovery of 102.5±6.5 percent (mean±standard deviation). Maximum holding times for all target compounds in the four validation matrices were 28 days for refrigerated samples and 90 days for frozen samples.

Techniques and Methods↗

Assessing microplastics, per- and polyfluoroalkyl substances (PFAS), and other contaminants of global concern in wadable agricultural streams

Microplastics, per- and polyfluoroalkyl substances (PFAS), antibiotic resistance genes (ARGs), pharmaceuticals and personal care products (PPCPs), and pesticides may lead to unintended environmental contamination through many pathways in multiple matrices. This statewide, multi-matrix study of contaminants of global concern (CGCs) in agricultural streams across Iowa (United States) is the first to examine multiple CGCs in water, bed sediment, and fish to understand their occurrence in small streams located in regions of intense agriculture activity. Iowa plays a pivotal role in agriculture, with more than 85% of Iowa’s landscape devoted to agriculture making it an ideal location for determining the prevalence of CGCs to provide critical baseline exposure data. Fifteen sites were sampled across a range of predominant land uses (e.g., poultry, swine); all sites had detections of microplastics in all matrices. Concentrations of PFAS varied but were detected in water and sediment; all fish had detections of perfluorooctanesulfonate (PFOS), a type of PFAS. More than 50% of water and bed sediment samples had detections of ARGs. The most frequently detected PPCP was metformin. No sites had a cumulative exposure activity ratio greater than 1.0 for chemical exposures; 13 sites were above the 0.001 precautionary threshold. Toxicity quotients calculated using Aquatic Life Benchmarks were below the 0.1 moderate risk threshold for chemical exposures for all but one site. For fish, all sites exceeded the moderate and high-risk thresholds proposed for microplastic particles for food dilution (both chronic and acute exposures) and all sites exceeded the microplastic moderate threshold proposed for chronic tissue translocation, and two sites exceeded the threshold for acute tissue translocation.

Iowa↗

Per- and polyfluoroalkyl substances (PFAS) in drinking water in Southeast Los Angeles: Industrial legacy and environmental justice

Per - and polyfluoroalkyl substances (PFAS) are persistent chemicals of increasing concern to human health. PFAS contamination in water systems has been linked to a variety of sources including hydrocarbon fire suppression activities, industrial and military land uses, agricultural applications of biosolids, and consumer products. To assess PFAS in California tap water, we collected 60 water samples from inside homes in four different geographic regions, both urban and rural. We selected mostly small water systems with known history of industrial chemical or pesticide contamination and that served socioeconomically disadvantaged communities. Thirty percent of the tap water samples (18) had a detection of at least one of the 32 targeted PFAS and most detections (89 %) occurred in heavily industrialized Southeast Los Angeles (SELA). The residents of SELA are predominately Latino and low-income. Concentrations of perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) ranged from 6.8 to 13.6 ng/L and 9.4–17.8 ng/L, respectively in SELA and were higher than State (PFOA: 0.007 ng/L; PFOS: 1.0 ng/L) and national health-based goals (zero). To look for geographic patterns, we mapped potential sources of PFAS contamination, such as chrome plating facilities, airports, landfills, and refineries, located near the SELA water systems; consistent with the multiple potential sources in the area, no clear spatial associations were observed. The results indicate the importance of systematic testing of PFAS in tap water, continued development of PFAS regulatory standards and advisories for a greater number of compounds, improved drinking-water treatments to mitigate potential health threats to communities, especially in socioeconomically disadvantaged and industrialized areas.

California↗

Mixed contaminant exposure in tapwater and the potential implications for human-health in disadvantaged communities in California

Water is an increasingly precious resource in California as years of drought, climate change, pollution, as well as an expanding population have all stressed the state's drinking water supplies. Currently, there are increasing concerns about whether regulated and unregulated contaminants in drinking water are linked to a variety of human-health outcomes particularly in socially disadvantaged communities with a history of health risks. To begin to address this data gap by broadly assessing contaminant mixture exposures, the current study was designed to collect tapwater samples from communities in Gold Country, the San Francisco Bay Area, two regions of the Central Valley (Merced/Fresno and Kern counties), and southeast Los Angeles for 251 organic chemicals and 32 inorganic constituents. Sampling prioritized low-income areas with suspected water quality challenges and elevated breast cancer rates. Results indicated that mixtures of regulated and unregulated contaminants were observed frequently in tapwater throughout the areas studied and the types and concentrations of detected contaminants varied by region, drinking-water source, and size of the public water system. Multiple exceedances of enforceable maximum contaminant level(s) (MCL), non-enforceable MCL goal(s) (MCLG), and other health advisories combined with frequent exceedances of benchmark-based hazard indices were also observed in samples collected in all five of the study regions. Given the current focus on improving water quality in socially disadvantaged communities, our study highlights the importance of assessing mixed-contaminant exposures in drinking water at the point of consumption to adequately address human-health concerns (e.g., breast cancer risk). Data from this pilot study provide a foundation for future studies across a greater number of communities in California to assess potential linkages between breast cancer rates and tapwater contaminants.

Callifornia↗

Contaminant exposure and transport from three potential reuse waters within a single watershed

Global demand for safe and sustainable water supplies necessitates a better understanding of contaminant exposures in potential reuse waters. In this study, we compared exposures and load contributions to surface water from the discharge of three reuse waters (wastewater effluent, urban stormwater, and agricultural runoff). Results document substantial and varying organic-chemical contribution to surface water from effluent discharges (e.g., disinfection byproducts [DBP], prescription pharmaceuticals, industrial/household chemicals), urban stormwater (e.g., polycyclic aromatic hydrocarbons, pesticides, nonprescription pharmaceuticals), and agricultural runoff (e.g., pesticides). Excluding DBPs, episodic storm-event organic concentrations and loads from urban stormwater were comparable to and often exceeded those of daily wastewater-effluent discharges. We also assessed if wastewater-effluent irrigation to corn resulted in measurable effects on organic-chemical concentrations in rain-induced agricultural runoff and harvested feedstock. Overall, the target-organic load of 491 g from wastewater-effluent irrigation to the study corn field during the 2019 growing season did not produce substantial dissolved organic-contaminant contributions in subsequent rain-induced runoff events. Out of the 140 detected organics in source wastewater-effluent irrigation, only imidacloprid and estrone had concentrations that resulted in observable differences between rain-induced agricultural runoff from the effluent-irrigated and nonirrigated corn fields. Analyses of pharmaceuticals and per-/polyfluoroalkyl substances in at-harvest corn-plant samples detected two prescription antibiotics, norfloxacin and ciprofloxacin, at concentrations of 36 and 70 ng/g, respectively, in effluent-irrigated corn-plant samples; no contaminants were detected in noneffluent irrigated corn-plant samples.

Oklahoma↗

Bottled water contaminant exposures and potential human effects

Bottled water (BW) consumption in the United States and globally has increased amidst heightened concern about environmental contaminant exposures and health risks in drinking water supplies, despite a paucity of directly comparable, environmentally-relevant contaminant exposure data for BW. This study provides insight into exposures and cumulative risks to human health from inorganic/organic/microbial contaminants in BW. Methods BW from 30 total domestic US (23) and imported (7) sources, including purified tapwater (7) and spring water (23), were analyzed for 3 field parameters, 53 inorganics, 465 organics, 14 microbial metrics, and in vitro estrogen receptor (ER) bioactivity. Health-benchmark-weighted cumulative hazard indices and ratios of organic-contaminant in vitro exposure-activity cutoffs were assessed for detected regulated and unregulated inorganic and organic contaminants. Results 48 inorganics and 45 organics were detected in sampled BW. No enforceable chemical quality standards were exceeded, but several inorganic and organic contaminants with maximum contaminant level goal(s) (MCLG) of zero (no known safe level of exposure to vulnerable sub-populations) were detected. Among these, arsenic, lead, and uranium were detected in 67 %, 17 %, and 57 % of BW, respectively, almost exclusively in spring-sourced samples not treated by advanced filtration. Organic MCLG exceedances included frequent detections of disinfection byproducts (DBP) in tapwater-sourced BW and sporadic detections of DBP and volatile organic chemicals in BW sourced from tapwater and springs. Precautionary health-based screening levels were exceeded frequently and attributed primarily to DBP in tapwater-sourced BW and co-occurring inorganic and organic contaminants in spring-sourced BW. Conclusion The results indicate that simultaneous exposures to multiple drinking-water contaminants of potential human-health concern are common in BW. Improved understandings of human exposures based on more environmentally realistic and directly comparable point-of-use exposure characterizations, like this BW study, are essential to public health because drinking water is a biological necessity and, consequently, a high-vulnerability vector for human contaminant exposures.

Environment International↗

Per- and polyfluoroalkyl substances (PFAS) in United States tapwater: Comparison of underserved private-well and public-supply exposures and associated health implications

Drinking-water quality is a rising concern in the United States (US), emphasizing the need to broadly assess exposures and potential health effects at the point-of-use. Drinking-water exposures to per- and poly-fluoroalkyl substances (PFAS) are a national concern, however, there is limited information on PFAS in residential tapwater at the point-of-use, especially from private-wells. We conducted a national reconnaissance to compare human PFAS exposures in unregulated private-well and regulated public-supply tapwater. Tapwater from 716 locations (269 private-wells; 447 public supply) across the US was collected during 2016–2021 including three locations where temporal sampling was conducted. Concentrations of PFAS were assessed by three laboratories and compared with land-use and potential-source metrics to explore drivers of contamination. The number of individual PFAS observed ranged from 1 to 9 (median: 2) with corresponding cumulative concentrations (sum of detected PFAS) ranging from 0.348 to 346 ng/L. Seventeen PFAS were observed at least once with PFBS, PFHxS and PFOA observed most frequently in approximately 15% of the samples. Across the US, PFAS profiles and estimated median cumulative concentrations were similar among private wells and public-supply tapwater. We estimate that at least one PFAS could be detected in about 45% of US drinking-water samples. These detection probabilities varied spatially with limited temporal variation in concentrations/numbers of PFAS detected. Benchmark screening approaches indicated potential human exposure risk was dominated by PFOA and PFOS, when detected. Potential source and land-use information was related to cumulative PFAS concentrations, and the number of PFAS detected; however, corresponding relations with specific PFAS were limited likely due to low detection frequencies and higher detection limits. Information generated supports the need for further assessments of cumulative health risks of PFAS as a class and in combination with other co-occurring contaminants, particularly in unmonitored private-wells where information is limited or not available.

U.S. Virgin Islands↗

Juxtaposition of intensive agriculture, vulnerable aquifers, and mixed chemical/microbial exposures in private-well tapwater in northeast Iowa

In the United States and globally, contaminant exposure in unregulated private-well point-of-use tapwater (TW) is a recognized public-health data gap and an obstacle to both risk-management and homeowner decision making. To help address the lack of data on broad contaminant exposures in private-well TW from hydrologically-vulnerable (alluvial, karst) aquifers in agriculturally-intensive landscapes, samples were collected in 2018–2019 from 47 northeast Iowa farms and analyzed for 35 inorganics, 437 unique organics, 5 in vitro bioassays, and 11 microbial assays. Twenty-six inorganics and 51 organics, dominated by pesticides and related transformation products (35 herbicide-, 5 insecticide-, and 2 fungicide-related), were observed in TW. Heterotrophic bacteria detections were near ubiquitous (94 % of the samples), with detection of total coliform bacteria in 28 % of the samples and growth on at least one putative-pathogen selective media across all TW samples. Health-based hazard index screening levels were exceeded frequently in private-well TW and attributed primarily to inorganics (nitrate, uranium). Results support incorporation of residential treatment systems to protect against contaminant exposure and the need for increased monitoring of rural private-well homes. Continued assessment of unmonitored and unregulated private-supply TW is needed to model contaminant exposures and human-health risks.

Iowa↗

Exposures and potential health implications of contaminant mixtures in linked source water, finished drinking water, and tapwater from public-supply drinking water systems in Minneapolis/St. Paul area, USA

Continued improvements in drinking-water quality characterization and treatment/distribution infrastructure are required to address the expanding number of documented environmental contaminants. To better understand the variability in contaminant exposures from the drinking water resource (surface and groundwater), through the distribution process, to the point-of-use (tapwater), in 2019 a synoptic assessment of broad chemical exposures was conducted in system-specific source waters, finished drinking water and service-area tapwater from 10 drinking water treatment facilities in the greater Minneapolis/St. Paul area of Minnesota, United States. Source water, finished water (collected pre-distribution in the treatment facility), and tapwater samples were analyzed for 465 unique organic compounds, 34 inorganic constituents, and 3 field parameters as well as in vitro estrogen, androgen, and glucocorticoid bioactivities. Mixtures of organic and inorganic contaminants were prevalent in source water, finished water, and tapwater samples, indicating the continued need for broad assessments of mixed contaminant exposures to characterize potential drinking-water human health outcomes. Contaminant concentrations were similar among drinking water sources and no exceedances of Environmental Protection Agency maximum contaminant level(s) (MCL) were observed in any treated sample (finished water or tapwater) in this study. No treated sample contained estrogenic, androgenic, or glucocorticoid activity at concentrations that may cause adverse human health effects. However, there were multiple exceedances of non-enforceable MCL goal(s) (MCLG), and other health advisories combined with frequent exceedances of benchmark-based hazard indices in both finished water and tapwater samples. These results indicate that exposure to contaminant mixtures is a potential public health concern underscoring our continued efforts to assess contaminant mixture exposures at the drinking-water point of consumption using a broad analytical scope.

Minnesota↗

Tapwater exposures, effects potential, and residential risk management in Northern Plains Nations

In the United States (US), private-supply tapwater (TW) is rarely monitored. This data gap undermines individual/community risk-management decision-making, leading to an increased probability of unrecognized contaminant exposures in rural and remote locations that rely on private wells. We assessed point-of-use (POU) TW in three northern plains Tribal Nations, where ongoing TW arsenic (As) interventions include expansion of small community water systems and POU adsorptive-media treatment for Strong Heart Water Study participants. Samples from 34 private-well and 22 public-supply sites were analyzed for 476 organics, 34 inorganics, and 3 in vitro bioactivities. 63 organics and 30 inorganics were detected. Arsenic, uranium (U), and lead (Pb) were detected in 54%, 43%, and 20% of samples, respectively. Concentrations equivalent to public-supply maximum contaminant level(s) (MCL) were exceeded only in untreated private-well samples (As 47%, U 3%). Precautionary health-based screening levels were exceeded frequently, due to inorganics in private supplies and chlorine-based disinfection byproducts in public supplies. The results indicate that simultaneous exposures to co-occurring TW contaminants are common, warranting consideration of expanded source, point-of-entry, or POU treatment(s). This study illustrates the importance of increased monitoring of private-well TW, employing a broad, environmentally informative analytical scope, to reduce the risks of unrecognized contaminant exposures.

North Dakota, South Dakota↗

Food, beverage, and feedstock processing facility wastewater: A unique and underappreciated source of contaminants to U.S. streams

Process wastewaters from food, beverage, and feedstock facilities, although regulated, are an under-investigated environmental contaminant source. Food process wastewaters (FPWWs) from 23 facilities in 17 U.S. states were sampled and documented for a plethora of chemical and microbial contaminants. Of the 576 analyzed organics, 184 (32%) were detected at least once, with concentrations as large as 143 μg L –1 (6:2 fluorotelomer sulfonic acid), and as many as 47 were detected in a single FPWW sample. Cumulative per/polyfluoroalkyl substance concentrations up to 185 μg L –1 and large pesticide transformation product concentrations (e.g., methomyl oxime, 40 μg L –1 ; clothianidin TMG, 2.02 μg L –1 ) were observed. Despite 48% of FPWW undergoing disinfection treatment prior to discharge, bacteria resistant to third-generation antibiotics were found in each facility type, and multiple bacterial groups were detected in all samples, including total coliforms. The exposure–activity ratios and toxicity quotients exceeded 1.0 in 13 and 22% of samples, respectively, indicating potential biological effects and toxicity to vertebrates and invertebrates associated with the discharge of FPWW. Organic contaminant profiles of FPWW differed from previously reported contaminant profiles of municipal effluents and urban storm water, indicating that FPWW is another important source of chemical and microbial contaminant mixtures discharged into receiving surface waters.

Alabama, Arkansas, California, Idaho, Illinois, Io↗

A comprehensive statewide spatiotemporal stream assessment of per- and polyfluoroalkyl substances (PFAS) in an agricultural region of the United States

Public concern regarding per- and polyfluoroalkyl substances (PFAS) has grown substantially in recent years. In addition, research has documented multiple potential agriculture-related release pathways for PFAS (e.g., biosolids and livestock manure). Nevertheless, little research on the environmental prevalence of PFAS has been conducted in agricultural regions of the United States. To fill this gap, we conducted the first statewide spatiotemporal assessment of PFAS in Iowa streams across a region of intense agricultural activity. At least one PFAS was detected at 19 of the 60 stream sites sampled (32%) with 10 different PFAS detected statewide. The number of PFAS detected in the stream samples ranged from one to nine. While PFAS were detected in agricultural streams, sites with the most PFAS detected and in the highest concentration were small, effluent-affected streams where wastewater treatment plant discharge is driving stream PFAS concentrations. No individual PFAS had an exposure:activity ratio (EAR) of >1.0 (exposure concentration shown to trigger observed adverse biological activity). Five stream locations, however, had at least one EAR of >0.001, a precautionary effect screening threshold. Additional targeted temporal sampling would be beneficial to specifically capture potential agricultural source applications and corresponding runoff conditions to fully characterize the prevalence of PFAS in such agricultural systems.

Iowa↗

Public and private tapwater: Comparative analysis of contaminant exposure and potential risk, Cape Cod, Massachusetts, USA

Background Humans are primary drivers of environmental contamination worldwide, including in drinking-water resources. In the United States (US), federal and state agencies regulate and monitor public-supply drinking water while private-supply monitoring is rare; the current lack of directly comparable information on contaminant-mixture exposures and risks between private- and public-supplies undermines tapwater (TW) consumer decision-making. Methods We compared private- and public-supply residential point-of-use TW at Cape Cod, Massachusetts, where both supplies share the same groundwater source. TW from 10 private- and 10 public-supply homes was analyzed for 487 organic, 38 inorganic, 8 microbial indicators, and 3 in vitro bioactivities. Concentrations were compared to existing protective health-based benchmarks, and aggregated Hazard Indices (HI) of regulated and unregulated TW contaminants were calculated along with ratios of in vitro exposure-activity cutoffs. Results Seventy organic and 28 inorganic constituents were detected in TW. Median detections were comparable, but median cumulative concentrations were substantially higher in public supply due to 6 chlorine–disinfected samples characterized by disinfection byproducts and corresponding lower heterotrophic plate counts. Public-supply applicable maximum contaminant (nitrate) and treatment action (lead and copper) levels were exceeded in private-supply TW samples only. Exceedances of health-based HI screening levels of concern were common to both TW supplies. Discussion These Cape Cod results indicate comparable cumulative human-health concerns from contaminant exposures in private- and public-supply TW in a shared source-water setting. Importantly, although this study’s analytical coverage exceeds that currently feasible for water purveyors or homeowners, it nevertheless is a substantial underestimation of the full breadth of contaminant mixtures documented in the environment and potentially present in drinking water. Conclusion Regardless of the supply, increased public engagement in source-water protection and drinking-water treatment, including consumer point-of-use treatment, is warranted to reduce risks associated with long-term TW contaminant exposures, especially in vulnerable populations.

Massachusetts↗