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Paul M. Bradley

Publications and source records attributed to Paul M. Bradley.

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↗

Comparative screening of private, public, and bottled drinking water in vitro bioactivity

This study compares in vitro bioactivity profiles of extracts from private tapwater (51 samples), public tapwater (143 samples), and bottled water (31 samples), using high-throughput, multiplex, transcription factor screening. Of 48 biological end points tested, 25 showed significant (≥50% above the field blank) activity. Frequently detected (≥10% of samples) bioactivities (in decreasing order) included xenobiotic metabolism (pregnane X receptor [ PXR ], aryl hydrocarbon receptor [ AhR ]), antioxidant response (antioxidant response element-binding nuclear factor erythroid 2-related factor 2 [ NRF2 ], activator protein 1 [ AP-1 ]), endocrine signaling (estrogen receptor [ ER ], peroxisome proliferator-activated receptor [ PPAR ]), and metals response (metals response element [ MRE ]). Significant bioactivities were observed across all drinking water supplies, with some statistical differences identified. Bioactivities were moderately to strongly correlated with several individual exposure and corresponding benchmark- or activity-weighted metrics, particularly for disinfection byproducts. Significant (α = 0.05) but weak correlations between measured bioactivity resemblance patterns and those of the inorganic–organic exposure, toxicity-quotient (TQ), and exposure-activity-ratio (EAR) resemblance matrices suggest that key drivers of observed drinking water bioactivity were not captured by the extensive, targeted exposure assessment. Results highlight the need for effects-based monitoring combined with improved exposure analysis to better assess health risks from low-level contaminant mixtures in drinking water.

ES&T Water↗

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↗

Insights and strategic opportunities from the USGS 2024 Per- and Polyfluoroalkyl Substances (PFAS) Interagency Workshop

Introduction In 2021, the U.S. Geological Survey (USGS) published Circular 1490 titled, “Integrated Science for the Study of Perfluoroalkyl and Polyfluoroalkyl Substances (PFAS) in the Environment: A Strategic Science Vision for the U.S. Geological Survey” (Tokranov and others, 2021). Circular 1490 was created to be a resource for USGS scientists prioritizing and planning research related to per- and polyfluoroalkyl substances (PFAS) and to be a guide for developing partnerships with other scientists, State and Federal agencies, and stakeholders engaged in PFAS research and management and mitigation of the environmental and human-health effects of PFAS. This USGS PFAS Strategic Science Vision document was intended to be the foundation for a “living strategic vision,” periodically providing updates on the state of USGS PFAS research, emerging PFAS data gaps and needs, and progress on interagency and stakeholder PFAS partnerships and priorities. To meet this objective, the USGS planned to host an Interagency and Stakeholder PFAS Workshop every 2–3 years. During September 10–12, 2024, the USGS hosted the first Interagency and Stakeholder PFAS Workshop in Reston, Virginia. The Workshop brought together experts from other Federal agencies (U.S. Environmental Protection Agency, National Institute of Environmental Health Sciences, Food and Drug Administration, Department of Defense [Air Force, Army]), State agencies (Washington Fish and Wildlife, Virginia Department of Transportation), and academia (Harvard University, University of Maryland) to address key challenges relating to the measurement and modeling of PFAS and the implications for environmental health. Participants engaged in in-depth discussions centered around six pivotal topics related to PFAS: (1) sampling protocols, methods and interpretation; (2) environmental sources, source apportionment, and occurrence; (3) environmental fate and transport; (4) human and wildlife exposure routes and risk; (5) bioconcentration, bioaccumulation, and biomagnification; and (6) ecotoxicology and effects. Each topic had three breakout sessions. A recurrent theme of workshop discussions was how data on a nationwide scale for PFAS occurrence in various environmental matrices, including air, water, food crops, biota, soil, and streambed sediment could help to advance scientific understanding. Participants noted significant geospatial data gaps, particularly in the midwestern and southern United States and the Pacific Northwest. PFAS data collection tends to be more robust along the eastern seaboard and in California. Participants stressed how enhancing the integration of large and small datasets across various agencies could help to support national scale understanding of PFAS. To address these gaps, attendees suggested leveraging datasets from Federal entities like the USGS and the U.S. Department of Defense, State agencies, and municipal utility services to develop predictive contaminant detection and transport models. Improved coordination between water quality programs and USGS research could help to facilitate access to valuable data, leading to comprehensive databases that inform PFAS point (wastewater treatment plants and landfills) and nonpoint (runoff from land, atmospheric deposition, food packaging) sources, environmental transport mechanisms, environmental detection and concentrations, potential exposure routes, and health effects on different biota, including humans. A specific request was made to develop a map demarking the depth of modern (1953 or later) groundwater, which is susceptible to surface-derived anthropogenic (that is, human-made) contamination, based on tritium-age dating. Emphasis was placed on incorporation of hydrology, groundwater flow paths, groundwater–surface water interactions, and landscape factors in predictive statistical models as a step to improve contaminant source identification and tracking. Molecular fingerprinting approaches garnered attention as techniques to link specific PFAS mixtures detected in a sample to environmental sources and levels in biota (Dávila-Santiago and others, 2022). Integrating data from abiotic (that is, water, soil, and air) and biotic (that is, living organisms) systems identified as a research opportunity. For example, understanding the composition of soils and sediments, which include a mixture of mineral, plant, and animal components, could advance understanding of exposure pathways. The discussions highlighted opportunities to explore and understand the potential redistribution and biotic exposures of PFAS from biosolid and wastewater treatment plant effluent land application practices, in addition to atmospheric releases and discharges from landfill and wastewater treatment plants. Participants identified research gaps surrounding how these sources may contribute to contamination and may affect surrounding ecosystems, including a better definition of anthropogenic background concentrations. Moving forward, the collection of co-occurrence data was noted as a means to improve understanding of complex mixtures and to leverage companion modeling efforts focused on areas with high and low contamination levels to identify areas of concern and unaffected resources. Participants emphasized how centralized USGS databases and the establishment of sample-metadata archives can help to ensure that samples are preserved and accessible for future research. In conclusion, the workshop participants identified opportunities to bridge data gaps and improve measurement techniques, modeling frameworks, databases, and communication, to enhance the understanding of PFAS and their effects on environmental and human health. Upon completion of the workshop, participants indicated an interest in developing strategic data collection, modeling, and analytical approaches to address these challenges.

Open-File Report↗

Municipal and industrial wastewater treatment plant effluent contributions to per- and polyfluoroalkyl substances in the Potomac River: A basin-scale measuring and modeling approach

Managing per- and polyfluoroalkyl substances (PFAS) in water resources requires a basin-scale approach. Predicted environmental concentrations (PEC) and stream-vulnerability scores for PFAS were determined for the Potomac River watershed in the eastern United States. Approximately 15% of stream reaches contained municipal and/or industrial wastewater treatment plant (WWTP) discharges that are presumptive PFAS sources, comprising from <1 to >90% of streamflow. Mean annual PEC, based on the summed concentrations of eight PFAS detected in WWTP effluents (ΣPFAS PEC ), for all stream reaches in the watershed was 3.8 ng L –1 , and stream reaches impacted by WWTP had perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS) PEC of 0.39 and 0.14 ng L –1 . For locations where measured-environmental concentrations (MEC) were determined, municipal and industrial WWTP contributed 7.8% (0 to 65%) of the total annual streamflow and MEC were greater than PEC in 99% of the samples, indicating additional potential PFAS sources. The mean ΣPFAS PEC was 9.1 ng L –1 compared to a mean sum of PFAS MEC of 34 ng L –1 . Under mean-August low-flow, 17% and 9.4% of the water-supply intakes had maximum PFOA and PFOS PEC exceeding drinking water maximum contaminant levels.

Maryland, Pennsylvania, Virginia, West Virginia↗

Public, bottled, and private drinking water: Shared contaminant-mixture exposures and effects challenge

BACKGROUND: Humans are primary drivers of environmental contaminant exposures worldwide, including in drinking-water (DW). In the United States (US), point-of-use DW (POU DW) is supplied via private tapwater (TW, predominantly private wells), public-supply TW, and bottled water (BW). Differences in management, monitoring, and messaging and lack of directly intercomparable exposure data influence the actual and perceived quality and safety of different DW supplies and directly impact consumer decision making. OBJECTIVES: The purpose of this paper is to provide a meta-analysis (quantitative synthesis) of POU DW contaminant mixture exposures and corresponding potential human health effects of private-TW, public-TW, and BW by aggregating exposure results and harmonizing apical health benchmark weighted and bioactivity weighted effects predictions across previous studies by this research group. DISCUSSION: Simultaneous exposures to multiple inorganic and organic contaminants of known or suspected human-health concern are common across all three DW supplies, with substantial variability observed in each and no systematic difference in predicted cumulative risk between supply chains. Differences in contaminant or contaminant class exposures (e.g., trace metals, disinfection byproducts), with important implications for DW quality improvements, were observed and attributed to corresponding differences in regulation and compliance monitoring. CONCLUSION: The results indicate that human-health risks from contaminant exposures are common to and comparable in all three DW supplies, including BW. Importantly, this study’s target analytical coverage, which exceeds that currently feasible for water purveyors or homeowners, nevertheless is a substantial underestimation of the full breadth of contaminant mixtures in the environment and potentially present in DW. Thus, the results emphasize the need for improved understanding of the adverse human-health implications of long-term exposures to low level inorganic /organic contaminant mixtures across all three distribution pipelines and do not support commercial messaging of BW as a systematically safer alternative to public-TW. Regardless of the supply, increased engagement in source-water protection and drinking-water treatment, including consumer point of use treatment, is necessary to reduce risks associated with long-term DW contaminant exposures, especially in vulnerable populations, and to reduce environmental waste and plastics contamination.

Environment International↗

Statewide cumulative human health risk assessment of inorganics-contaminated groundwater wells, Montana, USA

Across the United States, rural residents rely on unregulated and generally unmonitored private wells for drinking water, which may pose serious health risks due to unrecognized contaminants. We assessed the nature, degree, and spatial distribution of cumulative health risks from inorganic contaminants in groundwater. Our analysis included nearly 84,000 data points from 6500+ wells, across 51 of Montana's 98 watersheds, using a public groundwater database. We compared a drinking water screening level cumulative risk assessment (CRA) for inorganics based on the U.S. Environmental Protection Agency (EPA) protective health thresholds (Maximum Contaminant Level Goals, Health Advisories [MCLG-HAs]) to a CRA based on EPA public supply enforceable Maximum Contaminant Levels (MCLs). Based on median concentrations of 19 inorganics (antimony, arsenic, barium, beryllium, boron, cadmium, chromium, copper, fluoride, manganese, molybdenum, nickel, nitrate, lead, selenium, strontium, thallium, uranium, zinc), 75% of watersheds had MCLG-HA-based cumulative risk values > 1.0; arsenic and uranium contributed the most risk, followed by strontium, fluoride, manganese and boron. Hence, this screening level (Tier I) CRA indicated widespread potential for unrecognized human health risk to private well users from inorganic contaminants considering both carcinogenic and non-carcinogenic risks. Sensitivity analysis showed that benchmarks applied (MCLG-HAs versus MCLs) exerted the largest control on results. Our findings identify priority regions for Tier 2 risk assessments to elucidate local sources and distributions of geogenic versus anthropomorphic contaminants. Our study is the first statewide assessment of cumulative health risk from groundwater that we are aware of, and results support increased statewide drinking water education and testing to reduce human health risks from contaminated private well water.

Montana↗

Tapwater exposures, residential risk, and mitigation in a PFAS-impacted-groundwater community

Tapwater (TW) safety and sustainability are priorities in the United States. Per/polyfluoroalkyl substance(s) (PFAS) contamination is a growing public-health concern due to prolific use, widespread TW exposures, and mounting human-health concerns. Historically-rural, actively-urbanizing communities that rely on surficial-aquifer private wells incur elevated risks of unrecognized TW exposures, including PFAS, due to limited private-well monitoring and contaminant-source proliferation in urbanizing landscapes. Here, a broad-analytical-scope TW-assessment was conducted in a hydrologically-vulnerable, Mississippi River alluvial-island community, where PFAS contamination of the shallow-alluvial drinking-water aquifer has been documented, but more comprehensive contaminant characterization to inform decision-making is currently lacking. In 2021, we analyzed 510 organics, 34 inorganics, and 3 microbial groups in 11 residential and community locations to assess (1) TW risks beyond recognized PFAS issues, (2) day-to-day and year-to-year risk variability, and (3) suitability of the underlying sandstone aquifer as an alternative source to mitigate TW-PFAS exposures. Seventy-six organics and 25 inorganics were detected. Potential human-health risks of detected TW exposures were explored based on cumulative benchmark-based toxicity quotients ( ∑ TQ ). Elevated risks ( ∑ TQ ≥ 1) from organic and inorganic contaminants were observed in all alluvial-aquifer-sourced synoptic samples but not in sandstone-aquifer-sourced samples. Repeated sampling at 3 sites over 52–55 h indicated limited variability in risk over the short-term. Comparable PFAS-specific ∑ TQ for spatial-synoptic, short-term (3 days) temporal, and long-term (3 years quarterly) temporal samples indicated that synoptic results provided useful insight into the risks of TW-PFAS exposures at French Island over the long-term. No PFAS detections in sandstone-aquifer-sourced samples over a 3 year period indicated no PFAS-associated risk and supported the sandstone aquifer as an alternative drinking-water source to mitigate community TW-PFAS exposures. This study illustrated the importance of expanded contaminant monitoring of private-well TW, beyond known concerns (in this case, PFAS), to reduce the risks of a range of unrecognized contaminant exposures.

Wisconsin↗

Tapwater-contaminant mixtures and risk in a biofuel-facility impacted private-well community

We assessed private-well drinking water (DW) at the point of use ( i.e. , tapwater, TW) within a rural Nebraska community around a state-closed biofuel facility, which used pesticide-treated corn seed as feedstock for ethanol production. Organic (485), inorganic (34), and microbial (13) analytes were assessed at 15 locations in June 2022, to evaluate the relative contribution of facility-consistent pesticides (seed-treatment fungicides and insecticides) to overall TW-contaminant exposures and predicted human-health risks. Thirty-three organics (12 pesticides) and 28 inorganics were detected, the former including the fungicide sedaxane, insecticide chlorantraniliprole, and multiple neonicotinoid insecticides/degradates, all consistent with seed treatment and respective biofuel-facility waste. Assessment of pesticides only at extant point-of-use (POU) treatment taps at three sites demonstrated complete elimination of all TW-pesticide detections. Based on detection of maximum pesticide concentrations in a home located downstream along a creek capturing facility runoff, pesticides only were assessed in January 2023 again at this home and at three adjacent locations, confirming results at the former and documenting decreasing TW-pesticide concentrations, including neonicotinoids, with increasing distance from the creek. Human-health DW benchmarks are not available for many detected pesticides, including the detected fungicide and insecticides, but precautionary screening levels were exceeded frequently due to multiple inorganics. The results indicate that exposures to multiple (median: 4.5; range: 1–7) co-occurring TW contaminants of potential human-health concern are common, warranting consideration of point-of-entry or POU treatment(s) throughout the community to reduce or eliminate unrecognized exposures to TW contaminants, including facility-associated pesticides in down-gradient locations. More broadly, results emphasize the importance of continued characterization of private-TW exposures, employing a environmentally informative analytical scope, to identify and mitigate risks of unrecognized exposures in private-well-dependent rural communities.

Nebraska↗

Occurrence of mixed organic and inorganic chemicals in groundwater and tapwater, town of Campbell, Wisconsin, 2021–22

In response to previous reports of per- and polyfluoroalkyl substances (PFAS) contamination in French Island’s (located in the Mississippi River within the town of Campbell, Wisconsin) primary source of drinking water, 11 locations were sampled by the U.S. Geological Survey (USGS) in October 2021 to assess the potential presence of contaminant mixtures, including PFAS, in tapwater. Three locations were assessed seven times each over the course of three days. These samples were chosen to evaluate the water quality of the deeper Mount Simon bedrock aquifer and the water quality of the shallower sand and gravel (alluvial) aquifer at two locations. The other eight sample locations were spatially distributed within Campbell and were sampled once each. For each of these 11 sites, tapwater samples were analyzed for disinfection byproducts (DBP), pesticides, PFAS, pharmaceuticals, semi-volatile organic compounds (SVOC), volatile organic compounds (VOC), cations, anions, trace elements, alkalinity, microbial indicators, as well as measurements of water temperature, specific conductance, and pH. Of the 506 organic compounds analyzed in each water-quality sample, 74 (14 percent) were detected at least one time in any of the samples collected. Of the 14 percent, detected analytes included 27 pesticides (5 percent), 14 PFAS (3 percent), 6 pharmaceuticals (1 percent), 7 SVOC (1 percent), and 20 VOC (4 percent). No DBP were detected. The total number of organic compounds detected per sample ranged from 0–20 (median of 10), with the sum of concentrations ranging from not detected (nd)–2.53 micrograms per liter (μg/L; median of 0.333 μg/L). Of the inorganic constituents measured, eight were not detected above their reporting limit in any of the samples. The inorganic constituents that were not detected were antimony, arsenic, beryllium, cadmium, cobalt, molybdenum, selenium, and vanadium. Along with the 11 sites sampled throughout Campbell, Wisconsin, beginning in October 2021, four more wells were sampled on the Upper Midwest Environmental Sciences Center (UMESC) campus for PFAS. Three of these sites withdraw water from the shallow alluvial aquifer (the same source water for tapwater site 002) and one from the Mount Simon aquifer (the same source of water for tapwater site 001). This sampling is ongoing with results from samples through December 2022 summarized in this report. Of the 33 PFAS analyzed in samples from the four UMESC locations, 15 individual PFAS were detected at least one time in any of the samples analyzed with the sum of PFAS concentrations ranging from nd–1.49 μg/L (median of 0.309 μg/L).

Wisconsin↗

Tire-derived contaminants 6PPD and 6PPD-Q: Analysis, sample handling, and reconnaissance of United States stream exposures

The environmental ubiquity of tire and road wear particles (TRWP) underscores the need to understand the occurrence, persistence, and environmental effects of tire-related chemicals in aquatic ecosystems. One such chemical is 6PPD-quinone (6PPD-Q), a transformation product of the tire antioxidant 6PPD. In urban stormwater runoff 6PPD-Q can exceed acute toxicity thresholds for several salmonid species and is being implicated in significant coho salmon losses in the Pacific Northwest. There is a critical need to understand the prevalence of 6PPD-Q across watersheds to identify habitats heavily affected by TRWPs. We conducted a reconnaissance of 6PPD and 6PPD-Q in surface waters across the United States from sites (N = 94) with varying land use (urban, agricultural, and forested) and streamflow to better understand stream exposures. A rapid, low-volume direct-inject, liquid chromatography mass spectrometry method was developed for the quantitation of 6PPD-Q and screening for 6PPD. Laboratory holding times, bottle material, headspace, and filter materials were investigated to inform best practices for 6PPD-Q sampling and analysis. Glass bottles with PTFE-lined caps minimized sorption and borosilicate glass fiber filters provided the highest recovery. 6PPD-Q was stable for at least 5 months in pure laboratory solutions and for 75 days at 5 °C with minimal headspace in the investigated surface water and stormwaters. Results also indicated samples can be frozen to extend holding times. 6PPD was not detected in any of the 526 analyzed samples and there were no detections of 6PPD-Q at agricultural or forested sites. 6PPD-Q was frequently detected in stormwater (57%, N = 90) and from urban impacted sites (45%, N = 276) with concentrations ranging from 0.002 to 0.29 μg/L. The highest concentrations, above the lethal level for coho salmon, occurred during stormwater runoff events. This highlights the importance of capturing episodic runoff events in urban areas near ecologically relevant habitat or nursery grounds for sensitive species.

Chemosphere↗

Temporal concentrations of Quaternary ammonium compounds in wastewater treatment effluents during the COVID-19 pandemic, 2020–2021

Quaternary ammonium compounds (QAC) are high production chemicals used in many commercial and household disinfection products. During the SARS-CoV-2 (COVID-19) pandemic, QACs were included on lists of COVID-19 disinfectants. Increased QAC use could lead to higher levels of QACs in wastewater treatment plant (WWTP) effluents, which could subsequently be released into the environment. To evaluate QACs in WWTP effluent, three WWTPs in the northeastern United States were monitored from May 2020 through August 2021. Target QACs included six benzylalkyldimethyl ammonium compounds (BAC), three dialkyldimethyl ammonium compounds (DADMAC), two ethylbenzylalkyldimethyl ammonium compounds (EBAC), and benzethonium. At least one QAC was detected in every sample with individual concentrations up to 1600 ng L −1 . BAC-C 14 was detected most frequently, found in 93% of effluent samples; BAC-C 12 , BAC-C 16 , EBAC-C 12 and EBAC-C 14 were all detected in greater than 80% of samples. Few temporal patterns were observed in QAC concentrations with respect to weekly COVID-19 cases: at WWTP 2, DADMAC-C 8 :C 10 and DADMAC-C 10 were positively correlated, and DADMAC-C 8 negatively correlated. There were several seasonal trends at WWTP 1, including significant differences of ƩDADMAC, which were higher in fall than summer; ƩBAC was higher during the fall than both spring and summer; and ƩQAC where higher during the fall than spring.

Chemosphere↗

Multiple lines of evidence point to pesticides as stressors affecting invertebrate communities in small streams in five United States regions

Multistressor studies were performed in five regions of the United States to assess the role of pesticides as stressors affecting invertebrate communities in wadable streams. Pesticides and other chemical and physical stressors were measured in 75 to 99 streams per region for 4 weeks, after which invertebrate communities were surveyed (435 total sites). Pesticides were sampled weekly in filtered water, and once in bed sediment. The role of pesticides as a stressor to invertebrate communities was assessed by evaluating multiple lines of evidence: toxicity predictions based on measured pesticide concentrations, multivariate models and other statistical analyses, and previously published mesocosm experiments. Toxicity predictions using benchmarks and species sensitivity distributions and statistical correlations suggested that pesticides were present at high enough concentrations to adversely affect invertebrate communities at the regional scale. Two undirected techniques—boosted regression tree models and distance-based linear models—identified which pesticides were predictors of (respectively) invertebrate metrics and community composition. To put insecticides in context with known, influential covariates of invertebrate response, generalized additive models were used to identify which individual pesticide(s) were important predictors of invertebrate community condition in each region, after accounting for natural covariates. Four insecticides were identified as stressors to invertebrate communities at the regional scale: bifenthrin, chlordane, fipronil and its degradates, and imidacloprid. Fipronil was particularly important in the Southeast region, and imidacloprid, bifenthrin, and chlordane were important in multiple regions. For imidacloprid, bifenthrin, and fipronil, toxicity predictions were supported by mesocosm experiments that demonstrated adverse effects on naïve aquatic communities when dosed under controlled conditions. These multiple lines of evidence do not prove causality—which is challenging in the field under multistressor conditions—but they make a strong case for the role of insecticides as stressors adversely affecting invertebrate communities in streams within the five sampled regions.

Science of the Total Environment↗

A brief note on substantial sub-daily arsenic variability in pumping drinking-water wells in New Hampshire

Large variations in redox-related water parameters, like pH and dissolved oxygen (DO), have been documented in New Hampshire (United States) drinking-water wells over the course of a few hours under pumping conditions. These findings suggest that comparable sub-daily variability in dissolved concentrations of redox-reactive and toxic arsenic (As) also may occur, representing a potentially critical public-health data gap and a fundamental challenge for long-term As-trends monitoring. To test this hypothesis, discrete groundwater As samples were collected approximately hourly during one day in May and again in August 2019 from three New Hampshire drinking-water wells (2 public-supply, 1 private) under active pumping conditions. Collected samples were assessed by laboratory analysis (total As [As Tot ], As(III), As(V)) and by field analysis (As Tot ) using a novel integrated biosensor system. Laboratory analysis revealed sub-daily variability (range) in As Tot concentrations equivalent to 16 % – 36 % of that observed in the antecedent 3-year bimonthly trend monitoring. Thus, the results indicated that, along with previously demonstrated seasonality effects, the timing and duration of pumping are important considerations when assessing trends in drinking-water As exposures and concomitant risks. Results also illustrated the utility of the field sensor for monitoring and management of As Tot exposures in near-real-time.

Science of the Total Environment↗

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↗

Predictions of groundwater PFAS occurrence at drinking water supply depths in the United States

Per- and polyfluoroalkyl substances (PFAS), known colloquially as “forever chemicals”, have been associated with adverse human health effects and have contaminated drinking water supplies across the United States owing to their long-term and widespread use. People in the United States may unknowingly be drinking water that contains PFAS because of a lack of systematic analysis, particularly in domestic water supplies. We present an extreme gradient boosting model for predicting the occurrence of PFAS in groundwater at the depths of drinking water supply for the conterminous United States. Our model results indicate that 71 to 95 million people in the conterminous United States potentially rely on groundwater with detectable concentrations of PFAS for their drinking-water supplies prior to any treatment.

conterminous United States↗

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↗