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At least 55 records · Page 3Linked to original sources

Machine-learning predictions of high arsenic and high manganese at drinking water depths of the glacial aquifer system, northern continental United States

Globally, over 200 million people are chronically exposed to arsenic (As) and/or manganese (Mn) from drinking water. We used machine-learning (ML) boosted regression tree (BRT) models to predict high As (>10 μg/L) and Mn (>300 μg/L) in groundwater from the glacial aquifer system (GLAC), which spans 25 states in the northern United States and provides drinking water to 30 million people. Our BRT models’ predictor variables (PVs) included recently developed three-dimensional estimates of a suite of groundwater age metrics, redox condition, and pH. We also demonstrated a successful approach to significantly improve ML prediction sensitivity for imbalanced data sets (small percentage of high values). We present predictions of the probability of high As and high Mn concentrations in groundwater, and uncertainty, at two nonuniform depth surfaces that represent moving median depths of GLAC domestic and public supply wells within the three-dimensional model domain. Predicted high likelihood of anoxic condition (high iron or low dissolved oxygen), predicted pH, relative well depth, several modeled groundwater age metrics, and hydrologic position were all PVs retained in both models; however, PV importance and influence differed between the models. High-As and high-Mn groundwater was predicted with high likelihood over large portions of the central part of the GLAC.

Environmental Science & Technology↗

Atmospheric processing of iron-bearing mineral dust aerosol and its effect on growth of a marine diatom, Cyclotella meneghiniana

Iron (Fe) is a growth-limiting micronutrient for phytoplankton in major areas of oceans and deposited wind-blown desert dust is a primary Fe source to these regions. Simulated atmospheric processing of four mineral dust proxies and two natural dust samples followed by subsequent growth studies of the marine planktic diatom Cyclotella meneghiniana in artificial sea-water (ASW) demonstrated higher growth response to ilmenite (FeTiO 3 ) and hematite (α-Fe 2 O 3 ) mixed with TiO 2 than hematite alone. The processed dust treatment enhanced diatom growth owing to dissolved Fe (DFe) content. The fresh dust-treated cultures demonstrated growth enhancements without adding such dissolved Fe. These significant growth enhancements and dissolved Fe measurements indicated that diatoms acquire Fe from solid particles. When diatoms were physically separated from mineral dust particles, the growth responses become smaller. The post-mineralogy analysis of mineral dust proxies added to ASW showed a diatom-induced increased formation of goethite, where the amount of goethite formed correlated with observed enhanced growth. The current work suggests that ocean primary productivity may not only depend on dissolved Fe but also on suspended solid Fe particles and their mineralogy. Further, the diatom C. meneghiniana benefits more from mineral dust particles in direct contact with cells than from physically impeded particles, suggesting the possibility for alternate Fe-acquisition mechanism/s.

Environmental Science & Technology↗

Isolating the AFFF signature in coastal watersheds using oxidizable PFAS precursors and unexplained organofluorine

Water supplies for millions of U.S. individuals exceed maximum contaminant levels for per- and polyfluoroalkyl substances (PFAS). Contemporary and legacy use of aqueous film forming foams (AFFF) is a major contamination source. However, diverse PFAS sources are present within watersheds, making it difficult to isolate their predominant origins. Here we examine PFAS source signatures among six adjacent coastal watersheds on Cape Cod, MA, U.S.A. using multivariate clustering techniques. A distinct signature of AFFF contamination enriched in precursors with six perfluorinated carbons (C6) was identified in watersheds with an AFFF source, while others were enriched in C4 precursors. Principal component analysis of PFAS composition in impacted watersheds showed a decline in precursor composition relative to AFFF stocks and a corresponding increase in terminal perfluoroalkyl sulfonates with < C6 but not those with ≥ C6. Prior work shows that in AFFF stocks, all extractable organofluorine (EOF) can be explained by targeted PFAS and precursors inferred using Bayesian inference on the total oxidizable precursor assay. Using the same techniques for the first time in impacted watersheds, we find that only 24%–63% of the EOF can be explained by targeted PFAS and oxidizable precursors. Our work thus indicates the presence of large non-AFFF organofluorine sources in these coastal watersheds.

Massachusetts↗

Untargeted lipidomics for determining cellular and sub-cellular responses in Zebrafish (Danio rerio) liver cells following exposure to complex mixtures in U.S. streams

Surface waters often contain a variety of chemical contaminants potentially capable of producing adverse outcomes in both humans and wildlife due to impacts from industrial, urban, and agricultural activity. Here, we report the results of a zebrafish liver (ZFL) cell-based lipidomics approach to assess the potential ecotoxicological effects of complex contaminant mixtures using water collected from eight impacted streams across the United States mainland and Puerto Rico. We initially characterized the ZFL lipidome using high resolution mass spectrometry, resulting in the annotation of 508 lipid species covering 27 classes. We then identified lipid changes induced by all streamwater samples (nonspecific stress indicators) as well as those unique to water samples taken from specific streams. Subcellular impacts were classified based on organelle-specific lipid changes, including increased lipid saturation (endoplasmic reticulum stress), elevated bis(monoacylglycero)phosphate (lysosomal overload), decreased ubiquinone (mitochondrial dysfunction), and elevated ether lipids (peroxisomal stress). Finally, we demonstrate how these results can uniquely inform environmental monitoring and risk assessments of surface waters.

Environmental Science & Technology↗

Discrete sample introduction module for quantitative and isotopic analysis of methane and other gases by cavity ring-down spectroscopy

Carbon dioxide (CO 2 ) and methane (CH 4 ) are natural and anthropogenic products that play a central role in the global carbon cycle and regulating Earth’s climate. Applications utilizing laser absorption spectroscopy, which continuously measure concentrations and stable isotope ratios of these greenhouse gases, are routinely employed to measure the source and magnitude of atmospheric inputs. We developed a discrete sample introduction module (DSIM) to enable measurements of methane and CO 2 concentrations and δ 13 C values from limited volume (5–100 mL) gas samples when interfaced with a commercially available cavity ring-down spectroscopy (CRDS) analyzer. The analysis has a dynamic range that spans six orders of magnitude from 100% analyte to the lower limit of instrument detection (2 ppm). We demonstrate system performance for methane by comparing concentrations and δ 13 C results from the DSIM-CRDS system and traditional methods for a variety of sample types, including low concentration (nanomolar CH 4 ) seawater and high concentration (>90% CH 4 ) natural gas. The expansive concentration range of the field-portable DSIM-CRDS system can measure enhances analytical performance for investigating methane and CO 2 dynamics and, potentially, other gases measured by laser absorption spectroscopy.

Environmental Science & Technology↗

Exposure and transport of alkaloids and phytoestrogens from soybeans to agricultural soils and streams in the Midwestern United States

Phytotoxins are naturally produced toxins with potencies similar/higher than many anthropogenic micropollutants. Nevertheless, little is known regarding their environmental fate and off-field transport to streams. To fill this research gap, a network of six basins in the Midwestern United States with substantial soybean production was selected for the study. Stream water ( n = 110), soybean plant tissues ( n = 8), and soil samples ( n = 16) were analyzed for 12 phytotoxins (5 alkaloids and 7 phytoestrogens) and 2 widely used herbicides (atrazine and metolachlor). Overall, at least 1 phytotoxin was detected in 82% of the samples, with as many as 11 phytotoxins detected in a single sample (median = 5), with a concentration range from below detection to 37 and 68 ng/L for alkaloids and phytoestrogens, respectively. In contrast, the herbicides were ubiquitously detected at substantially higher concentrations (atrazine: 99% and metolachlor: 83%; the concentrations range from below detection to 150 and 410 ng/L, respectively). There was an apparent seasonal pattern for phytotoxins, where occurrence prior to and during harvest season (September to November) and during the snow melt season (March) was higher than that in December–January. Runoff events increased phytotoxin and herbicide concentrations compared to those in base-flow conditions. Phytotoxin plant concentrations were orders of magnitude higher compared to those measured in soil and streams. These results demonstrate the potential exposure of aquatic and terrestrial organisms to soybean-derived phytotoxins.

Illinois, Indiana, Iowa, Minnesota, Missouri, Sout↗

Characterization of halogenated organic compounds in pelagic sharks and sea turtles using a nontargeted approach

Halogenated organic compounds (HOCs) in marine species collected from the Atlantic Ocean [3 shortfin mako ( Isurus oxyrinchus ) and 1 porbeagle ( Lamna nasus )], and 12 sea turtles collected from the Pacific Ocean [3 loggerhead ( Caretta caretta ), 3 green ( Chelonia mydas ), 3 olive ridley ( Lepidochelys olivacea ), and 3 hawksbill ( Eretmochelys imbricata )] were analyzed with a nontargeted analytical method using two-dimensional gas chromatography coupled to high-resolution time-of-flight mass spectrometry. Sharks and sea turtles had distinct HOC profiles. Halogenated methoxyphenols (halo-MeOPs) were the most abundant compound class identified in sea turtle livers, while polychlorinated biphenyls (PCBs) were the most abundant in shark livers. In addition to legacy contaminants and halo-MeOPs, a total of 110 nontargeted/novel HOCs (NHOCs) were observed in the shark livers. Shortfin mako collected from the northern Gulf of Mexico contained the largest number (89) and most diverse structural classes of NHOCs. Among all NHOCs, a group of compounds with the elemental composition C 14 H 12– n Cl n ( n = 5–8) exhibited the highest concentrations, followed by chlorocarbazoles and tris(chlorophenyl) methanes (TCPMs). Using nontargeted workflows, a variety of known and unknown HOCs were observed, which demonstrate the need to develop more complete chemical profiles in the marine environment.

Environmental Science & Technology↗

Watershed-scale risk to aquatic organisms from complex chemical mixtures in the Shenandoah River

River waters contain complex chemical mixtures derived from natural and anthropogenic sources. Aquatic organisms are exposed to the entire chemical composition of the water, resulting in potential effects at the organismal through ecosystem level. This study applied a holistic approach to assess landscape, hydrological, chemical, and biological variables. On-site mobile laboratory experiments were conducted to evaluate biological effects of exposure to chemical mixtures in the Shenandoah River Watershed. A suite of 534 inorganic and organic constituents were analyzed, of which 273 were detected. A watershed-scale accumulated wastewater model was developed to predict environmental concentrations of chemicals derived from wastewater treatment plants (WWTPs) to assess potential aquatic organism exposure for all stream reaches in the watershed. Measured and modeled concentrations generally were within a factor of 2. Ecotoxicological effects from exposure to individual components of the chemical mixture were evaluated using risk quotients (RQs) based on measured or predicted environmental concentrations and no effect concentrations or chronic toxicity threshold values. Seventy-two percent of the compounds had RQ values <0.1, indicating limited risk from individual chemicals. However, when individual RQs were aggregated into a risk index, most stream reaches receiving WWTP effluent posed potential risk to aquatic organisms from exposure to complex chemical mixtures.

Virginia↗

Perfluoroalkyl and polyfluoroalkyl substances in groundwater used as a source of drinking water in the eastern United States

In 2019, 254 samples were collected from five aquifer systems to evaluate per- and polyfluoroalkyl substance (PFAS) occurrence in groundwater used as a source of drinking water in the eastern United States. The samples were analyzed for 24 PFAS, major ions, nutrients, trace elements, dissolved organic carbon (DOC), volatile organic compounds (VOCs), pharmaceuticals, and tritium. Fourteen of the 24 PFAS were detected in groundwater, with 60% and 20% of public-supply and domestic wells, respectively, containing at least one PFAS detection. Concentrations of tritium, chloride, sulfate, DOC, and manganese+iron; percent urban land use within 500 m of the wells; and VOC and pharmaceutical detection frequencies were significantly higher in samples containing PFAS detections than in samples with no detections. Boosted Regression Tree models that consider 57 chemical and land-use variables show that tritium concentration, distance to the nearest fire-training area, percentage of urban land use, and DOC and VOC concentrations are the top five predictors of PFAS detections, consistent with hydrologic position, geochemistry, and land use being important controls on PFAS occurrence in groundwater. Model results indicate it may be possible to predict PFAS detections in groundwater using existing data sources.

Glacial aquifer, Mississippi Embayment aquifer, So↗

Nutrient improvements in Chesapeake Bay: Direct effect of load reductions and implications for coastal management

In Chesapeake Bay in the United States, decades of management efforts have resulted in modest reductions of nutrient loads from the watershed, but corresponding improvements in estuarine water quality have not clearly materialized. Generalized additive models were used to directly link river flows and nutrient loads from the watershed to nutrient trends in the estuary on a station-by-station basis, which allowed for identification of exactly when and where responses are happening. Results show that Chesapeake Bay total nitrogen and total phosphorus conditions are mostly improving after accounting for variation in freshwater flow. Almost all of these improving nutrient concentrations in the estuary can be explained by reductions in watershed loads entering through 16 rivers and 145 nearby point sources. These two major types of loads from multiple locations across the watershed are together necessary and responsible for improving estuarine nutrient conditions, a finding that is highly relevant to managing valuable estuarine resources worldwide.

Maryland, Virginia↗

Statewide quantitative microbial risk assessment for waterborne viruses, bacteria, and protozoa in public water supply wells in Minnesota

Infection risk from waterborne pathogens can be estimated via quantitative microbial risk assessment (QMRA) and forms an important consideration in the management of public groundwater systems. However, few groundwater QMRAs use site-specific hazard identification and exposure assessment, so prevailing risks in these systems remain poorly defined. We estimated the infection risk for 9 waterborne pathogens based on a 2-year pathogen occurrence study in which 964 water samples were collected from 145 public wells throughout Minnesota, USA. Annual risk across all nine pathogens combined was 3.3 × 10 –1 (95% CI: 2.3 × 10 –1 to 4.2 × 10 –1 ), 3.9 × 10 –2 (2.3 × 10 –2 to 5.4 × 10 –2 ), and 1.2 × 10 –1 (2.6 × 10 –2 to 2.7 × 10 –1 ) infections person –1 year –1 for noncommunity, nondisinfecting community, and disinfecting community wells, respectively. Risk estimates exceeded the U.S. benchmark of 10 –4 infections person –1 year –1 in 59% of well-years, indicating that the risk was widespread. While the annual risk for all pathogens combined was relatively high, the average daily doses for individual pathogens were low, indicating that significant risk results from sporadic pathogen exposure. Cryptosporidium dominated annual risk, so improved identification of wells susceptible to Cryptosporidium contamination may be important for risk mitigation.

Minnesota↗

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↗

Rock-to-metal ratio: A foundational metric for understanding mine wastes

The quantity of ore mined and waste rock (i.e., overburden or barren rock) removed to produce a refined unit of a mineral commodity, its rock-to-metal ratio (RMR), is an important metric for understanding mine wastes and environmental burdens. In this analysis, we provide a comprehensive examination of RMRs for 25 commodities for 2018. The results indicate significant variability across commodities. Precious metals like gold have RMRs in the range of 10 5 –10 6 , while iron ore and aluminum are on the order of 10 1 . The results also indicate significant variability across operations for a single commodity. The interquartile range of RMRs for individual cobalt operations, for example, varies from 465 to 2157, with a global RMR of 859. RMR variability is mainly driven by ore grades and revenue contribution. The total attributable ore mined and waste rock removed in the production of these 25 commodities sums to 37.6 billion metric tons, 83% of which is attributable to iron ore, copper, and gold. RMRs provide an additional dimension for evaluating the impact of materials and material choice trade-offs. The results can enhance life cycle inventories and be extended to evaluate areas of surface disturbances, mine tailings, energy requirements, and associated greenhouse gas emissions.

Environmental Science & Technology↗

Complex life histories alter patterns of mercury exposure and accumulation in a pond-breeding amphibian

Quantifying how contaminants change across life cycles of species that undergo metamorphosis is critical to assessing organismal risk, particularly for consumers. Pond-breeding amphibians can dominate aquatic animal biomass as larvae and are terrestrial prey as juveniles and adults. Thus, amphibians can be vectors of mercury exposure in both aquatic and terrestrial food webs. However, it is still unclear how mercury concentrations are affected by exogenous (e.g., habitat or diet) vs endogenous factors (e.g., catabolism during hibernation) as amphibians undergo large diet shifts and periods of fasting during ontogeny. We measured total mercury (THg), methylmercury (MeHg), and isotopic compositions (δ 13 C, δ 15 N) in boreal chorus frogs ( Pseudacris maculata ) across five life stages in two Colorado (USA) metapopulations. We found large differences in concentrations and percent MeHg (of THg) among life stages. Frog MeHg concentrations peaked during metamorphosis and hibernation coinciding with the most energetically demanding life cycle stages. Indeed, life history transitions involving periods of fasting coupled with high metabolic demands led to large increases in mercury concentrations. The endogenous processes of metamorphosis and hibernation resulted in MeHg bioamplification, thus decoupling it from the light isotopic proxies of diet and trophic position. These step changes are not often considered in conventional expectations of how MeHg concentrations within organisms are assessed.

Environmental Science & Technology↗

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↗

Mercury bioaccumulation and cortisol interact to influence endocrine and immune biomarkers in a free-ranging marine mammal

Mercury bioaccumulation from deep-ocean prey and the extreme life history strategies of adult female northern elephant seals ( Mirounga angustirostris ) provide a unique system to assess the interactive effects of mercury and stress on animal health by quantifying blood biomarkers in relation to mercury (skeletal muscle and blood mercury) and cortisol concentrations. The thyroid hormone thyroxine (tT4) and the antibody immunoglobulin E (IgE) were associated with mercury and cortisol concentrations interactively, where the magnitude and direction of the association of each biomarker with mercury or cortisol changed depending on the concentration of the other factor. For example, when cortisol concentrations were lowest, tT4 was positively related to muscle mercury, whereas tT4 had a negative relationship with muscle mercury in seals that had the highest cortisol concentrations. Additionally, we observed that two thyroid hormones, triiodothyronine (tT3) and reverse triiodothyronine (rT3), were negatively (tT3) and positively (rT3) associated with mercury concentrations and cortisol in an additive manner. As an example, tT3 concentrations in late breeding seals at the median cortisol concentration decreased by 14% across the range of observed muscle mercury concentrations. We also observed that immunoglobulin M (IgM), the pro-inflammatory cytokine IL-6 (IL-6), and a reproductive hormone, estradiol, were negatively related to muscle mercury concentrations but were not related to cortisol. Specifically, estradiol concentrations in late molting seals decreased by 50% across the range of muscle mercury concentrations. These results indicate important physiological effects of mercury on free-ranging apex marine predators and interactions between mercury bioaccumulation and extrinsic stressors. Deleterious effects on animals’ abilities to maintain homeostasis (thyroid hormones), fight off pathogens and disease (innate and adaptive immune system), and successfully reproduce (endocrine system) can have significant individual- and population-level consequences.

Environmental Science & Technology↗

Centurial persistence of forever chemicals at military fire training sites

Drinking water contamination by per- and polyfluoroalkyl substances (PFAS) is widespread near more than 300 United States (U.S.) military bases that used aqueous film-forming foams (AFFF) for fire training and firefighting activities. Much of the PFAS at these sites consist of precursors that can transform into terminal compounds of known health concern but are omitted from standard analytical methods. Here, we estimate the expected duration and contribution of precursor biotransformation to groundwater PFAS contamination at an AFFF-contaminated military base on Cape Cod, Massachusetts, United States, by optimizing a geochemical box model using measured PFAS concentrations from a multidecadal time series of groundwater and a soil survey in the source zone. A toolbox of analytical techniques used to reconstruct the mass budget of PFAS showed that precursors accounted for 46 ± 8% of the extractable organofluorine (a proxy for total PFAS) across years. Terminal PFAS still exceed regulatory limits by 2000-fold decades after AFFF use ceased. Measurements and numerical modeling show that sulfonamido precursors are retained in the vadose zone and their slow biotransformation into perfluoroalkyl sulfonates (half-life > 66 yr) sustains groundwater concentrations of perfluorobutane sulfonate (PFBS) and perfluorohexane sulfonate (PFHxS). The estimated PFAS reservoir in the vadose zone and modeled flux into groundwater suggest PFAS contamination above regulatory guidelines will persist for centuries without remediation.

Massachusetts↗

Tire-derived transformation product 6PPD-quinone induces mortality and transcriptionally disrupts vascular permeability pathways in developing coho salmon

Urban stormwater runoff frequently contains the car tire transformation product 6PPD-quinone, which is highly toxic to juvenile and adult coho salmon ( Onchorychus kisutch ). However, it is currently unclear if embryonic stages are impacted. We addressed this by exposing developing coho salmon embryos starting at the eyed stage to three concentrations of 6PPD-quinone twice weekly until hatch. Impacts on survival and growth were assessed. Further, whole-transcriptome sequencing was performed on recently hatched alevin to address the potential mechanism of 6PPD-quinone-induced toxicity. Acute mortality was not elicited in developing coho salmon embryos at environmentally measured concentrations lethal to juveniles and adults, however, growth was inhibited. Immediately after hatching, coho salmon were sensitive to 6PPD-quinone mortality, implicating a large window of juvenile vulnerability prior to smoltification. Molecularly, 6PPD-quinone induced dose-dependent effects that implicated broad dysregulation of genomic pathways governing cell–cell contacts and endothelial permeability. These pathways are consistent with previous observations of macromolecule accumulation in the brains of coho salmon exposed to 6PPD-quinone, implicating blood–brain barrier disruption as a potential pathway for toxicity. Overall, our data suggests that developing coho salmon exposed to 6PPD-quinone are at risk for adverse health events upon hatching while indicating potential mechanism(s) of action for this highly toxic chemical.

Environmental Science & Technology↗