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At least 1,153 records · Page 64Linked to original sources

Radium accumulation in carbonate river sediments at oil and gas produced water discharges: Implications for beneficial use as disposal management

In the western U.S., produced water from oil and gas wells discharged to surface water augments downstream supplies used for irrigation and livestock watering. Here we investigate six permitted discharges on three neighboring tributary systems in Wyoming. During 2013-16, we evaluated radium activities of the permitted discharges and the potential for radium accumulation in associated stream sediments. Radium activities of the sediments at the points of discharge ranged from approximately 200-3600 Bq/kg with elevated activities above the background of 74 Bq/kg over 30 km downstream of one permitted discharge. Sediment as deep as 30 cm near the point of discharge had radium activities elevated above background. X-ray diffraction and targeted sequential extraction of radium in sediments indicate that radium is likely coprecipitated with carbonate, and to a lesser extent sulfate minerals. PHREEQC modeling predicts radium coprecipitation with aragonite and barite, but over-estimates the latter compared to observations of downstream sediment, where carbonate predominates. Mass-balance calculations indicate over 3 billion Bq of radium activity (226Ra+228Ra) is discharged each year from five of the discharges, combined, with only 5 percent of the annual load retained in stream sediments within 100m of the effluent discharges; the remaining 95 percent of the radium is transported farther downstream as sediment-associated and aqueous species

Environmental Science↗

Accuracy of methods for reporting inorganic element concentrations and radioactivity in oil and gas wastewaters from the Appalachian Basin, U.S. based on an inter-laboratory comparison.

Accurate and precise analyses of oil and gas (O&G) wastewaters and solids ( e.g. , sediments and sludge) are important for the regulatory monitoring of O&G development and tracing potential O&G contamination in the environment. In this study, 15 laboratories participated in an inter-laboratory comparison on the chemical characterization of three O&G wastewaters from the Appalachian Basin and four solids impacted by O&G development, with the goal of evaluating the quality of data and the accuracy of measurements for various analytes of concern. Using a variety of different methods, analytes in the wastewaters with high concentrations ( i.e. , >5 mg L −1 ) were easily detectable with relatively high accuracy, often within ±10% of the most probable value (MPV). In contrast, often less than 7 of the 15 labs were able to report detectable trace metal(loid) concentrations ( i.e. , Cr, Ni, Cu, Zn, As, and Pb) with accuracies of approximately ±40%. Despite most labs using inductively coupled plasma mass spectrometry (ICP-MS) with low instrument detection capabilities for trace metal analyses, large dilution factors during sample preparation and low trace metal concentrations in the wastewaters limited the number of quantifiable determinations and likely influenced analytical accuracy. In contrast, all the labs measuring Ra in the wastewaters were able to report detectable concentrations using a variety of methods including gamma spectroscopy and wet chemical approaches following Environmental Protection Agency (EPA) standard methods. However, the reported radium activities were often greater than ±30% different to the MPV possibly due to calibration inconsistencies among labs, radon leakage, or failing to correct for self-attenuation. Reported radium activities in solid materials had less variability (±20% from MPV) but accuracy could likely be improved by using certified radium standards and accounting for self-attenuation that results from matrix interferences or a density difference between the calibration standard and the unknown sample. This inter-laboratory comparison illustrates that numerous methods can be used to measure major cation, minor cation, and anion concentrations in O&G wastewaters with relatively high accuracy while trace metal(loid) and radioactivity analyses in liquids may often be over ±20% different from the MPV.

Appalachian Basin↗

Emerging investigator series: Atmospheric cycling of indium in the northeastern United States

Indium is critical to the global economy and is used in an increasing number of electronics and new energy technologies. However, little is known about its environmental behavior or impacts, including its concentrations or cycling in the atmosphere. This study determined indium concentrations in air particulate matter at five locations across the northeastern United States over the course of one year, in 1995. Historical records from a Massachusetts bog core showed that indium atmospheric concentrations in this region changed only modestly between 1995 and 2010. Atmospheric indium concentrations varied significantly both geographically and temporally, with average concentrations in PM 3 of 2.1 ± 1.6 pg m −3 (1 standard deviation), and average particle-normalized concentrations of 0.2 ± 0.2 μg In per g PM 3 . Peaks in the particle-normalized concentrations in two New York sites were correlated with wind direction; air coming from the north contributed higher concentrations of indium than air coming from the west. This correlation, along with measurements of indium in zinc smelter emissions and coal fly ash, suggests that indium in the atmosphere in the northeastern United States comes from a relatively constant low-level input from coal combustion in the midwest, and higher but more sporadic contributions from the smelting of lead, zinc, copper, tin, and nickel north of the New York sample sites. Understanding the industrial sources of indium to the atmosphere and how they compare with natural sources can lead to a better understanding of the impact of human activities on the indium cycle, and may help to establish a baseline for monitoring future impacts as indium use grows.

Massachusetts, New York↗

Spatial distribution of heavy metals in the West Dongting Lake floodplain, China

The protection of Dongting Lake is important because it is an overwintering and migration route for many rare and endangered birds of East Asia and Australasia, but an assessment of heavy metal contamination in West Dongting Lake is lacking. A total of 75 sediment samples (five sites x three sediment depths x five repeats) were collected in West Dongting Lake in January 2017 to assess the spatial distribution and ecological risk of heavy metal in West Dongting Lake. Heavy metal values varied by sediment depth including As, Cd, Zn, and Cu, with depth giving an indication of recent vs. historical deposition. The major input of Hg, Cu, Ni may come from continued anthropogenic activities related to regional industrial activities within Yuan River and Li River whereas, the major sources of spread Cd pollution may be from agricultural fertilizers.

West Dongting Lake floodplain↗

A critical review on the potential impacts of neonicotinoid insecticide use: Current knowledge of environmental fate, toxicity, and implications for human health

Neonicotinoid insecticides are widely used in both urban and agricultural settings around the world. Historically, neonicotinoid insecticides have been viewed as ideal replacements for more toxic compounds, like organophosphates, due in part to their perceived limited potential to affect the environment and human health. This critical review investigates the environmental fate and toxicity of neonicotinoids and their metabolites and the potential risks associated with exposure. Neonicotinoids are found to be ubiquitous in the environment, drinking water, and food, with low-level exposure commonly documented below acceptable daily intake standards. Available toxicological data from animal studies indicate possible genotoxicity, cytotoxicity, impaired immune function, and reduced growth and reproductive success at low concentrations, while limited data from ecological or cross-sectional epidemiological studies have identified acute and chronic health effects ranging from acute respiratory, cardiovascular, and neurological symptoms to oxidative genetic damage and birth defects. Due to the heavy use of neonicotinoids and potential for cumulative chronic exposure, these insecticides represent novel risks and necessitate further study to fully understand their risks to humans.

Environmental Science: Processes and Impacts↗

De facto reuse and disinfection by-products in drinking water systems in the Shenandoah River watershed

De facto reuse is increasingly being studied among the variety of stressors that are relevant to drinking water systems that obtain their source water from surface waters. De facto reuse may influence the levels and types of precursors relevant to formation of disinfection by-products (DBPs) in surface water systems. DBPs such as trihalomethanes (THMs) and haloacetic acids (HAAs) have been associated with bladder cancer and other health concerns in people who use drinking water provided by public water systems (PWSs). In this study, we used compliance monitoring data from conventional surface water PWSs in the Shenandoah River watershed to evaluate the relationship between de facto reuse in the watershed with DBP formation in those systems. The Shenandoah River watershed was selected for this study because it has a relatively small group of PWSs that draw their source water from surface waters in the watershed, the majority of whom treat their water using chlorine, and are less likely to have confounding factors (such as complex distribution systems or lengthy residence times) than other watersheds. We found that concentrations of THM4 and HAA5 increase in drinking water systems as de facto reuse increases in their source waters and that the relation is observed at both annual average and low streamflow conditions (annual average and low streamflow increases were statistically significant for THM4 with p values of 0.027 and 0,021, respectively). In addition, using a t -test, we found that a 1% level of de facto reuse was associated with significantly higher levels of THM4 and HAA5 ( p < 0.05) under annual average streamflow conditions. While the concentrations of HAA5 were also higher under annual average and low streamflow conditions, we did not find that they achieved a level of a significant difference. Results from this research will be helpful to operators of PWSs and other researchers and stakeholders with an interest in water reuse and DBPs.

Virginia↗

Landfill leachate contributes per-/poly-fluoroalkyl substances (PFAS) and pharmaceuticals to municipal wastewater

Widespread disposal of landfill leachate to municipal sewer infrastructure in the United States calls for an improved understanding of the relative organic-chemical contributions to the wastewater treatment plant (WWTP) waste stream and associated surface-water discharge to receptors in the environment. Landfill leachate, WWTP influent, and WWTP effluent samples were collected from three landfill-WWTP systems and compared with analogous influent and effluent samples from two WWTPs that did not receive leachate. Samples were analyzed for 73 per-/poly-fluoroalkyl substances (PFAS), 109 pharmaceuticals, and 21 hormones and related compounds. PFAS were detected more frequently in leachate (92%) than in influent (55%). Total PFAS concentrations in leachate (93,100 ng/L) were more than ten times higher than in influent (6,950 ng/L), and effluent samples (3,730 ng/L). Concentrations of bisphenol A; the nonprescription pharmaceuticals cotinine, lidocaine, nicotine; and the prescription pharmaceuticals amphetamine, carisoprodol, pentoxifylline, and thiabendazole were an order of magnitude higher in landfill leachate than WWTP influent. Leachate load contributions for PFAS (0.78 to 31 g/d), bisphenol A (0.97 to 8.3 g/d), and nonprescription (2.0 to 3.1 g/d) and prescription (0.48 to 2.5 g/d) pharmaceuticals to WWTP influent were generally low (<10 g/d) for most compounds because of high influent-to-leachate volumetric ratios (0.983). No clear differences in concentrations were apparent between effluents from WWTPs receiving landfill leachate and those that did not receive landfill leachate.

Environmental Science: Water Research & Technology↗

Emerging investigator series: Municipal wastewater as a year-round point source of neonicotinoid insecticides that persist in an effluent-dominated stream

Neonicotinoids in aquatic systems have been predominantly associated with agriculture, but some are increasingly being linked to municipal wastewater. Thus, the aim of this work was to understand the municipal wastewater contribution to neonicotinoids in a representative, characterized effluent-dominated temperate-region stream. Our approach was to quantify the spatiotemporal concentrations of imidacloprid, clothianidin, thiamethoxam, and transformation product imidacloprid urea: 0.1 km upstream, the municipal wastewater effluent, and 0.1 and 5.1 km downstream from the wastewater outfall (collected twice-monthly for one year under baseflow conditions). Quantified results demonstrated that wastewater effluent was a point-source of imidacloprid (consistently) and clothianidin (episodically), where chronic invertebrate exposure benchmarks were exceeded for imidacloprid (36/52 samples; 3/52 > acute exposure benchmark) and clothianidin (8/52 samples). Neonicotinoids persisted downstream where mass loads were not significantly different than those in the effluent. The combined analysis of neonicotinoid effluent concentrations, instream seasonality, and registered uses in Iowa all indicate imidacloprid, and seasonally clothianidin, were driven by wastewater effluent, whereas thiamethoxam and imidacloprid urea were primarily from upstream non-point sources (or potential in-stream transformation for imidacloprid urea). This is the first study to quantify neonicotinoid persistence in an effluent-dominated stream throughout the year—implicating wastewater effluent as a point-source for imidacloprid (year-round) and clothianidin (seasonal). These findings suggest possible overlooked neonicotinoid indoor human exposure routes with subsequent implications for instream ecotoxicological exposure.

Environmental Sciences: Processes & Impacts↗

Water–rock interaction and the concentrations of major, trace, and rare earth elements in hydrocarbon-associated produced waters of the United States

Studies of co-produced waters from hydrocarbon extraction across multiple energy-producing basins have generally focused on major ions or a few select tracers, and studies that examine trace elements and involve laboratory experiments have generally been basin specific. Here, new perspective is sought through a broad analysis of concentration data for 26 elements from three hydrocarbon well types using the U.S. Geological Survey National Produced Waters Geochemical Database (v2.3). Those data are compared to leachates (water, hydrochloric acid, and artificial brine) from 12 energy-resource related shales from across the United States. Both lower pH and higher ionic strength were associated with greater concentrations of many trace elements in produced waters. However, individual effects were difficult to distinguish because higher ionic strengths drive decreases in pH. Water–rock interactions in the leaching experiments generally replicated produced water concentrations for trace elements including Al, As, Cd, Co, Cu, Mo, Ni, Pb, Sb, Si, and Zn. Enhanced middle rare earth element (REE) mobilization relative to shale REE content occurred with low pH leachates. Produced water concentrations of Li, Sr, and Ba were not replicated by the leaching experiments. Patterns of high Li, Sr, and Ba concentrations and ratios relative to other elements across produced waters types indicate controls on these elements in many settings related to pore space pools of salts, brines, and ion-exchange sites affected by diagenetic processes. The size of those pools is diluted and masked by other water–rock interaction processes at the water–rock ratios necessitated by laboratory experiments. The results broadly link water–rock interaction processes and environmental patterns across a wide variety of produced waters and host formations and thus provide context for trace element data from other environmental and laboratory studies of such waters.

Environmental Science: Processes & Impacts↗

Surface-water/groundwater boundaries affect seasonal PFAS concentrations and PFAA precursor transformations​

Elevated concentrations of per- and polyfluoroalkyl substances (PFAS) in drinking-water supplies are a major concern for human health. It is therefore essential to understand factors that affect PFAS concentrations in surface water and groundwater and the transformation of perfluoroalkyl acid (PFAA) precursors that degrade into terminal compounds. Surface-water/groundwater exchange can occur along the flow path downgradient from PFAS point sources and biogeochemical conditions can change rapidly at these exchange boundaries. Here, we investigate the influence of surface-water/groundwater boundaries on PFAS transport and transformation. To do this, we conducted an extensive field-based analysis of PFAS concentrations in water and sediment from a flow-through lake fed by contaminated groundwater and its downgradient surface-water/groundwater boundary (defined as ≤100 cm below the lake bottom). PFAA precursors comprised 45 ± 4.6% of PFAS (PFAA precursors + 18 targeted PFAA) in the predominantly oxic lake impacted by a former fire-training area and historical wastewater discharges. In shallow porewater downgradient from the lake, this percentage decreased significantly to 25 ± 11%. PFAA precursor concentrations decreased by 85% between the lake and 84–100 cm below the lake bottom. PFAA concentrations increased significantly within the surface-water/groundwater boundary and in downgradient groundwater during the winter months despite lower stable concentrations in the lake water source. These results suggest that natural biogeochemical fluctuations associated with surface-water/groundwater boundaries may lead to PFAA precursor loss and seasonal variations in PFAA concentrations. Results of this work highlight the importance of dynamic biogeochemical conditions along the hydrological flow path from PFAS point sources to potentially affected drinking water supplies.

Massachusetts↗

Tracing the sources and depositional history of mercury to coastal northeastern U.S. lakes

Mercury (Hg) deposition was reconstructed in sediment cores from lakes in two coastal U.S. National Parks: Acadia National Park (ANP) and Cape Cod National Seashore (CCNS), to fill an important spatial gap in Hg deposition records and to explore changing sources of Hg and processes affecting Hg accumulation in these coastal sites. Recent Hg deposition chronology was assessed using (1) a newly developed lead-210 ( 210 Pb) based sediment age model which employs 7 Be to constrain deposition and sediment mixing of 210 Pb-excess, (2) coinciding Pb flux and isotope ratios ( 206 Pb/ 207 Pb), and (3) Hg isotope ratios and their response to changes in Hg flux. At both sites, Hg flux increased substantially from pre-1850 levels, with accumulation in ANP peaking in the 1970s, whereas in CCNS, Hg levels were highest in recent sediments. Negative values of δ 202 Hg and Δ 199 Hg indicated terrestrially-derived Hg was a major constituent of Hg flux to Sargent Mountain Pond, ANP, although recent decreases in Hg flux were in agreement with precipitation Hg records, indicating a rapid watershed response. By contrast, δ 202 Hg and Δ 199 Hg profiles in Long Pond, CNNS reflect direct Hg deposition, but disturbances in the sedimentary record were indicated by bomb fallout radionuclide inventories and by peaks in both Pb and Hg isotope depth profiles. These cores provided poor reconstructions of atmospheric deposition and reveal responses that are decoupled from emissions reduction due to complex post-depositional redistribution of atmospheric metals including Hg. The application of multiple tracers of Hg deposition provide insight into the sources and pathways governing Hg accumulation in these lakes.

Maine, Massachusetts↗

RNA-seq reveals potential gene biomarkers in fathead minnows (Pimephales promelas) for exposure to treated wastewater effluent

Discharged wastewater treatment plant (WWTP) effluent greatly contributes to the generation of complex mixtures of contaminants of emerging concern (CECs) in aquatic environments which often contain neuropharmaceuticals and other emerging contaminants that may impact neurological function. However, there is a paucity of knowledge on the neurological impacts of these exposures to aquatic organisms. In this study, caged fathead minnows ( Pimephales promelas ) were exposed in situ in a temperate-region effluent-dominated stream ( i.e. , Muddy Creek) in Coralville, Iowa, USA upstream and downstream of a WWTP effluent outfall. The pharmaceutical composition of Muddy Creek was recently characterized by our team and revealed many compounds there were at a low microgram to high nanogram per liter concentration. Total RNA sequencing analysis on brain tissues revealed 280 gene isoforms that were significantly differentially expressed in male fish and 293 gene isoforms in female fish between the upstream and downstream site. Only 66 (13%) of such gene isoforms overlapped amongst male and female fish, demonstrating sex-dependent impacts on neuronal gene expression. By using a systems biology approach paired with functional enrichment analyses, we identified several potential novel gene biomarkers for treated effluent exposure that could be used to expand monitoring of environmental effects with respect to complex CEC mixtures. Lastly, when comparing the results of this study to those that relied on a single-compound approach, there was relatively little overlap in terms of gene-specific effects. This discovery brings into question the application of single-compound exposures in accurately characterizing environmental risks of complex mixtures and for gene biomarker identification.

Iowa↗

Discovery and potential ramifications of reduced iron-bearing nanoparticles — Magnetite, wüstite, and zero-valent iron — In wildland–urban interface fire ashes

The increase in fires at the wildland–urban interface has raised concerns about the potential environmental impact of ash remaining after burning. Here, we examined the concentrations and speciation of iron-bearing nanoparticles in wildland–urban interface ash. Total iron concentrations in ash varied between 4 and 66 mg g −1 . Synchrotron X-ray absorption near-edge structure (XANES) spectroscopy of bulk ash samples was used to quantify the relative abundance of major Fe phases, which were corroborated by transmission electron microscopy measurements. Maghemite (γ-(Fe 3+ ) 2 O 3 ) and magnetite (γ-Fe 2+ (Fe 3+ ) 2 O 4 ) were detected in most ashes and accounted for 0–90 and 0–81% of the spectral weight, respectively. Ferrihydrite (amorphous Fe( III )–hydroxide, (Fe 3+ ) 5 HO 8 ·4H 2 O), goethite (α-Fe 3+ OOH), and hematite (α-Fe 3+ 2 O 3 ) were identified less frequently in ashes than maghemite and magnetite and accounted for 0–65, 0–54, and 0–50% of spectral weight, respectively. Other iron phases identified in ashes include wüstite (Fe 2+ O), zerovalent iron, FeS, FeCl 2 , FeCl 3 , FeSO 4 , Fe 2 (SO 4 ) 3 , and Fe(NO 3 ) 3 . Our findings demonstrate the impact of fires at the wildland–urban interface on iron speciation; that is, fires can convert iron oxides ( e.g. , maghemite, hematite, and goethite) to reduced iron phases such as magnetite, wüstite, and zerovalent iron. Magnetite concentrations ( e.g. , up to 25 mg g −1 ) decreased from black to gray to white ashes. Based on transmission electron microscopy (TEM) analyses, most of the magnetite nanoparticles were less than 500 nm in size, although larger particles were identified. Magnetite nanoparticles have been linked to neurodegenerative diseases as well as climate change. This study provides important information for understanding the potential environmental impacts of fires at the wildland–urban interface, which are currently poorly understood.

Environmental Science Nano↗

Improving gas-derived parameterization of groundwater using free phase gas measurements

Dissolved atmogenic gasses in groundwater provide significant information about recharge conditions, flowpath, and age. Free phase gas in aquifers is largely ignored in these analyses and there is a lack of quantitative analysis for gas flux mechanisms. Many related fields encountering multiphase flow acknowledge that the presence of bubbles allows for the rapid exsolution of dissolved gasses and volatile compounds through diffusive and polar forces. By measuring the mass flow of the exsolved gas at a spring, coupled with compositional analysis in the free and dissolved phases, we show that not incorporating the effects of the free gas phase of bubbling springs introduces error in the estimation of total gas quantities, particularly light noble gasses. This can significantly affect the corresponding estimation of noble gas temperature (NGT) and apparent age. We examine the transport of free and dissolved gas from the recharge zone, using water level variation data, to the discharge location where the gases are measured. This technique of using the free gas phase for assessing aquifer dynamics will improve groundwater conceptual models, particularly in karstic aquifers where rapid fluctuations in the water table facilitate the development of excess air, generating multiphase spring discharge.

Environmental Science: Water Research & Technology↗

Modeling risk dynamics of contaminants of emerging concern in a temperate-region wastewater effluent-dominated stream

Wastewater effluent-dominated streams are becoming increasingly common worldwide, including in temperate regions, with potential impacts on ecological systems and drinking water sources. We recently quantified the occurrence/spatiotemporal dynamics of pharmaceutical mixtures in a representative temperate-region wastewater effluent-dominated stream (Muddy Creek, Iowa) under baseflow conditions and characterized relevant fate processes. Herein, we quantified the ecological risk quotients (RQs) of 19 effluent-derived contaminants of emerging concern (CECs; including: 14 pharmaceuticals, 2 industrial chemicals, and 3 neonicotinoid insecticides) and 1 run-off-derived compound (atrazine) in the stream under baseflow conditions, and estimated the probabilistic risks of effluent-derived CECs under all-flow conditions ( i.e. , including runoff events) using stochastic risk modeling. We determined that 11 out of 20 CECs pose medium-to-high risks to local ecological systems ( i.e. , algae, invertebrates, fish) based on literature-derived acute effects under measured baseflow conditions. Stochastic risk modeling indicated decreased, but still problematic, risk of effluent-derived CECs ( i.e. , RQ ≥ 0.1) under all-flow conditions when runoff events were included. Dilution of effluent-derived chemicals from storm flows thus only minimally decreased risk to aquatic biota in the effluent-dominated stream. We also modeled in-stream transport. Thirteen out of 14 pharmaceuticals persisted along the stream reach (median attenuation rate constant k < 0.1 h −1 ) and entered the Iowa River at elevated concentrations. Predicted and measured concentrations in the drinking water treatment plant were below the human health benchmarks. This study demonstrates the application of probabilistic risk assessments for effluent-derived CECs in a representative effluent-dominated stream under variable flow conditions (when measurements are less practical) and provides an enhanced prediction tool transferable to other effluent-dominated systems.

Iowa↗

Predicted aquatic exposure effects from a national urban stormwater study

A multi-agency study of 438 organic and 62 inorganic chemicals measured in urban stormwater during 50 total runoff events at 21 sites across the United States demonstrated that stormwater discharges can generate localized, aquatic exposures to extensive contaminant mixtures, including organics suspected to cause adverse aquatic-health effects. The aggregated risks to multiple aquatic trophic levels (fish, invertebrates, plants) of the stormwater mixture exposures, which were documented in the national study, were explored herein by calculating cumulative ratios of organic-contaminant in vitro exposure–activity cutoffs (∑ EAR ) and health-benchmark-weighted cumulative toxicity quotients (∑ TQ ). Both risk assessment approaches indicated substantial (moderate to high) risk for acute adverse effects to aquatic organisms across multiple trophic levels (fish, macroinvertebrates, non-vascular/vascular plants) at or near stormwater discharge points across the United States. The results are interpreted as potential orders of magnitude underestimates of actual aquatic risk in stormwater control wetlands or in the immediate vicinity of such discharges to surface-water receptors, because the 438 organic-compound analytical space assessed in this study is orders of magnitude less than the 350 000 parent compounds estimated to be in current commercial use globally and the incalculable chemical-space of potential metabolites and degradates.

Environmental Science: Water Research and Technolo↗

Biogeochemical and hydrologic synergy control mercury fate in an arid land river-reservoir system

Reservoirs in arid landscapes provide critical water storage and hydroelectric power but influence the transport and biogeochemical cycling of mercury (Hg). Improved management of reservoirs to mitigate the supply and uptake of bioavailable methylmercury (MeHg) in aquatic food webs will benefit from a mechanistic understanding of inorganic divalent Hg (Hg( II )) and MeHg fate within and downstream of reservoirs. Here, we quantified Hg( II ), MeHg, and other pertinent biogeochemical constituents in water (filtered and associated with particles) at high temporal resolution from 2016–2020. This was done (1) at inflow and outflow locations of three successive hydroelectric reservoirs (Snake River, Idaho, Oregon) and (2) vertically and longitudinally within the first reservoir (Brownlee Reservoir). Under spring high flow, upstream inputs of particulate Hg (Hg( II ) and MeHg) and filter-passing Hg( II ) to Brownlee Reservoir were governed by total suspended solids and dissolved organic matter, respectively. Under redox stratified conditions in summer, net MeHg formation in the meta- and hypolimnion of Brownlee reservoir yielded elevated filter-passing and particulate MeHg concentrations, the latter exceeding 500 ng g −1 on particles. Simultaneously, the organic matter content of particulates increased longitudinally in the reservoir (from 9–29%) and temporally with stratified duration. In late summer and fall, destratification mobilized MeHg from the upgradient metalimnion and the downgradient hypolimnion of Brownlee Reservoir, respectively, resulting in downstream export of elevated filter-passing MeHg and organic-rich particles enriched in MeHg (up to 43% MeHg). We document coupled biogeochemical and hydrologic processes that yield in-reservoir MeHg accumulation and MeHg export in water and particles, which impacts MeHg uptake in aquatic food webs within and downstream of reservoirs.

Environmental Science: Processes & Impacts↗

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↗