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At least 235 records · Page 13Linked to original sources

Assessing the lead solubility potential of untreated groundwater of the United States

In the U.S., about 44 million people rely on self-supplied groundwater for drinking water. Because most self-supplied homeowners do not treat their water to control corrosion, drinking water can be susceptible to lead (Pb) contamination from metal plumbing. To assess the types and locations of susceptible groundwater, a geochemical reaction model that included pure Pb minerals and solid solutions of calcite (Ca x Pb 1– x CO 3 ) and apatite [Ca x Pb 5-x (PO 4 ) 3 (OH; Cl; F)] was developed to estimate the lead solubility potential (LSP) for over 8300 untreated groundwater samples collected from domestic and public-supply sites between 2000 and 2016 in the U.S. The LSP is the calculated amount of Pb metal that could dissolve at 25 °C before a Pb-bearing mineral precipitates. About 33% of untreated groundwater samples had LSP greater than 15 μg/L—the USEPA action level for dissolved plus particulate forms of Pb. Five percent of samples had high LSP (above 300 μg/L) and tended to occur in the eastern and southeastern U.S. Measured Pb concentrations above 15 μg/L were rarely detected (<1%) but always coincided with high LSP values. Future work will provide a better understanding of the relation between water chemistry, Pb-mineral formation, and dissolved Pb concentrations in tap water.

Environmental Science & Technology

Reconnaissance of mixed organic and inorganic chemicals in private and public supply tapwaters at selected residential and workplace sites in the United States

Safe drinking water at the point-of-use (tapwater, TW) is a United States public health priority. Multiple lines of evidence were used to evaluate potential human health concerns of 482 organics and 19 inorganics in TW from 13 (7 public supply, 6 private well self-supply) home and 12 (public supply) workplace locations in 11 states. Only uranium (61.9 μg L –1 , private well) exceeded a National Primary Drinking Water Regulation maximum contaminant level (MCL: 30 μg L –1 ). Lead was detected in 23 samples (MCL goal: zero). Seventy-five organics were detected at least once, with median detections of 5 and 17 compounds in self-supply and public supply samples, respectively (corresponding maxima: 12 and 29). Disinfection byproducts predominated in public supply samples, comprising 21% of all detected and 6 of the 10 most frequently detected. Chemicals designed to be bioactive (26 pesticides, 10 pharmaceuticals) comprised 48% of detected organics. Site-specific cumulative exposure–activity ratios (∑ EAR ) were calculated for the 36 detected organics with ToxCast data. Because these detections are fractional indicators of a largely uncharacterized contaminant space, ∑ EAR in excess of 0.001 and 0.01 in 74 and 26% of public supply samples, respectively, provide an argument for prioritized assessment of cumulative effects to vulnerable populations from trace-level TW exposures.

Environmental Science & Technology

Cryptosporidium incidence and surface water influence of groundwater supplying public water systems in Minnesota, USA

Regulations for public water systems (PWS) in the U.S. consider Cryptosporidium a microbial contaminant of surface water supplies. Ground- water is assumed free of Cryptosporidium unless surface water is entering supply wells. We determined the incidence of Cryptosporidium in PWS wells varying in surface water influence. Community and noncommunity PWS wells (n = 145) were sampled (n = 964) and analyzed for Cryptosporidium by qPCR and immunofluorescence assay (IFA). Surface water influence was assessed by stable isotopes and the expert judgment of hydrogeologists using site-specific data. Fifty-eight wells (40%) and 107 samples (11%) were Cryptosporidium- positive by qPCR, and of these samples 67 were positive by IFA. Cryptosporidium concentrations measured by qPCR and IFA were significantly correlated (p < 0.001). Cryptosporidium incidence was not associated with surface water influence as assessed by stable isotopes or expert judgment. We successfully sequenced 45 of the 107 positive samples to identify species, including C. parvum (41), C. andersoni (2), and C. hominis (2), and the predominant subtype was C. parvum IIa A17G2R1. Assuming USA regulations for surface water-supplied PWS were applicable to the study wells, wells positive for Cryptosporidium by IFA would likely be required to add treatment. Cryptosporidium is not uncommon in groundwater, even when surface water influence is absent.

Minnesota

Hormones and pharmaceuticals in groundwater used as a source of drinking water across the United States

This is the first large-scale, systematic assessment of hormone and pharmaceutical occurrence in groundwater used for drinking across the United States. Samples from 1091 sites in Principal Aquifers representing 60% of the volume pumped for drinking-water supply had final data for 21 hormones and 103 pharmaceuticals. At least one compound was detected at 5.9% of 844 sites representing the resource used for public supply across the entirety of 15 Principal Aquifers, and at 11.3% of 247 sites representing the resource used for domestic supply over subareas of nine Principal Aquifers. Of 34 compounds detected, one plastics component (bisphenol A), three pharmaceuticals (carbamazepine, sulfamethoxazole, and meprobamate), and the caffeine degradate 1,7-dimethylxanthine were detected in more than 0.5% of samples. Hydrocortisone had a concentration greater than a human-health benchmark at 1 site. Compounds with high solubility and low K oc were most likely to be detected. Detections were most common in shallow wells with a component of recent recharge, particularly in crystalline-rock and mixed land-use settings. Results indicate vulnerability of groundwater used for drinking water in the U.S. to contamination by these compounds is generally limited, and exposure to these compounds at detected concentrations is unlikely to have adverse effects on human health.

Environmental Science & Technology

Integrated assessment of wastewater reuse, exposure risk, and fish endocrine disruption in the Shenandoah River watershed

Reuse of municipal and industrial wastewater treatment plant (WWTP) effluent is an important component in augmenting global freshwater supplies. The Shenandoah River Watershed was selected to conduct on-site exposure experiments to assess endocrine disrupting characteristics of different source waters. This investigation of the Shenandoah River Watershed integrates WWTP wastewater reuse modeling, hydrological and chemical characterization, and in vivo endocrine disruption bioassessment to assess contaminant sources, exposure pathways, and biological effects. The percentage of accumulated WWTP effluent in each river reach (ACCWW) was used to predict environmental concentrations for consumer product chemicals (boron), pharmaceutical compounds (carbamazepine), and steroidal estrogens (estrone, 17-beta-estradiol, estriol, and 17-alpha-ethinylestradiol). Fish endocrine disruption was evaluated using vitellogenin induction in male or juvenile fathead minnows. Water samples were analyzed for >500 inorganic and organic constituents to characterize the complex contaminant mixtures. Municipal ACCWW at drinking water treatment plant surface-water intakes ranged from <0.01 to 2.1 % under mean-annual streamflow and up to 4.7 % under August streamflow. Measured and predicted environmental concentrations resulted in 17-beta-estradiol equivalency quotients ranging from <0.05 to 5.1 ng L-1 indicating low-to-moderate risk of fish endocrine disruption. Results from the fish exposure experiments also showed limited estrogenic effects as indicated by the low (0.5- to 3.2-fold) vitellogenin induction.

Shenandoah River watershed

Geochemical factors controlling dissolved elemental mercury and methylmercury formation in Alaskan wetlands of varying trophic status

Transformations of aqueous inorganic divalent mercury (Hg(II)i) to volatile dissolved gaseous mercury (Hg(0)(aq)) and toxic methylmercury (MeHg) governs mercury bioavailability and fate in northern ecosystems. This study quantified concentrations of aqueous mercury species (Hg(II)i, Hg(0)(aq), MeHg) and relevant geochemical constituents in pore waters of eight Alaskan wetlands that differ in trophic status (i.e., bog-to-fen gradient) to gain insight on processes controlling dark Hg(II)i reduction and Hg(II)i methylation. Regardless of wetland trophic status, positive correlations were observed between pore water Hg(II)i and dissolved organic carbon (DOC) concentrations. The concentration ratio of Hg(0)(aq) to Hg(II)i exhibited an inverse relationship to Hg(II)i concentration. A ubiquitous pathway for Hg(0)(aq) formation was not identified based on geochemical data, but we surmise that dissolved organic matter (DOM) influences mercury retention in wetland pore waters by complexing Hg(II)i and decreasing the concentration of volatile Hg(0)(aq) relative to Hg(II)i. There was no evidence of Hg(0)(aq) abundance directly limiting mercury methylation. The concentration of MeHg relative to Hg(II)i was greatest in wetlands of intermediate trophic status, and geochemical data suggest mercury methylation pathways vary between wetlands. Our insights on geochemical factors influencing aqueous mercury speciation should be considered in context of the long-term fate of mercury in northern wetlands.

Environmental Science & Technology

Toxicokinetics of imidacloprid-coated wheat seeds in Japanese quail (Coturnix japonica) and an evaluation of hazard

Birds are potentially exposed to neonicotinoid insecticides by ingestion of coated seeds during crop planting. Adult male Japanese quail were orally dosed with wheat seeds coated with an imidacloprid (IMI) formulation at either 0.9 mg/kg body weight (BW) or 2.7 mg/kg BW (~3 and 9% of IMI LD50 for Japanese quail, respectively) for 1 or 10 days. Quail were euthanized between 1 and 24 h post-exposure to assess toxicokinetics. Analysis revealed rapid absorption (1 h) into blood, and distribution to brain, muscle, kidney and liver. Clearance to below detection limits occurred at both dose levels and exposure durations in all tissues within 24 h. Metabolism was extensive, with 5-OH-IMI and IMI-olefin detected at greater concentrations than IMI in tissues and fecal samples. There was no lethality or overt signs of toxicity at either dose level. Furthermore, no evidence of enhanced expression of mRNA genes associated with hepatic xenobiotic metabolism, oxidative DNA damage or alterations in concentrations of corticosterone and thyroid hormones was observed. Application of the toxicokinetic data was used to predict IMI residue levels in liver with reasonable results for some field exposure and avian mortality events. It would appear that some affected species are either consuming larger quantities of seeds or exhibit differences in ADME or sensitivity than predicted by read-across from these data.

Environmental Science & Technology

Mercury exposure and altered parental nesting behavior in a wild songbird

Methylmercury is a neurotoxin and endocrine disruptor and may impair avian reproduction directly through embryotoxicity or by altering parental care behaviors. We studied mercury exposure and incubation behavior of free-living tree swallows (Tachycineta bicolor) nesting in artificial nest boxes. Using small temperature dataloggers, we measured incubation constancy (the proportion of each day the female spent incubating eggs), the number of incubation recesses taken per day, and the duration of incubation recesses. We also assessed maternal mercury exposure by measuring mercury concentrations in both blood and eggs. Females with higher mercury concentrations exhibited lower incubation constancy, took more frequent and shorter incubation recesses, and were more likely to take incubation recesses that caused nest temperature decreases that were likely to slow embryonic development. Overall, females that laid eggs with the highest observed mercury concentration (0.53 μg/g fww) spent an average of 12% less time incubating their eggs over the 14-day incubation period than females that laid eggs with the lowest mercury concentration (0.07 μg/g fww). Because less time spent incubating can lower egg temperatures, slow embryonic development, and potentially lengthen the incubation period, these results suggest that environmentally relevant mercury concentrations may negatively influence reproduction by altering parental nesting behaviors of wild songbirds

Environmental Science & Technology

Kinetic study on clogging of a geothermal pumping well triggered by mixing-induced biogeochemical reactions

The sustainability of ground-source geothermal systems can be severely impacted by microbially mediated clogging processes. Biofouling of water wells by hydrous ferric oxide is a widespread problem. Although the mechanisms and critical environmental factors associated with clogging development are widely recognized, effects of mixing processes within the wells and time scales for clogging processes are not well characterized. Here we report insights from a joint hydrological, geochemical, and metagenomics characterization of a geothermal doublet in which hydrous ferric oxide and hydrous manganese oxide deposits had formed as a consequence of mixing shallow groundwater containing dissolved oxygen and nitrate with deeper, anoxic groundwater containing dissolved iron (Fe II ) and manganese (Mn II ). Metagenomics identify distinct bacteria consortia in the pumping well oxic and anoxic zones, including autotrophic iron-oxidizing bacteria. Batch mixing experiments and geochemical kinetics modeling of the associated reactions indicate that Fe II and Mn II oxidation are slow compared to the residence time of water in the pumping well; however, adsorption of Fe II and Mn II by accumulated hydrous ferric oxide and hydrous manganese oxide in the well bore and pump riser provides “infinite” time for surface-catalyzed oxidation and a convenient source of energy for iron-oxidizing bacteria, which colonize the surfaces and also catalyze oxidation. Thus, rapid clogging is caused by mixing-induced redox reactions and is exacerbated by microbial activity on accumulated hydrous oxide surfaces.

Orleans

Hydrocarbons in upland groundwater, Marcellus Shale Region, Northeastern Pennsylvania and Southern New York, USA

Water samples from 50 domestic wells located <1 km (proximal) and >1 km (distal) from shale-gas wells in upland areas of the Marcellus Shale region were analyzed for chemical, isotopic, and groundwater-age tracers. Uplands were targeted because natural mixing with brine and hydrocarbons from deep formations is less common in those areas compared to valleys. CH 4 -isotope, predrill CH 4 -concentration, and other data indicate that one proximal sample (5% of proximal samples) contains thermogenic CH 4 (2.6 mg/L) from a relatively shallow source (Catskill/Lock Haven Formations) that appears to have been mobilized by shale-gas production activities. Another proximal sample contains five other volatile hydrocarbons (0.03–0.4 μg/L), including benzene, more hydrocarbons than in any other sample. Modeled groundwater-age distributions, calibrated to 3 H, SF 6 , and 14 C concentrations, indicate that water in that sample recharged prior to shale-gas development, suggesting that land-surface releases associated with shale-gas production were not the source of those hydrocarbons, although subsurface leakage from a nearby gas well directly into the groundwater cannot be ruled out. Age distributions in the samples span ∼20 to >10000 years and have implications for relating occurrences of hydrocarbons in groundwater to land-surface releases associated with recent shale-gas production and for the time required to flush contaminants from the system.

New York, Pennsylvania

Occurrence and sources of radium in groundwater associated with oil fields in the southern San Joaquin Valley, California

Geochemical data from 40 water wells were used to examine the occurrence and sources of radium (Ra) in groundwater associated with three oil fields in California (Fruitvale, Lost Hills, South Belridge). 226Ra+228Ra activities (range=0.010-0.51 Bq/L) exceeded the 0.185 Bq/L drinking-water standard in 18% of the wells (not drinking-water wells). Radium activities were correlated with TDS concentrations (p<0.001, ρ=0.90, range=145-15,900 mg/L), Mn+Fe concentrations (p<0.001, ρ=0.82, range=<0.005-18.5 mg/L), and pH (p<0.001, ρ=-0.67, range=6.2-9.2), indicating Ra in groundwater was influenced by salinity, redox, and pH. Ra-rich groundwater was mixed with up to 45% oil-field water at some locations, primarily infiltrating through unlined disposal ponds, based on Cl, Li, noble-gas, and other data. Yet 228Ra/226Ra ratios in pond-impacted groundwater (median=3.1) differed from those in oil-field water (median=0.51). PHREEQC mixing calculations and spatial geochemical variations suggest the Ra in oil-field water was removed by co-precipitation with secondary barite and adsorption on Mn-Fe precipitates in the near-pond environment. The saline, organic-rich oil-field water subsequently mobilized Ra from downgradient aquifer sediments via Ra-desorption and Mn/Fe-reduction processes. This study demonstrates that infiltration of oil-field water may leach Ra into groundwater by changing salinity and redox conditions in the subsurface rather than by mixing with a high-Ra source.

California

Cell-Based metabolomics for untargeted screening and prioritization of vertebrate-active stressors in streams across the United States

The U.S. Geological Survey and the U.S. Environmental Protection Agency have assessed contaminants in 38 streams across the U.S., using an extensive suite of target-chemical analysis methods along with a variety of biological effects tools. Here we report zebrafish liver (ZFL) cell-culture based NMR metabolomic analysis of these split stream samples. We used this untargeted approach to evaluate the sites according to overall impact on the ZFL metabolome and found that neither the total number of organics detected at the sites, nor their cumulative concentrations, were good predictors of these impacts. Further, we used partial-least squares regression to compare ZFL endogenous metabolite profiles to values for 455 potential stressors (organics, inorganics, and physical properties) measured in these waters and found that the profiles covaried with at most 280 of the stressors, which were subsequently ranked into quartiles based on the strength of their covariance. While contaminants of emerging concern (CECs) were well represented in the top, most strongly, covarying quartile – suggesting considerable potential for eliciting biological responses at these sites – there was even higher representation of various well-characterized legacy contaminants (e.g., PCBs). These results emphasize the importance of complementing chemical analysis with untargeted bioassays to help focus regulatory efforts on the most significant ecosystem threats.

Environmental Science & Technology

Urban stormwater: An overlooked pathway of extensive mixed contaminants to surface and groundwaters in the United States

Increasing global reliance on stormwater control measures to reduce discharge to surface water, increase groundwater recharge, and minimize contaminant delivery to receiving waterbodies necessitates improved understanding of stormwater-contaminant profiles. A multi-agency study of organic and inorganic chemicals in urban stormwater from 50 runoff events at 21 sites across the United States demonstrated that stormwater transports substantial mixtures of polycyclic aromatic hydrocarbons, bioactive contaminants (pesticides and pharmaceuticals), and other organic chemicals known or suspected to pose environmental health concern. Numerous organic-chemical detections per site (median number of chemicals detected = 73), individual concentrations exceeding 10,000 ng/L, and cumulative concentrations up to 263,000 ng/L suggested concern for potential environmental effects during runoff events. Organic concentrations, loads, and yields were positively correlated with impervious surfaces and highly developed urban catchments. Episodic storm-event organic concentrations and loads were comparable to and often exceeded those of daily wastewater plant discharges. Inorganic chemical concentrations were generally dilute in concentration and did not exceed chronic aquatic life criteria. Methylmercury was measured in 90% of samples with concentrations that ranged from 0.05 to 1.0 ng/L.

Environmental Science & Technology

Predictive analysis using chemical-gene interaction networks consistent with observed endocrine activity and mutagenicity of U.S. streams

In a recent U.S. Geological Survey/U.S. Environmental Protection Agency study assessing >700 organic compounds in 38 streams, in vitro assays indicated generally low estrogen, androgen, and glucocorticoid receptor activities, but identified 13 surface waters with 17β estradiol equivalent (E2Eq) activities greater than the 1 ng/L level of concern for feminization of male fish. Among the 36 samples assayed for mutagenicity in the Salmonella bioassay (reported here), 25% were considered mutagenic (statistically significant slope and at least a two-fold increase in revertants/plate). Endocrine and mutagenic activities of the water samples were well correlated with each other and with the total number and cumulative concentrations of detected chemical contaminants. To test the predictive utility of knowledgebase-leveraging approaches, site-specific predicted chemical-gene (pCGA) and predicted analogous pathway-linked (pPLA) association networks identified in the Comparative Toxicogenomics Database were compared with observed endocrine/mutagenic bioactivities. We evaluated pCGA/pPLA patterns among sites by cluster analysis and principal component analysis and grouped the pPLA into broad mode-of-action classes. Measured E2Eq and mutagenic activities correlated well with predicted pathways. The pPLA analysis also revealed correlations with signaling, metabolic, and regulatory groups, suggesting that other effects pathways may be associated with chemical contaminants in these waters and indicating the need for broader bioassay coverage to assess potential adverse impacts.

Environmental Science & Technology

Chemical and physical controls on mercury source signatures in stream fish from the northeastern United States

Streams in the northeastern U.S. receive mercury (Hg) in varying proportions from atmospheric deposition and legacy point sources, making it difficult to attribute shifts in fish concentrations directly back to changes in Hg source management. Mercury stable isotope tracers were utilized to relate sources of Hg to co-located fish and bed sediments from 23 streams across a forested to urban-industrial land-use gradient within this region. Mass-dependent isotopes (δ202Hg) in prey and game fish at forested sites were depleted (medians -0.95 and -0.83 ‰, respectively) in comparison to fish from urban-industrial settings (medians -0.26 and -0.38 ‰, respectively); the forested site group also had higher prey fish Hg concentrations. The separation of Hg isotope signatures in fish was strongly related to in-stream and watershed land-use indicator variables. Fish isotopes were strongly correlated with bed sediment isotopes, but the comparison of isotopic composition between fish and sediment was variable due to differing ecosystem-specific drivers controlling the extent of MeHg formation. The multivariable approach of analyzing watershed characteristics and stream chemistry reveals that the Hg isotope composition in fish is linked to current and historic Hg sources in the northeastern U.S. and can be used to trace bioaccumulated Hg.

Environmental Science & Technology

Wintering in the western subarctic pacific increases mercury contamination of Red-legged Kittiwakes

Marine methylmercury concentrations vary geographically and with depth, exposing organisms to different mercury levels in unique habitats. Red-legged kittiwakes (Rissa brevirostris), a specialist predator, forage on fish and invertebrates from the mesopelagic zone, a part of the ocean with elevated methylmercury concentrations. We used kittiwakes as bioindicators of MeHg concentrations in remote mesopelagic systems by examining how wintering distribution and habitat affected kittiwakes’ mercury exposure. In 2011-2017, we sampled winter-grown feathers on St. George Island, Alaska, from birds equipped with geolocation loggers. We measured total mercury (THg) and nitrogen stable in nape and head feathers grown during winter, respectively. THg concentration of kittiwake nape feathers averaged 4.61 ± 0.97 µg/g dry weight. Hierarchical cluster analysis was used to classify winter habitats with remotely sensed environmental variables along each bird’s track. Five habitat clusters were identified. Birds that spent more time in the Western Subarctic Gyre and those that wintered further south had elevated THg concentrations. In contrast to THg, trophic level varied annually but did not show strong spatial patterns. Our results documented spatial variability in THg exposure based on the oceanic wintering locations of red-legged kittiwakes and highlight their use as a bioindicator of MeHg across ocean basins.

Alaska

Vertical distribution of microplastics in the water column and surficial sediment from the Milwaukee River basin to Lake Michigan

Microplastic contamination was studied along a freshwater continuum from inland streams to the Milwaukee River estuary to Lake Michigan, and vertically from the water surface, water subsurface and sediment. Microplastics were detected in all 96 water samples and nine sediment samples collected. Results indicated a gradient of polymer presence with depth: low-density particles decreased from water surface to subsurface to sediment, and high-density particles had the opposite result. Polymer identification results indicated water surface and subsurface samples were dominated by low-density polypropylene particles and sediment samples were dominated by more dense polyethylene terephthalate particles. Of the five particle-type categories (fragments, films, foams, pellets/beads and fibers/lines), fibers/lines were the most common particle type and were present in every water and sediment sample collected. Fibers represented 45% of all particles in water samples and were distributed vertically throughout the water column regardless of density. Sediment samples were dominated by black foams (66%, identified as styrene-butadiene rubber, SBR) and to a lesser extent fibers/lines (29%) with approximately 89% of all the sediment particles coming from polymers with densities greater than 1.1 g cm-3. Results demonstrated polymer density influenced partitioning between water surface and subsurface and the underlying surficial sediment and the common practice of sampling only the water surface can result in substantial bias, especially in estuarine, harbor and lake locations where water surface concentrations tend to overestimate mean water column concentrations.

Wisconsin

History and sources of co-occurring pesticides in an abstraction well unravelled by age distributions of depth specific groundwater samples

When groundwater-based drinking water supply becomes contaminated, the timing and source of contamination are obvious questions. However, contaminants often have diffuse sources and different contaminants may have different sources even in a single groundwater well, making these questions complicated to answer. Age dating of groundwater has been used to reconstruct contaminant travel times to wells; however, critics have highlighted that groundwater flow is often complex with mixing of groundwater of different ages. In drinking water wells, where water is typically abstracted from a large depth interval, such mixing is even more problematic. We present a way to overcome some of the obstacles in identifying the source and age of contaminants in drinking water wells by combining depth-specific sampling with age tracer modeling, particle tracking simulations, geological characterization, and contaminant properties. This multitool approach was applied to a drinking water well, where bentazon and dichlorprop contamination was found to have different pollutant sources and release histories, even though both pesticides can be associated with the same land use. Bentazon was derived from recent application to a golf course, while dichlorprop was derived from agricultural use more than 30 years ago. The advantages, limitations, and pitfalls of the proposed course of action are then further discussed.

Environmental Science & Technology