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At least 811 records · Page 45Linked to original sources
USGS2020

Factors affecting nitrate concentrations in stream base flow

Elevated nitrogen concentrations in streams and rivers in the Chesapeake Bay watershed have adversely affected the ecosystem health of the bay. Much of this nitrogen is derived as nitrate from groundwater that discharges to streams as base flow. In this study, boosted regression trees (BRTs) were used to relate nitrate concentrations in base flow ( n = 156) to explanatory variables describing nitrogen sources, geology, and soil and catchment characteristics. From these relations, a BRT model was developed to predict base flow nitrate concentrations in streams throughout the Chesapeake Bay watershed. The highest base flow nitrate concentrations were associated with intensive agricultural land use, carbonate geology, and sparse riparian canopy, which suggested that reduced nitrogen inputs, particularly over carbonate terrane, are critical for limiting nitrate concentrations. The lowest nitrate concentrations in the BRT model were associated with extensive riparian canopy, high levels of organic carbon in soils, and suboxic conditions at shallow depths, which suggested that denitrification in the subsurface, particularly in the riparian zone, is limiting base flow nitrate concentrations. Nitrate transport from aquifers to streams can take decades to occur, resulting in decades-long lag times between the time when a land-use activity is implemented and when its effects are fully observed in streams. Predictive models of base flow nitrate concentrations in streams will help identify which portions of a watershed are likely to have large fractions of total stream nitrogen load derived from pathways with significant lag times.

Delaware, Maryland, New York, North Carolina, Penn↗
USGS2020

Differences in neonicotinoid and metabolite sorption to activated carbon are driven by alterations to the insecticidal pharmacophore

Widespread application of neonicotinoids has led to their proliferation in waters. Despite low neonicotinoid hydrophobicity, our prior studies implicated granular activated carbon (GAC) in neonicotinoid removal. Based on known receptor binding characteristics, we hypothesized that the insecticidal pharmacophore influences neonicotinoid sorption. Our objectives were to illuminate drivers of neonicotinoid sorption for parent neonicotinoids (imidacloprid, clothianidin, thiamethoxam, and thiacloprid) and pharmacophore-altered metabolites (desnitro-imidacloprid and imidacloprid urea) to GAC, powdered activated carbon, and carbon nanotubes (CNTs). Neonicotinoid sorption to GAC was extensive and largely irreversible, with significantly greater sorption of imidacloprid than desnitro-imidacloprid. Imidacloprid and imidacloprid urea (electronegative pharmacophores) sorbed most extensively to nonfunctionalized CNTs, whereas desnitro-imidacloprid (positive pharmacophore) sorbed most to COOH-CNTs, indicating the importance of charge interactions and/or hydrogen bonding between the pharmacophore and carbon surface. Water chemistry parameters (temperature, alkalinity, ionic strength, and humic acid) inhibited overall neonicotinoid sorption, suggesting that pharmacophore-driven sorption in real waters may be diminished. Analysis of a full-scale drinking water treatment plant GAC filter influent, effluent, and spent GAC attributes neonicotinoid/metabolite removal to GAC under real-world conditions for the first time. Our results demonstrate that the neonicotinoid pharmacophore not only confers insecticide selectivity but also impacts sorption behavior, leading to less effective removal of metabolites by GAC filters in water treatment.

Environmental Science and Technology↗
USGS2021

Machine learning models of arsenic in private wells throughout the conterminous United States as a tool for exposure assessment in human health studies

Arsenic from geologic sources is widespread in groundwater within the United States (U.S.). In several areas, groundwater arsenic concentrations exceed the U.S. Environmental Protection Agency maximum contaminant level of 10 μg per liter (μg/L). However, this standard applies only to public-supply drinking water and not to private-supply, which is not federally regulated and is rarely monitored. As a result, arsenic exposure from private wells is a potentially substantial, but largely hidden, public health concern. Machine learning models using boosted regression trees (BRT) and random forest classification (RFC) techniques were developed to estimate probabilities and concentration ranges of arsenic in private wells throughout the conterminous U.S. Three BRT models were fit separately to estimate the probability of private well arsenic concentrations exceeding 1, 5, or 10 μg/L whereas the RFC model estimates the most probable category (≤5, >5 to ≤10, or >10 μg/L). Overall, the models perform best at identifying areas with low concentrations of arsenic in private wells. The BRT 10 μg/L model estimates for testing data have an overall accuracy of 91.2%, sensitivity of 33.9%, and specificity of 98.2%. Influential variables identified across all models included average annual precipitation and soil geochemistry. Models were developed in collaboration with public health experts to support U.S.-based studies focused on health effects from arsenic exposure.

Environmental Science and Technology↗
USGS2020

Effects-based monitoring of bioactive chemicals discharged to the Colorado River before and after a municipal wastewater treatment plant replacement

Monitoring of the Colorado River near the Moab, Utah, wastewater treatment plant (WWTP) outflow has detected pharmaceuticals, hormones, and estrogen-receptor (ER)-, glucocorticoid receptor (GR)-, and peroxisome proliferator-activated receptor-gamma (PPARγ)-mediated biological activities. The aim of the present multi-year study was to assess effects of a WWTP replacement on bioactive chemical (BC) concentrations. Water samples were collected bimonthly, pre- and post-replacement, at 11 sites along the Colorado River upstream and downstream of the WWTP and analyzed for in vitro bioactivities (e.g., agonism of ER, GR, and PPARγ) and BC concentrations; fathead minnows were cage deployed pre- and post-replacement at sites with varying proximities to the WWTP. Before the WWTP replacement, in vitro ER (24 ng 17β-estradiol equivalents/L)-, GR (60 ng dexamethasone equivalents/L)-, and PPARγ-mediated activities were detected at the WWTP outflow but diminished downstream. In March 2018, the WWTP effluent was acutely toxic to the fish, likely due to elevated ammonia concentrations. Following the WWTP replacement, ER, GR, and PPARγ bioactivities were reduced by approximately 60–79%, no toxicity was observed in caged fish, and there were marked decreases in concentrations of many BCs. Results suggest that replacement of the Moab WWTP achieved a significant reduction in BC concentrations to the Colorado River.

Utah↗
USGS2021

Widespread use of the nitrification inhibitor nitrapyrin: Assessing benefits and costs to agriculture, ecosystems, and environmental health

Agricultural production and associated applications of nitrogen (N) fertilizers have increased dramatically in the last century, and current projections to 2050 show that demands will continue to increase as the human population grows. Applied in both organic and inorganic fertilizer forms, N is an essential nutrient in crop productivity. Increased fertilizer applications, however, create the potential for more N loss before plant uptake. One strategy for minimizing N loss is the use of enhanced efficiency fertilizers, fortified with a nitrification inhibitor, such as nitrapyrin. In soils and water, nitrapyrin inhibits the activity of ammonia monooxygenase, a microbial enzyme that catalyzes the first step of nitrification from ammonium to nitrite. Potential benefits of using nitrification inhibitors range from reduced nitrate leaching and nitrous oxide emissions to increased crop yield. The extent of these benefits, however, depends on environmental conditions and management practices. Thus, such benefits are not always realized. Additionally, nitrapyrin has been shown to transport off-field, and it is unknown what effects environmental nitrapyrin could have on nontarget organisms and the ecological nitrogen cycle. Here, we review the agronomic and environmental benefits and costs of nitrapyrin use and present a series of research questions and considerations to be addressed with future nitrification inhibitor research.

Environmental Science and Technology↗
USGS2021

Temporal influences on selenium partitioning, trophic transfer, and exposure in a major U.S. river

Hydrologic and irrigation regimes mediate the timing of selenium (Se) mobilization to rivers, but the extent to which patterns in Se uptake and trophic transfer through recipient food webs reflect the temporal variation in Se delivery is unknown. We investigated Se mobilization, partitioning, and trophic transfer along approximately 60 river miles of the selenium-impaired segment of the Lower Gunnison River (Colorado, USA) during six sampling trips between June 2015 and October 2016. We found temporal patterns in Se partitioning and trophic transfer to be independent of those in dissolved Se concentrations and that the recipient food web sustained elevated Se concentrations from earlier periods of high Se mobilization. Using an ecosystem-scale Se accumulation model tailored to the Lower Gunnison River, we predicted that the endangered Razorback Sucker ( Xyrauchen texanus ) and Colorado Pikeminnow ( Ptychocheilus lucius ) achieve whole-body Se concentrations exceeding aquatic life protection criteria during periods of high runoff and irrigation activity (April–August) that coincide with susceptible phases of reproduction and early-life development. The results of this study challenge assumptions about Se trophodynamics in fast-flowing waters and introduce important considerations for the management of Se risks for biota in river ecosystems.

Colorado↗
USGS2021

Inclusion of pesticide transformation products is key to estimating pesticide exposures and effects in small U.S. streams

Improved analytical methods can quantify hundreds of pesticide transformation products (TPs), but understanding of TP occurrence and potential toxicity in aquatic ecosystems remains limited. We quantified 108 parent pesticides and 116 TPs in more than 3 700 samples from 442 small streams in mostly urban basins across five major regions of the United States. TPs were detected nearly as frequently as parents (90 and 95% of streams, respectively); 102 TPs were detected at least once and 28 were detected in >20% samples in at least one region—TPs of 9 herbicides, 2 fungicides (chlorothalonil and thiophanate-methyl), and 1 insecticide (fipronil) were the most frequently detected. TPs occurred commonly during baseflow conditions, indicating chronic environmental TP exposures to aquatic organisms and the likely importance of groundwater as a TP source. Hazard quotients based on acute aquatic-life benchmarks for invertebrates and nonvascular plants and vertebrate-centric molecular endpoints (sublethal effects) quantify the range of the potential contribution of TPs to environmental risk and highlight several TP exposure–response data gaps. A precautionary approach using equimolar substitution of parent benchmarks or endpoints for missing TP benchmarks indicates that potential aquatic effects of pesticide TPs could be underestimated by an order of magnitude or more.

Environmental Science and Technology↗
USGS2021

Insights on geochemical, isotopic, and volumetric compositions of produced water from hydraulically fractured Williston Basin oil wells

Tracing produced water origins from wells hydraulically fractured with freshwater-based fluids is sometimes predicated on assumptions that (1) each geological formation contains compositionally unique brine and (2) produced water from recently hydraulically fractured wells resembles fresher meteoric water more so than produced water from older wells. These assumptions are not valid in Williston Basin oil wells sampled in this study. Although distinct average 228 Ra/ 226 Ra ratios were found in water produced from the Bakken and Three Forks Formations, average δ 2 H, δ 18 O, specific gravity, and conductivity were similar but exhibited significant variability across five oil fields within each formation. Furthermore, initial produced water (“flowback”) was operationally defined based on the presence of glycol ether compounds and water from wells that had produced <56% of the amount of fluids injected and sampled within 160 days of fracturing. Flowback unexpectedly exhibited higher temperature, specific gravity, conductivity, δ 2 H, and δ 18 O, but lower oxidation–reduction potential and δ 11 B, relative to the wells thought to be producing formation brines (from wells with a produced-to-injected water ratio [PIWR] > 0.84 and sampled more than 316 days after fracturing). As such, establishing an overall geochemical and isotopic signature of produced water compositions based solely on chemical similarity to meteoric water and formation without the consideration of well treatments, well completion depth, or lateral location across the basin could be misleading if these signatures are assumed to be applicable across the entire basin. These findings have implications for using produced water compositions to understand the interbasin fluid flow and trace sources of hydraulic fracturing fluids.

Montana, North Dakota↗
USGS2022

Sediment sources and sealed-pavement area drive polycyclic aromatic hydrocarbon and metal occurrence in urban streams

Metals and polycyclic aromatic hydrocarbons (PAHs) are common pollutants in urban streambed sediment, yet their occurrence is highly variable and difficult to predict. To investigate sources of PAHs and metals to streambed sediment, we sampled pavement dust, soil, and streambed sediment in 10 urban watersheds in three regions of the United States and applied a fallout-radionuclide-based sediment-source analysis to quantify the pavement dust contribution to stream sediment (%dust). We also mapped the area of sealcoated pavement in each watershed (%sealed) to investigate the role of coal-tar pavement sealant (CTS) as a PAH source. Median total and carbon-normalized total PAH concentrations were significantly higher in streambed sediment in the Northeast (54.3 mg/kg and 2.71 mg/gOC) and Southeast (5.37 mg/kg and 1.36 mg/gOC), where CTS is commonly used, than in the Northwest (2.11 mg/kg and 0.071 mg/gOC), where CTS is rarely used. Generalized additive models indicated that %sealed and in some cases %dust significantly affected total PAH concentrations in streambed sediments. The %dust was a significant variable for common urban metals: Cu, Pb, and Zn. These findings advance our quantitative understanding of the role of pavement dust as a source and a vector of contaminants to urban streams.

Georgia, New York, North Carolina, Oregon, Virgini↗
USGS2021

Small mammal shooting as a conduit for lead exposure in avian scavengers

Lead (Pb) exposure is a widespread wildlife conservation threat. Although commonly associated with Pb-based ammunition from big-game hunting, small mammals (e.g., ground squirrels) shot for recreational or pest-management purposes represent a potentially important Pb vector in agricultural regions. We measured the responses of avian scavengers to pest-shooting events and examined their Pb exposure through consumption of shot mammals. There were 3.4-fold more avian scavengers at shooting fields relative to those at fields with no recent shooting, and avian scavengers spent 1.8-fold more time feeding after recent shooting events. We isotopically labeled shot ground squirrels in the field with an enriched 15N isotope tracer; 6% of avian scavengers sampled within a 39 km radius reflected this tracer in their blood. However, 33% of the avian scavengers within the average foraging dispersal distance of nests (0.6−3.7 km) were labeled, demonstrating the importance of these shooting fields as a source of food for birds nesting in close proximity. Additionally, Pb concentrations in 48% of avian scavengers exceeded subclinical poisoning benchmarks for sensitive species (0.03−0.20 μg/g w/w), and those birds exhibited reduced δ-aminolevulinic acid dehydratase activity, indicating a biochemical effect of Pb. The use of shooting to manage small mammal pests is a common practice globally. Efforts that can reduce the use of Pb-based ammunition may lessen the negative physiological effects of Pb exposure on avian scavengers.

Oregon↗
USGS2021

Enhanced susceptibility of methylmercury bioaccumulation into seston of the Laurentian Great Lakes

Mercury concentrations in the Laurentian Great Lakes waters are among the lowest reported in the literature, while game fish concentrations approach consumption advisory limits, particularly in Lakes Superior, Huron, and Michigan, indicating efficient methylmercury transfer from water to game fish. To determine if increased transfer efficiency is evident within the lower food web, we measured (2010–2018) mercury and dissolved organic carbon (DOC) in water, and in size-sieved seston, dietary tracers (carbon and nitrogen isotope ratios), phytoplankton methylmercury bioaccumulation, and methylmercury biomagnification between increasing seston size fractions. We observed consistently low filter-passing methylmercury (<0.010 ng L –1 ) and comparatively variable DOC (1.1 to 3.4 mg L –1 ) concentrations. Methylmercury biomagnification factors between size-sieved seston were similar between lakes. Bioaccumulation factors in phytoplankton were among the highest in the literature (log 5.5 to 6.1), exceeding those in oceans, smaller lakes, and streams, and was influenced by DOC. Higher bioaccumulation rates increase the susceptibility of methylmercury accumulation into the food web. Because mercury is dominantly delivered to the Great Lakes through the atmosphere and the biota therein is highly susceptible to methylmercury uptake, we propose that the Laurentian Great Lakes are excellent sentinels to trace the success of efforts to decrease global mercury emissions (e.g., Minamata Treaty) in the future.

Environmental Science and Technology↗
USGS2021

Persistent nitrate in alpine waters with changing atmospheric deposition and warming trends

Nitrate concentrations in high-elevation lakes of the Colorado Front Range remain elevated despite declining trends in atmospherically deposited nitrate since 2000. The current source of this elevated nitrate in surface waters remains elusive, given shifts in additional nitrogen sources via glacial inputs and atmospheric ammonium deposition. We present the complete isotopic composition of nitrate (δ 15 N, δ 18 O, and Δ 17 O) from a suite of nitrate-bearing source waters collected during the summers of 2017–2018 from two alpine ecosystems to constrain the provenance of elevated nitrate in surface waters during the summer open-water season. The results indicate a consistent contribution of uncycled atmospheric nitrate throughout the summer (13–23%) to alpine lakes, despite seasonal changes in source water inputs. The balance of nitrate (as high as 87% in late summer) is likely from nitrate production within the catchment via nitrification of reduced nitrogen sources (e.g., thawed soil organic matter and ammonium deposition) and released with rock glacier meltwater. The role of microbially produced nitrate has become increasingly important over time based on historical surface water samples from the mid-90s to present, a trend coincident with increasing ammonium deposition to alpine systems.

Colorado↗
USGS2021

Optical properties of water for prediction of wastewater contamination, human-associated bacteria, and fecal indicator bacteria in surface water at three watershed scales

Relations between spectral absorbance and fluorescence properties of water and human-associated and fecal indicator bacteria were developed for facilitating field sensor applications to estimate wastewater contamination in waterways. Leaking wastewater conveyance infrastructure commonly contaminates receiving waters. Methods to quantify such contamination can be time consuming, expensive, and often nonspecific. Human-associated bacteria are wastewater specific but require discrete sampling and laboratory analyses, introducing latency. Human sewage has fluorescence and absorbance properties different than those of natural waters. To assist real-time field sensor development, this study investigated optical properties for use as surrogates for human-associated bacteria to estimate wastewater prevalence in environmental waters. Three spatial scales were studied: Eight watershed-scale sites, five subwatershed-scale sites, and 213 storm sewers and open channels within three small watersheds (small-scale sites) were sampled (996 total samples) for optical properties, human-associated bacteria, fecal indicator bacteria, and, for selected samples, human viruses. Regression analysis indicated that bacteria concentrations could be estimated by optical properties used in existing field sensors for watershed and subwatershed scales. Human virus occurrence increased with modeled human-associated bacteria concentration, providing confidence in these regressions as surrogates for wastewater contamination. Adequate regressions were not found for small-scale sites to reliably estimate bacteria concentrations likely due to inconsistent local sanitary sewer inputs.

Michigan, New York, Ohio, Wisconsin↗
USGS2021

Mercury isotope fractionation by internal demethylation and biomineralization reactions in seabirds: Implications for environmental mercury science

A prerequisite for environmental and toxicological applications of mercury (Hg) stable isotopes in wildlife and humans is quantifying the isotopic fractionation of biological reactions. Here, we measured stable Hg isotope values of relevant tissues of giant petrels ( Macronectes spp.). Isotopic data were interpreted with published HR-XANES spectroscopic data that document a stepwise transformation of methylmercury (MeHg) to Hg-tetraselenolate (Hg(Sec) 4 ) and mercury selenide (HgSe) (Sec = selenocysteine). By mathematical inversion of isotopic and spectroscopic data, identical δ 202 Hg values for MeHg (2.69 ± 0.04‰), Hg(Sec) 4 (−1.37 ± 0.06‰), and HgSe (0.18 ± 0.02‰) were determined in 23 tissues of eight birds from the Kerguelen Islands and Adélie Land (Antarctica). Isotopic differences in δ 202 Hg between MeHg and Hg(Sec) 4 (−4.1 ± 0.1‰) reflect mass-dependent fractionation from a kinetic isotope effect due to the MeHg → Hg(Sec) 4 demethylation reaction. Surprisingly, Hg(Sec) 4 and HgSe differed isotopically in δ 202 Hg (+1.6 ± 0.1‰) and mass-independent anomalies (i.e., changes in Δ 199 Hg of ≤0.3‰), consistent with equilibrium isotope effects of mass-dependent and nuclear volume fractionation from Hg(Sec) 4 → HgSe biomineralization. The invariance of species-specific δ 202 Hg values across tissues and individual birds reflects the kinetic lability of Hg-ligand bonds and tissue-specific redistribution of MeHg and inorganic Hg, likely as Hg(Sec) 4 . These observations provide fundamental information necessary to improve the interpretation of stable Hg isotope data and provoke a revisitation of processes governing isotopic fractionation in biota and toxicological risk assessment in wildlife.

Environmental Science and Technology↗
USGS2022

In situ enhancement and isotopic labeling of biogenic coalbed methane

Subsurface microbial (biogenic) methane production is an important part of the global carbon cycle that has resulted in natural gas accumulations in many coal beds worldwide. Laboratory studies suggest that complex carbon-containing nutrients (e.g., yeast or algae extract) can stimulate methane production, yet the effectiveness of these nutrients within coal beds is unknown. Here, we use downhole monitoring methods in combination with deuterated water (D 2 O) and a 200-liter injection of 0.1% yeast extract (YE) to stimulate and isotopically label newly generated methane. A total dissolved gas pressure sensor enabled real-time gas measurements (641 days preinjection and for 478 days postinjection). Downhole samples, collected with subsurface environmental samplers, indicate that methane increased 132% above preinjection levels based on isotopic labeling from D 2 O, 108% based on pressure readings, and 183% based on methane measurements 266 days postinjection. Demonstrating that YE enhances biogenic coalbed methane production in situ using multiple novel measurement methods has immediate implications for other field-scale biogenic methane investigations, including in situ methods to detect and track microbial activities related to the methanogenic turnover of recalcitrant carbon in the subsurface.

Montana↗
USGS2022

Nitrogen enrichment during soil organic matter burning and molecular evidence of maillard reactions

Wildfires in forested watersheds dramatically alter stored and labile soil organic matter (SOM) pools and the export of dissolved organic matter (DOM). Ecosystem recovery after wildfires depends on soil microbial communities and revegetation and therefore is limited by the availability of nutrients, such as nitrogen-containing and labile, water-soluble compounds. However, SOM byproducts produced at different wildfire intensities are poorly understood, leading to difficulties in assessing wildfire severity and predicting ecosystem recovery. In this work, water-extractable organic matter (WEOM) from laboratory microcosms of soil burned at discrete temperatures was characterized by ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry to study the impacts of fire temperature on SOM and DOM composition. The molecular composition derived from different burn temperatures indicated that nitrogen-containing byproducts were enriched with heating and composed of a wide range of aromatic features and oxidation states. Mass difference-based analysis also suggested that products formed during heating could be modeled using transformations along the Maillard reaction pathway. The enrichment of N-containing SOM and DOM at different soil burning intensities has important implications for ecosystem recovery and downstream water quality.

Environmental Science and Technology↗
USGS2022

Brief oil exposure reduces fitness in wild Gulf of Mexico mahi-mahi (Coryphaena hippurus)

The Deepwater Horizon (DWH) disaster released 3.19 million barrels of crude oil into the Gulf of Mexico (GOM) in 2010, overlapping the habitat of pelagic fish populations. Using mahi-mahi ( Coryphaena hippurus )─a highly migratory marine teleost present in the GOM during the spill─as a model species, laboratory experiments demonstrate injuries to physiology and behavior following oil exposure. However, more than a decade postspill, impacts on wild populations remain unknown. To address this gap, we exposed wild mahi-mahi to crude oil or control conditions onboard a research vessel, collected fin clip samples, and tagged them with electronic tags prior to release into the GOM. We demonstrate profound effects on survival and reproduction in the wild. In addition to significant changes in gene expression profiles and predation mortality, we documented altered acceleration and habitat use in the first 8 days oil-exposed individuals were at liberty as well as a cessation of apparent spawning activity for at least 37 days. These data reveal that even a brief and low-dose exposure to crude oil impairs fitness in wild mahi-mahi. These findings offer new perspectives on the lasting impacts of the DWH blowout and provide insight about the impacts of future deep-sea oil spills.

Environmental Science and Technology↗