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USGS2013

Vulnerability of streams to legacy nitrate sources

The influence of hydrogeologic setting on the susceptibility of streams to legacy nitrate was examined at seven study sites having a wide range of base flow index (BFI) values. BFI is the ratio of base flow to total streamflow volume. The portion of annual stream nitrate loads from base flow was strongly correlated with BFI. Furthermore, dissolved oxygen concentrations in streambed pore water were significantly higher in high BFI watersheds than in low BFI watersheds suggesting that geochemical conditions favor nitrate transport through the bed when BFI is high. Results from a groundwater-surface water interaction study at a high BFI watershed indicate that decades old nitrate-laden water is discharging to this stream. These findings indicate that high nitrate levels in this stream may be sustained for decades to come regardless of current practices. It is hypothesized that a first approximation of stream vulnerability to legacy nutrients may be made by geospatial analysis of watersheds with high nitrogen inputs and a strong connection to groundwater (e.g., high BFI).

Indiana;Maryl;Nebraska;North Carolina;Washington;W↗

USGS2013

Emergence flux declines disproportionately to larval density along a stream metals gradient

Effects of contaminants on adult aquatic insect emergence are less well understood than effects on insect larvae. We compared responses of larval density and adult emergence along a metal contamination gradient. Nonlinear threshold responses were generally observed for larvae and emergers. Larval densities decreased significantly at low metal concentrations but precipitously at concentrations of metal mixtures above aquatic life criteria (Cumulative Criterion Accumulation Ratio (CCAR) ≥ 1). In contrast, adult emergence declined precipitously at low metal concentrations (CCAR ≤ 1), followed by a modest decline above this threshold. Adult emergence was a more sensitive indicator of the effect of low metals concentrations on aquatic insect communities compared to larvae, presumably because emergence is limited by a combination of larval survival and other factors limiting successful emergence. Thus effects of exposure to larvae are not manifest until later in life (during metamorphosis and emergence). This loss in emergence reduces prey subsidies to riparian communities at concentrations considered safe for aquatic life. Our results also challenge the widely held assumption that adult emergence is a constant proportion of larval densities in all streams.

Environmental Science & Technology↗

USGS2013

Novel and non-traditional use of stable isotope tracers to study metal bioavailability from natural particles

We devised a novel tracing approach that involves enriching test organisms with a stable metal isotope of low natural abundance prior to characterizing metal bioavailability from natural inorganic particles. In addition to circumventing uncertainties associated with labeling natural particles and distinguishing background metals, the proposed "reverse labeling" technique overcomes many drawbacks inherent to using radioisotope tracers. Specifically, we chronically exposed freshwater snails (Lymnaea stagnalis) to synthetic water spiked with Cu that was 99.4% 65 Cu to increase the relative abundance of 65 Cu in the snail’s tissues from 32% to >80%. The isotopically enriched snails were then exposed to benthic algae mixed with Cu-bearing Fe–Al particles collected from the Animas River (Colorado), an acid mine drainage impacted river. We used 63 Cu to trace Cu uptake from the natural particles and inferred their bioavailability from calculation of Cu assimilation into tissues. Cu assimilation from these particles was 44%, indicating that 44% of the particulate Cu was absorbed by the invertebrate. This demonstrates that inorganic particulate Cu can be bioavailable. The reverse labeling approach shows great potential in various scientific areas such as environmental contamination and nutrition for addressing questions involving uptake of an element that naturally has multiple isotopes.

Environmental Science & Technology↗

USGS2013

Uranium(VI) interactions with mackinawite in the presence and absence of bicarbonate and oxygen

Mackinawite, Fe(II)S, samples loaded with uranium (10 -5 , 10 -4 , and 10 -3 mol U/g FeS) at pH 5, 7, and 9, were characterized using X-ray absorption spectroscopy and X-ray diffraction to determine the effects of pH, bicarbonate, and oxidation on uptake. Under anoxic conditions, a 5 g/L suspension of mackinawite lowered 5 × 10 -5 M uranium(VI) to below 30 ppb (1.26 × 10 -7 M) U. Between 82 and 88% of the uranium removed from solution by mackinawite was U(IV) and was nearly completely reduced to U(IV) when 0.012 M bicarbonate was added. Near-neighbor coordination consisting of uranium–oxygen and uranium-uranium distances indicates the formation of uraninite in the presence and absence of bicarbonate, suggesting reductive precipitation as the dominant removal mechanism. Following equilibration in air, mackinawite was oxidized to mainly goethite and sulfur and about 76% of U(IV) was reoxidized to U(VI) with coordination of uranium to axial and equatorial oxygen, similar to uranyl. Additionally, uranium-iron distances, typical of coprecipitation of uranium with iron oxides, and uranium-sulfur distances indicating bidentate coordination of U(VI) to sulfate were evident. The affinity of mackinawite and its oxidation products for U(VI) provides impetus for further study of mackinawite as a potential reactive medium for remediation of uranium-contaminated water.

Environmental Science & Technology↗

USGS2013

Increases in dissolved organic carbon accelerate loss of toxic Al in Adirondack lakes recovering from acidification

Increasing pH and decreasing Al in surface waters recovering from acidification have been accompanied by increasing concentrations of dissolved organic carbon (DOC) and associated organic acids that partially offset pH increases and complicate assessments of recovery from acidification. To better understand the processes of recovery, monthly chemistry from 42 lakes in the Adirondack region, NY, collected from 1994 to 2011, were used to (1) evaluate long-term changes in DOC and associated strongly acidic organic acids and (2) use the base-cation surplus (BCS) as a chemical index to assess the effects of increasing DOC concentrations on the Al chemistry of these lakes. Over the study period, the BCS increased (p < 0.01) and concentrations of toxic inorganic monomeric Al (IMAl) decreased (p < 0.01). The decreases in IMAl were greater than expected from the increases in the BCS. Higher DOC concentrations that increased organic complexation of Al resulted in a decrease in the IMAl fraction of total monomeric Al from 57% in 1994 to 23% in 2011. Increasing DOC concentrations have accelerated recovery in terms of decreasing toxic Al beyond that directly accomplished by reducing atmospheric deposition of strong mineral acids.

Environmental Science & Technology↗

USGS2013

Source and transport of human enteric viruses in deep municipal water supply wells

Until recently, few water utilities or researchers were aware of possible virus presence in deep aquifers and wells. During 2008 and 2009 we collected a time series of virus samples from six deep municipal water-supply wells. The wells range in depth from approximately 220 to 300 m and draw water from a sandstone aquifer. Three of these wells draw water from beneath a regional aquitard, and three draw water from both above and below the aquitard. We also sampled a local lake and untreated sewage as potential virus sources. Viruses were detected up to 61% of the time in each well sampled, and many groundwater samples were positive for virus infectivity. Lake samples contained viruses over 75% of the time. Virus concentrations and serotypes observed varied markedly with time in all samples. Sewage samples were all extremely high in virus concentration. Virus serotypes detected in sewage and groundwater were temporally correlated, suggesting very rapid virus transport, on the order of weeks, from the source(s) to wells. Adenovirus and enterovirus levels in the wells were associated with precipitation events. The most likely source of the viruses in the wells was leakage of untreated sewage from sanitary sewer pipes.

Wisconsin↗

USGS2013

Sorption of pure N 2 O to biochars and other organic and inorganic materials under anhydrous conditions

Suppression of nitrous oxide (N 2 O) emissions from soil is commonly observed after amendment with biochar. The mechanisms accounting for this suppression are not yet understood. One possible contributing mechanism is N 2 O sorption to biochar. The sorption of N 2 O and carbon dioxide (CO 2 ) to four biochars was measured in an anhydrous system with pure N 2 O. The biochar data were compared to those for two activated carbons and other components potentially present in soils—uncharred pine wood and peat—and five inorganic metal oxides with variable surface areas. Langmuir maximum sorption capacities ( Q max ) for N 2 O on the pine wood biochars (generated between 250 and 500 °C) and activated carbons were 17–73 cm 3 g –1 at 20 °C (median 51 cm 3 g –1 ), with Langmuir affinities ( b ) of 2–5 atm –1 (median 3.4 atm –1 ). Both Q max and b of the charred materials were substantially higher than those for peat, uncharred wood, and metal oxides [ Q max 1–34 cm 3 g –1 (median 7 cm 3 g –1 ); b 0.4–1.7 atm –1 (median 0.7 atm –1 )]. This indicates that biochar can bind N 2 O more strongly than both mineral and organic soil materials. Q max and b for CO 2 were comparable to those for N 2 O. Modeled sorption coefficients obtained with an independent polyparameter—linear free-energy relationship matched measured data within a factor 2 for mineral surfaces but underestimated by a factor of 5–24 for biochar and carbonaceous surfaces. Isosteric enthalpies of sorption of N 2 O were mostly between −20 and −30 kJ mol –1 , slightly more exothermic than enthalpies of condensation (−16.1 kJ mol –1 ). Q max of N 2 O on biochar (50000–130000 μg g –1 biochar at 20 °C) exceeded the N 2 O emission suppressions observed in the literature (range 0.5–960 μg g –1 biochar; median 16 μg g –1 ) by several orders of magnitude. Thus, the hypothesis could not be falsified that sorption of N 2 O to biochar is a mechanism of N 2 O emission suppression.

Environmental Science & Technology↗

USGS2013

Marsh wrens as bioindicators of mercury in wetlands of Great Salt Lake: do blood and feathers reflect site-specific exposure risk to bird reproduction?

Nonlethal sampling of bird blood and feathers are among the more common ways of estimating the risk of mercury exposure to songbird reproduction. The implicit assumption is that mercury concentrations in blood or feathers of individuals captured in a given area are correlated with mercury concentrations in eggs from the same area. Yet, this assumption is rarely tested. We evaluated mercury concentrations in blood, feathers, and eggs of marsh wrens in wetlands of Great Salt Lake, Utah, and, at two spatial scales, specifically tested the assumption that mercury concentrations in blood and feather samples from birds captured in a defined area were predictive of mercury concentrations in eggs collected in the same area. Mercury concentrations in blood were not correlated with mercury concentrations in eggs collected within the same wetland unit, and were poorly correlated with mercury concentrations in eggs collected at the smaller home range spatial scale of analysis. Moreover, mercury exposure risk, as estimated via tissue concentrations, differed among wetland units depending upon whether blood or egg mercury concentrations were sampled. Mercury concentrations in feathers also were uncorrelated with mercury concentrations in eggs, and were poorly correlated with mercury concentrations in blood. These results demonstrate the potential for contrasting management actions that may be implemented based solely on the specific avian tissue that is sampled, and highlight the importance of developing avian tissues as biomonitoring tools for assessing local risk of mercury exposure to bird reproduction.

Environmental Science & Technology↗

USGS2013

Quantifying groundwater’s role in delaying improvements to Chesapeake Bay water quality

A study has been undertaken to determine the time required for the effects of nitrogen-reducing best management practices (BMPs) implemented at the land surface to reach the Chesapeake Bay via groundwater transport to streams. To accomplish this, a nitrogen mass-balance regression (NMBR) model was developed and applied to seven watersheds on the Delmarva Peninsula. The model included the distribution of groundwater return times obtained from a regional groundwater-flow (GWF) model, the history of nitrogen application at the land surface over the last century, and parameters that account for denitrification. The model was (1) able to reproduce nitrate concentrations in streams and wells over time, including a recent decline in the rate at which concentrations have been increasing, and (2) used to forecast future nitrogen delivery from the Delmarva Peninsula to the Bay given different scenarios of nitrogen load reduction to the water table. The relatively deep porous aquifers of the Delmarva yield longer groundwater return times than those reported earlier for western parts of the Bay watershed. Accordingly, several decades will be required to see the full effects of current and future BMPs. The magnitude of this time lag is critical information for Chesapeake Bay watershed managers and stakeholders.

Delaware, Maryland↗

USGS2013

Evaluating chemical extraction techniques for the determination of uranium oxidation state in reduced aquifer sediments

Extraction techniques utilizing high pH and (bi)carbonate concentrations were evaluated for their efficacy in determining the oxidation state of uranium (U) in reduced sediments collected from Rifle, CO. Differences in dissolved concentrations between oxic and anoxic extractions have been proposed as a means to quantify the U(VI) and U(IV) content of sediments. An additional step was added to anoxic extractions using a strong anion exchange resin to separate dissolved U(IV) and U(VI). X-ray spectroscopy showed that U(IV) in the sediments was present as polymerized precipitates similar to uraninite and/or less ordered U(IV), referred to as non-uraninite U(IV) species associated with biomass (NUSAB). Extractions of sediment containing both uraninite and NUSAB displayed higher dissolved uranium concentrations under oxic than anoxic conditions while extractions of sediment dominated by NUSAB resulted in identical dissolved U concentrations. Dissolved U(IV) was rapidly oxidized under anoxic conditions in all experiments. Uraninite reacted minimally under anoxic conditions but thermodynamic calculations show that its propensity to oxidize is sensitive to solution chemistry and sediment mineralogy. A universal method for quantification of U(IV) and U(VI) in sediments has not yet been developed but the chemical extractions, when combined with solid-phase characterization, have a narrow range of applicability for sediments without U(VI).

Colorado↗

USGS2013

Kinetics of homogeneous and surface-catalyzed mercury(II) reduction by iron(II)

Production of elemental mercury, Hg(0), via Hg(II) reduction is an important pathway that should be considered when studying Hg fate in environment. We conducted a kinetic study of abiotic homogeneous and surface-catalyzed Hg(0) production by Fe(II) under dark anoxic conditions. Hg(0) production rate, from initial 50 pM Hg(II) concentration, increased with increasing pH (5.5–8.1) and aqueous Fe(II) concentration (0.1–1 mM). The homogeneous rate was best described by the expression, r hom = k hom [FeOH + ] [Hg(OH) 2 ]; k hom = 7.19 × 10 +3 L (mol min) −1 . Compared to the homogeneous case, goethite (α-FeOOH) and hematite (α-Fe 2 O 3 ) increased and γ-alumina (γ-Al 2 O 3 ) decreased the Hg(0) production rate. Heterogeneous Hg(0) production rates were well described by a model incorporating equilibrium Fe(II) adsorption, rate-limited Hg(II) reduction by dissolved and adsorbed Fe(II), and rate-limited Hg(II) adsorption. Equilibrium Fe(II) adsorption was described using a surface complexation model calibrated with previously published experimental data. The Hg(0) production rate was well described by the expression r het = k het [>SOFe (II) ] [Hg(OH) 2 ], where >SOFe (II) is the total adsorbed Fe(II) concentration; k het values were 5.36 × 10 +3 , 4.69 × 10 +3 , and 1.08 × 10 +2 L (mol min) −1 for hematite, goethite, and γ-alumina, respectively. Hg(0) production coupled to reduction by Fe(II) may be an important process to consider in ecosystem Hg studies.

Environmental Science & Technology↗

USGS2013

In situ spectrophotometric measurement of dissolved inorganic carbon in seawater

Autonomous in situ sensors are needed to document the effects of today’s rapid ocean uptake of atmospheric carbon dioxide (e.g., ocean acidification). General environmental conditions (e.g., biofouling, turbidity) and carbon-specific conditions (e.g., wide diel variations) present significant challenges to acquiring long-term measurements of dissolved inorganic carbon (DIC) with satisfactory accuracy and resolution. SEAS-DIC is a new in situ instrument designed to provide calibrated, high-frequency, long-term measurements of DIC in marine and fresh waters. Sample water is first acidified to convert all DIC to carbon dioxide (CO 2 ). The sample and a known reagent solution are then equilibrated across a gas-permeable membrane. Spectrophotometric measurement of reagent pH can thereby determine the sample DIC over a wide dynamic range, with inherent calibration provided by the pH indicator’s molecular characteristics. Field trials indicate that SEAS-DIC performs well in biofouling and turbid waters, with a DIC accuracy and precision of &sim;2 μmol kg –1 and a measurement rate of approximately once per minute. The acidic reagent protects the sensor cell from biofouling, and the gas-permeable membrane excludes particulates from the optical path. This instrument, the first spectrophotometric system capable of automated in situ DIC measurements, positions DIC to become a key parameter for in situ CO 2 -system characterizations.

Environmental Science & Technology↗

USGS2013

Effects of acidic deposition and soil acidification on sugar maple trees in the Adirondack Mountains, New York

We documented the effects of acidic atmospheric deposition and soil acidification on the canopy health, basal area increment, and regeneration of sugar maple (SM) trees across the Adirondack region of New York State, in the northeastern United States, where SM are plentiful but not well studied and where widespread depletion of soil calcium (Ca) has been documented. Sugar maple is a dominant canopy species in the Adirondack Mountain ecoregion, and it has a high demand for Ca. Trees in this region growing on soils with poor acid–base chemistry (low exchangeable Ca and % base saturation [BS]) that receive relatively high levels of atmospheric sulfur and nitrogen deposition exhibited a near absence of SM seedling regeneration and lower crown vigor compared with study plots with relatively high exchangeable Ca and BS and lower levels of acidic deposition. Basal area increment averaged over the 20th century was correlated (p < 0.1) with acid–base chemistry of the Oa, A, and upper B soil horizons. A lack of Adirondack SM regeneration, reduced canopy condition, and possibly decreased basal area growth over recent decades are associated with low concentrations of nutrient base cations in this region that has undergone soil Ca depletion from acidic deposition.

New York↗

USGS2013

Understanding water column and streambed thermal refugia for endangered mussels in the Delaware River

Groundwater discharge locations along the upper Delaware River, both discrete bank seeps and diffuse streambed upwelling, may create thermal niche environments that benefit the endangered dwarf wedgemussel (Alasmidonta heterodon). We seek to identify whether discrete or diffuse groundwater inflow is the dominant control on refugia. Numerous springs and seeps were identified at all locations where dwarf wedgemussels still can be found. Infrared imagery and custom high spatial resolution fiber-optic distributed temperature sensors reveal complex thermal dynamics at one of the seeps with a relatively stable, cold groundwater plume extending along the streambed/water-column interface during mid-summer. This plume, primarily fed by a discrete bank seep, was shown through analytical and numerical heat-transport modeling to dominate temperature dynamics in the region of potential habitation by the adult dwarf wedgemussel.

Pennsylvania↗

USGS2013

In-stream attenuation of neuro-active pharmaceuticals and their metabolites

In-stream attenuation was determined for 14 neuro-active pharmaceuticals and associated metabolites. Lagrangian sampling, which follows a parcel of water as it moves downstream, was used to link hydrological and chemical transformation processes. Wastewater loading of neuro-active compounds varied considerably over a span of several hours, and thus a sampling regime was used to verify that the Lagrangian parcel was being sampled and a mechanism was developed to correct measured concentrations if it was not. In-stream attenuation over the 5.4-km evaluated reach could be modeled as pseudo-first-order decay for 11 of the 14 evaluated neuro-active pharmaceutical compounds, illustrating the capacity of streams to reduce conveyance of neuro-active compounds downstream. Fluoxetine and N -desmethyl citalopram were the most rapidly attenuated compounds ( t 1/2 = 3.6 ± 0.3 h, 4.0 ± 0.2 h, respectively). Lamotrigine, 10,11,-dihydro-10,11,-dihydroxy-carbamazepine, and carbamazepine were the most persistent ( t 1/2 = 12 ± 2.0 h, 12 ± 2.6 h, 21 ± 4.5 h, respectively). Parent compounds (e.g., buproprion, carbamazepine, lamotrigine) generally were more persistent relative to their metabolites. Several compounds (citalopram, venlafaxine, O -desmethyl-venlafaxine) were not attenuated. It was postulated that the primary mechanism of removal for these compounds was interaction with bed sediments and stream biofilms, based on measured concentrations in stream biofilms and a column experiment using stream sediments.

Environmental Science & Technology↗

USGS2013

New Method for Electrical Conductivity Temperature Compensation

Electrical conductivity (κ) measurements of natural waters are typically referenced to 25 °C (κ 25 ) using standard temperature compensation factors (α). For acidic waters (pH < 4), this can result in a large κ 25 error (δκ 25 ). The more the sample temperature departs from 25 °C, the larger the potential δκ 25 . For pH < 4, the hydrogen ion transport number becomes substantial and its mode of transport is different from most other ions resulting in a different α. A new method for determining α as a function of pH and temperature is presented. Samples with varying amounts of H 2 SO 4 and NaCl were used to develop the new α, which was then applied to 65 natural water samples including acid mine waters, geothermal waters, seawater, and stream waters. For each sample, the κ and pH were measured at several temperatures from 5 to 90 °C and κ 25 was calculated. The δκ 25 ranged from −11 to 9% for the new method as compared to −42 to 25% and −53 to 27% for the constant α (0.019) and ISO-7888 methods, respectively. The new method for determining α is a substantial improvement for acidic waters and performs as well as or better than the standard methods for circumneutral waters.

Environmental Science & Technology↗

USGS2013

Geographic setting influences Great Lakes beach microbiological water quality

Understanding of factors that influence Escherichia coli (EC) and enterococci (ENT) concentrations, pathogen occurrence, and microbial sources at Great Lakes beaches comes largely from individual beach studies. Using 12 representative beaches, we tested enrichment cultures from 273 beach water and 22 tributary samples for EC, ENT, and genes indicating the bacterial pathogens Shiga-toxin producing E. coli (STEC), Shigella spp., Salmonella spp, Campylobacter jejuni/coli, and methicillin-resistant Staphylococcus aureus, and 108–145 samples for Bacteroides human, ruminant, and gull source-marker genes. EC/ENT temporal patterns, general Bacteroides concentration, and pathogen types and occurrence were regionally consistent (up to 40 km), but beach catchment variables (drains/creeks, impervious surface, urban land cover) influenced exceedances of EC/ENT standards and detections of Salmonella and STEC. Pathogen detections were more numerous when the EC/ENT Beach Action Value (but not when the Geometric Mean and Statistical Threshold Value) was exceeded. EC, ENT, and pathogens were not necessarily influenced by the same variables. Multiple Bacteroides sources, varying by date, occurred at every beach. Study of multiple beaches in different geographic settings provided new insights on the contrasting influences of regional and local variables, and a broader-scale perspective, on significance of EC/ENT exceedances, bacterial sources, and pathogen occurrence.

Great Lakes↗

USGS2013

Mercury speciation and mobilization in a wastewater-contaminated groundwater plume

We measured the concentration and speciation of mercury (Hg) in groundwater down-gradient from the site of wastewater infiltration beds operated by the Massachusetts Military Reservation, western Cape Cod, Massachusetts. Total mercury concentrations in oxic, mildly acidic, uncontaminated groundwater are 0.5–1 pM, and aquifer sediments have 0.5–1 ppb mercury. The plume of impacted groundwater created by the wastewater disposal is still evident, although inputs ceased in 1995, as indicated by anoxia extending at least 3 km down-gradient from the disposal site. Solutes indicative of a progression of anaerobic metabolisms are observed vertically and horizontally within the plume, with elevated nitrate concentrations and nitrate reduction surrounding a region with elevated iron concentrations indicating iron reduction. Mercury concentrations up to 800 pM were observed in shallow groundwater directly under the former infiltration beds, but concentrations decreased with depth and with distance down-gradient. Mercury speciation showed significant connections to the redox and metabolic state of the groundwater, with relatively little methylated Hg within the iron reducing sector of the plume, and dominance of this form within the higher nitrate/ammonium zone. Furthermore, substantial reduction of Hg(II) to Hg0 within the core of the anoxic zone was observed when iron reduction was evident. These trends not only provide insight into the biogeochemical factors controlling the interplay of Hg species in natural waters, but also support hypotheses that anoxia and eutrophication in groundwater facilitate the mobilization of natural and anthropogenic Hg from watersheds/aquifers, which can be transported down-gradient to freshwaters and the coastal zone.

Massachusetts↗