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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↗

USGS2013

Groundwater ages and mixing in the Piceance Basin natural gas province, Colorado

Reliably identifying the effects of energy development on groundwater quality can be difficult because baseline assessments of water quality completed before the onset of energy development are rare and because interactions between hydrocarbon reservoirs and aquifers can be complex, involving both natural and human processes. Groundwater age and mixing data can strengthen interpretations of monitoring data from those areas by providing better understanding of the groundwater flow systems. Chemical, isotopic, and age tracers were used to characterize groundwater ages and mixing with deeper saline water in three areas of the Piceance Basin natural gas province. The data revealed a complex array of groundwater ages (<10 to >50,000 years) and mixing patterns in the basin that helped explain concentrations and sources of methane in groundwater. Age and mixing data also can strengthen the design of monitoring programs by providing information on time scales at which water quality changes in aquifers might be expected to occur. This information could be used to establish maximum allowable distances of monitoring wells from energy development activity and the appropriate duration of monitoring.

Colorado↗

USGS2013

A scenario and forecast model for Gulf of Mexico hypoxic area and volume

For almost three decades, the relative size of the hypoxic region on the Louisiana-Texas continental shelf has drawn scientific and policy attention. During that time, both simple and complex models have been used to explore hypoxia dynamics and to provide management guidance relating the size of the hypoxic zone to key drivers. Throughout much of that development, analyses had to accommodate an apparent change in hypoxic sensitivity to loads and often cull observations due to anomalous meteorological conditions. Here, we describe an adaptation of our earlier, simple biophysical model, calibrated to revised hypoxic area estimates and new hypoxic volume estimates through Bayesian estimation. This application eliminates the need to cull observations and provides revised hypoxic extent estimates with uncertainties, corresponding to different nutrient loading reduction scenarios. We compare guidance from this model application, suggesting an approximately 62% nutrient loading reduction is required to reduce Gulf hypoxia to the Action Plan goal of 5,000 km 2 , to that of previous applications. In addition, we describe for the first time, the corresponding response of hypoxic volume. We also analyze model results to test for increasing system sensitivity to hypoxia formation, but find no strong evidence of such change.

Environmental Science & Technology↗

USGS2014

Processes of zinc attenuation by biogenic manganese oxides forming in the hyporheic zone of Pinal Creek, Arizona

The distribution and speciation of Zn sorbed to biogenic Mn oxides forming in the hyporheic zone of Pinal Creek, AZ, was investigated using extended X-ray absorption fine structure (EXAFS) and microfocused synchrotron X-ray fluorescence (μSXRF) mapping, and chemical extraction. μSXRF and chemical extractions show that contaminant Zn co-varied with Mn in streambed sediment grain coatings. Bulk and microfocused EXAFS spectra of Zn in the biogenic Mn oxide coating are indicative of Zn forming triple-corner-sharing inner-sphere complexes over octahedral vacancies in the Mn oxide sheet structure. Zn desorbed in response to the decrease in pH in batch experiments and resulted in near-equal dissolved Zn at each pH over a 10-fold range in the solid/solution ratio. The geometry of sorbed Zn was unchanged after 50% desorption at pH 5, indicating that desorption is not controlled by dissolution of secondary Zn phases. In summary, these findings support the idea that Zn attenuation in Pinal Creek is largely controlled by sorption to microbial Mn oxides forming in the streambed during hyporheic exchange. Sorption to biogenic Mn oxides is likely an important process of Zn attenuation in circum-neutral pH reaches of many acid-mine drainage contaminated streams when dissolved Mn is present.

Arizona↗

USGS2013

Comprehensive assessment of hormones, phytoestrogens, and estrogenic activity in an anaerobic swine waste lagoon

In this study, the distribution of steroid hormones, phytoestrogens, and estrogenic activity was thoroughly characterized within the anaerobic waste lagoon of a typical commercial swine sow operation. Three independent rounds of sampling were conducted in June 2009, April 2010, and February 2011. Thirty-seven analytes in lagoon slurry and sludge were assessed using LC/MS-MS, and yeast estrogen screen was used to determine estrogenic activity. Of the hormone analytes, steroidal estrogens were more abundant than androgens or progesterone, with estrone being the predominant estrogen species. Conjugated hormones were detected only at low levels. The isoflavone metabolite equol was by far the predominant phytoestrogen species, with daidzein, genistein, formononetin, and coumestrol present at lower levels. Phytoestrogens were often more abundant than steroidal estrogens, but contributed minimally towards total estrogenic activity. Analytes were significantly elevated in the solid phases of the lagoon; although low observed log KOC values suggest enhanced solubility in the aqueous phase, perhaps due to dissolved or colloidal organic carbon. The association with the solid phase, as well as recalcitrance of analytes to anaerobic degradation, results in a markedly elevated load of analytes and estrogenic activity within lagoon sludge. Overall, findings emphasize the importance of adsorption and transformation processes in governing the fate of these compounds in lagoon waste, which is ultimately used for broadcast application as a fertilizer.

Environmental Science & Technology↗

USGS2013

Microbiological reduction of Sb(V) in anoxic freshwater sediments

Microbiological reduction of millimolar concentrations of Sb(V) to Sb(III) was observed in anoxic sediments from two freshwater settings: (1) a Sb- and As-contaminated mine site (Stibnite Mine) in central Idaho and 2) an uncontaminated suburban lake (Searsville Lake) in the San Francisco Bay Area. Rates of Sb(V) reduction in anoxic sediment microcosms and enrichment cultures were enhanced by amendment with lactate or acetate as electron donors but not by H2, and no reduction occurred in sterilized controls. Addition of 2- 14 C-acetate to Stibnite Mine microcosms resulted in the production of 14 CO 2 coupled to Sb(V) reduction, suggesting that this process proceeds by a dissimilatory respiratory pathway in those sediments. Antimony(V) reduction in Searsville Lake sediments was not coupled to acetate mineralization and may be associated with Sb-resistance. The microcosms and enrichment cultures also reduced sulfate, and the precipitation of insoluble Sb(III)-sulfide complexes was a major sink for reduced Sb. The reduction of Sb(V) by Stibnite Mine sediments was inhibited by As(V), suggesting that As(V) is a preferred electron acceptor for the indigenous community. These findings indicate a novel pathway for anaerobic microbiological respiration and suggest that communities capable of reducing high concentrations of Sb(V) commonly occur naturally in the environment.

Environmental Science & Technology↗

USGS2013

Probabilistic analysis showing that a combination of bacteroides and methanobrevibacter source tracking markers is effective for identifying waters contaminated by human fecal pollution

Microbial source tracking assays to identify sources of waterborne contamination typically target genetic markers of host-specific microorganisms. However, no bacterial marker has been shown to be 100% host-specific, and cross-reactivity has been noted in studies evaluating known source samples. Using 485 challenge samples from 20 different human and animal fecal sources, this study evaluated microbial source tracking markers including the Bacteroides HF183 16S rRNA, M. smithii nifH, and Enterococcus esp gene targets that have been proposed as potential indicators of human fecal contamination. Bayes' Theorem was used to calculate the conditional probability that these markers or a combination of markers can correctly identify human sources of fecal pollution. All three human-associated markers were detected in 100% of the sewage samples analyzed. Bacteroides HF183 was the most effective marker for determining whether contamination was specifically from a human source, and greater than 98% certainty that contamination was from a human source was shown when both Bacteroides HF183 and M. smithii nifH markers were present. A high degree of certainty was attained even in cases where the prior probability of human fecal contamination was as low as 8.5%. The combination of Bacteroides HF183 and M. smithii nifH source tracking markers can help identify surface waters impacted by human fecal contamination, information useful for prioritizing restoration activities or assessing health risks from exposure to contaminated waters.

Environmental Science & Technology↗

USGS2014

Transcriptomic effects-based monitoring for endocrine active chemicals: Assessing relative contribution of treated wastewater to downstream pollution

The present study investigated whether a combination of targeted analytical chemistry information with unsupervised, data-rich biological methodology (i.e., transcriptomics) could be utilized to evaluate relative contributions of wastewater treatment plant (WWTP) effluents to biological effects. The effects of WWTP effluents on fish exposed to ambient, receiving waters were studied at three locations with distinct WWTP and watershed characteristics. At each location, 4 d exposures of male fathead minnows to the WWTP effluent and upstream and downstream ambient waters were conducted. Transcriptomic analyses were performed on livers using 15 000 feature microarrays, followed by a canonical pathway and gene set enrichment analyses. Enrichment of gene sets indicative of teleost brain–pituitary–gonadal–hepatic (BPGH) axis function indicated that WWTPs serve as an important source of endocrine active chemicals (EACs) that affect the BPGH axis (e.g., cholesterol and steroid metabolism were altered). The results indicated that transcriptomics may even pinpoint pertinent adverse outcomes (i.e., liver vacuolization) and groups of chemicals that preselected chemical analytes may miss. Transcriptomic Effects-Based monitoring was capable of distinguishing sites, and it reflected chemical pollution gradients, thus holding promise for assessment of relative contributions of point sources to pollution and the efficacy of pollution remediation.

Environmental Science & Technology↗

USGS2013

Trophic shift, not collapse

Jerald Schnoor’s editorial describes the recent changes in Lake Huron’s aquatic ecosystem as a trophic collapse and attributes this collapse to invasive species dominating energy and nutrient ﬂows in the food web. As state and federal scientists who are closely monitoring Lake Huron’s food web, we believe that the ongoing changes are more accurately characterized as a trophic shift in which benthic pathways have become more prominent. While decreases in abundance have occurred for some species, others are experiencing improved reproduction resulting in the restoration of several important native species.

Environmental Science & Technology↗

USGS2014

A spatial modeling framework to evaluate domestic biofuel-induced potential land use changed and emissions

We present a novel bottom-up approach to estimate biofuel-induced land-use change (LUC) and resulting CO 2 emissions in the U.S. from 2010 to 2022, based on a consistent methodology across four essential components: land availability, land suitability, LUC decision-making, and induced CO 2 emissions. Using high-resolution geospatial data and modeling, we construct probabilistic assessments of county-, state-, and national-level LUC and emissions for macroeconomic scenarios. We use the Cropland Data Layer and the Protected Areas Database to characterize availability of land for biofuel crop cultivation, and the CERES-Maize and BioCro biophysical crop growth models to estimate the suitability (yield potential) of available lands for biofuel crops. For LUC decisionmaking, we use a county-level stochastic partial-equilibrium modeling framework and consider five scenarios involving annual ethanol production scaling to 15, 22, and 29 BG, respectively, in 2022, with corn providing feedstock for the first 15 BG and the remainder coming from one of two dedicated energy crops. Finally, we derive high-resolution above-ground carbon factors from the National Biomass and Carbon Data set to estimate emissions from each LUC pathway. Based on these inputs, we obtain estimates for average total LUC emissions of 6.1, 2.2, 1.0, 2.2, and 2.4 gCO2e/MJ for Corn-15 Billion gallons (BG), Miscanthus × giganteus (MxG)-7 BG, Switchgrass (SG)-7 BG, MxG-14 BG, and SG-14 BG scenarios, respectively.

Environmental Science & Technology↗