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USGS2015

High mercury wet deposition at a “clean Air” site in Puerto Rico

Atmospheric mercury deposition measurements are rare in tropical latitudes. Here we report on seven years (April 2005 to April 2012, with gaps) of wet Hg deposition measurements at a tropical wet forest in the Luquillo Mountains, northeastern Puerto Rico, U.S. Despite receiving unpolluted air off the Atlantic Ocean from northeasterly trade winds, during two complete years the site averaged 27.9 μg m –2 yr –1 wet Hg deposition, or about 30% more than Florida and the Gulf Coast, the highest deposition areas within the U.S. These high Hg deposition rates are driven in part by high rainfall, which averaged 2855 mm yr –1 . The volume-weighted mean Hg concentration was 9.8 ng L –1 , and was highest during summer and lowest during the winter dry season. Rainout of Hg (decreasing concentration with increasing rainfall depth) was minimal. The high Hg deposition was not supported by gaseous oxidized mercury (GOM) at ground level, which remained near global background concentrations (<10 pg m –3 ). Rather, a strong positive correlation between Hg concentrations and the maximum height of rain detected within clouds (echo tops) suggests that droplets in high convective cloud tops scavenge GOM from above the mixing layer. The high wet Hg deposition at this “clean air” site suggests that other tropical areas may be hotspots for Hg deposition as well.

Puerto Rico↗

USGS2015

Role of anaerobic ammonium oxidation (anammox) in nitrogen removal from a freshwater aquifer

Anaerobic ammonium oxidation (anammox) couples the oxidation of ammonium with the reduction of nitrite, producing N 2 . The presence and activity of anammox bacteria in groundwater were investigated at multiple locations in an aquifer variably affected by a large, wastewater-derived contaminant plume. Anammox bacteria were detected at all locations tested using 16S rRNA gene sequencing and quantification of hydrazine oxidoreductase ( hzo ) gene transcripts. Anammox and denitrification activities were quantified by in situ 15 NO 2 – tracer tests along anoxic flow paths in areas of varying ammonium, nitrate, and organic carbon abundances. Rates of denitrification and anammox were determined by quantifying changes in 28 N 2 , 29 N 2 , 30 N 2 , 15 NO 3 – , 15 NO 2 – , and 15 NH 4 + with groundwater travel time. Anammox was present and active in all areas tested, including where ammonium and dissolved organic carbon concentrations were low, but decreased in proportion to denitrification when acetate was added to increase available electron supply. Anammox contributed 39–90% of potential N 2 production in this aquifer, with rates on the order of 10 nmol N 2 –N L –1 day –1 . Although rates of both anammox and denitrification during the tracer tests were low, they were sufficient to reduce inorganic nitrogen concentrations substantially during the overall groundwater residence times in the aquifer. These results demonstrate that anammox activity in groundwater can rival that of denitrification and may need to be considered when assessing nitrogen mass transport and permanent loss of fixed nitrogen in aquifers.

Environmental Science & Technology↗

USGS2015

Formation of mercury sulfide from Hg(II)−thiolate complexes in natural organic matter

Methylmercury is the environmental form of neurotoxic mercury that is biomagnified in the food chain. Methylation rates are reduced when the metal is sequestered in crystalline mercury sulfides or bound to thiol groups in macromolecular natural organic matter. Mercury sulfide minerals are known to nucleate in anoxic zones, by reaction of the thiol-bound mercury with biogenic sulfide, but not in oxic environments. We present experimental evidence that mercury sulfide forms from thiol-bound mercury alone in aqueous dark systems in contact with air. The maximum amount of nanoparticulate mercury sulfide relative to thiol-bound mercury obtained by reacting dissolved mercury and soil organic matter matches that detected in the organic horizon of a contaminated soil situated downstream from Oak Ridge, TN, in the United States. The nearly identical ratios of the two forms of mercury in field and experimental systems suggest a common reaction mechanism for nucleating the mineral. We identified a chemical reaction mechanism that is thermodynamically favorable in which thiol-bound mercury polymerizes to mercury–sulfur clusters. The clusters form by elimination of sulfur from the thiol complexes via breaking of mercury–sulfur bonds as in an alkylation reaction. Addition of sulfide is not required. This nucleation mechanism provides one explanation for how mercury may be immobilized, and eventually sequestered, in oxygenated surface environments.

Environmental Science & Technology↗

USGS2015

Estimating mercury exposure of piscivorous birds and sport fish using prey fish monitoring

Methylmercury is a global pollutant of aquatic ecosystems, and monitoring programs need tools to predict mercury exposure of wildlife. We developed equations to estimate methylmercury exposure of piscivorous birds and sport fish using mercury concentrations in prey fish. We collected original data on western grebes ( Aechmophorus occidentalis ) and Clark’s grebes ( Aechmophorus clarkii ) and summarized the published literature to generate predictive equations specific to grebes and a general equation for piscivorous birds. We measured mercury concentrations in 354 grebes (blood averaged 1.06 ± 0.08 μg/g ww), 101 grebe eggs, 230 sport fish (predominantly largemouth bass and rainbow trout), and 505 prey fish (14 species) at 25 lakes throughout California. Mercury concentrations in grebe blood, grebe eggs, and sport fish were strongly related to mercury concentrations in prey fish among lakes. Each 1.0 μg/g dw (&sim;0.24 μg/g ww) increase in prey fish resulted in an increase in mercury concentrations of 103% in grebe blood, 92% in grebe eggs, and 116% in sport fish. We also found strong correlations between mercury concentrations in grebes and sport fish among lakes. Our results indicate that prey fish monitoring can be used to estimate mercury exposure of piscivorous birds and sport fish when wildlife cannot be directly sampled.

Environmental Science & Technology↗

USGS2015

Declining acidic deposition begins reversal of forest-soil acidification in the northeastern U.S. and eastern Canada

Decreasing trends in acidic deposition levels over the past several decades have led to partial chemical recovery of surface waters. However, depletion of soil Ca from acidic deposition has slowed surface water recovery and led to the impairment of both aquatic and terrestrial ecosystems. Nevertheless, documentation of acidic deposition effects on soils has been limited, and little is known regarding soil responses to ongoing acidic deposition decreases. In this study, resampling of soils in eastern Canada and the northeastern U.S. was done at 27 sites exposed to reductions in wet SO 4 2 – deposition of 5.7–76%, over intervals of 8–24 y. Decreases of exchangeable Al in the O horizon and increases in pH in the O and B horizons were seen at most sites. Among all sites, reductions in SO 4 2 – deposition were positively correlated with ratios (final sampling/initial sampling) of base saturation ( P < 0.01) and negatively correlated with exchangeable Al ratios ( P < 0.05) in the O horizon. However, base saturation in the B horizon decreased at one-third of the sites, with no increases. These results are unique in showing that the effects of acidic deposition on North American soils have begun to reverse.

Environmental Science & Technology↗

USGS2015

Tracing the cycling and fate of the explosive 2,4,6-trinitrotoluene in coastal marine systems with a stable isotopic tracer, 15N-[TNT]

2,4,6-Trinitrotoluene (TNT) has been used as a military explosive for over a hundred years. Contamination concerns have arisen as a result of manufacturing and use on a large scale; however, despite decades of work addressing TNT contamination in the environment, its fate in marine ecosystems is not fully resolved. Here we examine the cycling and fate of TNT in the coastal marine systems by spiking a marine mesocosm containing seawater, sediments, and macrobiota with isotopically labeled TNT ( 15 N-[TNT]), simultaneously monitoring removal, transformation, mineralization, sorption, and biological uptake over a period of 16 days. TNT degradation was rapid, and we observed accumulation of reduced transformation products dissolved in the water column and in pore waters, sorbed to sediments and suspended particulate matter (SPM), and in the tissues of macrobiota. Bulk δ 15 N analysis of sediments, SPM, and tissues revealed large quantities of 15 N beyond that accounted for in identifiable derivatives. TNT-derived N was also found in the dissolved inorganic N (DIN) pool. Using multivariate statistical analysis and a 15 N mass balance approach, we identify the major transformation pathways of TNT, including the deamination of reduced TNT derivatives, potentially promoted by sorption to SPM and oxic surface sediments.

Environmental Science & Technology↗

USGS2015

Declining Dioxin concentrations in the Rhone River, France, attest to the effectiveness of emissions controls

Emission-control policies have been implemented in Europe and North America since the 1990s for polychlorodibenzodioxins (PCDDs) and furans (PCDFs). To assess the effect of these policies on temporal trends and spatial patterns for these compounds in a large European river system, sediment cores were collected in seven depositional areas along the Rhone River in France, dated, and analyzed for PCDDs and PCDFs. Results show concentrations increase in the downstream direction and have decreased temporally at all sites during the last two decades, with an average decrease of 83% from 1992 to 2010. The time for a 50% decrease in concentrations (t1/2) averaged 6.9 ± 2.6 and 9.1 ± 2.9 years for the sum of measured PCDDs and PCDFs, respectively. Congener patterns are similar among cores and indicate dominance of regional atmospheric deposition and possibly weathered local sources. Local sources are clearly indicated at the most downstream site, where concentrations of the most toxic dioxin, TCDD, are about 2 orders of magnitude higher than at the other six sites. The relatively steep downward trends attest to the effects of the dioxin emissions reduction policy in Europe and suggest that risks posed to aquatic life in the Rhone River basin from dioxins and furans have been greatly reduced.

Environmental Science & Technology↗

USGS2016

Regional effects of agricultural conservation practices on nutrient transport in the Upper Mississippi River Basin

Despite progress in the implementation of conservation practices, related improvements in water quality have been challenging to measure in larger river systems. In this paper we quantify these downstream effects by applying the empirical U.S. Geological Survey water-quality model SPARROW to investigate whether spatial differences in conservation intensity were statistically correlated with variations in nutrient loads. In contrast to other forms of water quality data analysis, the application of SPARROW controls for confounding factors such as hydrologic variability, multiple sources and environmental processes. A measure of conservation intensity was derived from the USDA-CEAP regional assessment of the Upper Mississippi River and used as an explanatory variable in a model of the Upper Midwest. The spatial pattern of conservation intensity was negatively correlated ( p = 0.003) with the total nitrogen loads in streams in the basin. Total phosphorus loads were weakly negatively correlated with conservation ( p = 0.25). Regional nitrogen reductions were estimated to range from 5 to 34% and phosphorus reductions from 1 to 10% in major river basins of the Upper Mississippi region. The statistical associations between conservation and nutrient loads are consistent with hydrological and biogeochemical processes such as denitrification. The results provide empirical evidence at the regional scale that conservation practices have had a larger statistically detectable effect on nitrogen than on phosphorus loadings in streams and rivers of the Upper Mississippi Basin.

Environmental Science & Technology↗

USGS2015

Identification of groundwater nitrate contamination from explosives used in road construction: Isotopic, chemical, and hydrologic evidence

Explosives used in construction have been implicated as sources of NO 3 – contamination in groundwater, but direct forensic evidence is limited. Identification of blasting-related NO 3 – can be complicated by other NO 3 – sources, including agriculture and wastewater disposal, and by hydrogeologic factors affecting NO 3 – transport and stability. Here we describe a study that used hydrogeology, chemistry, stable isotopes, and mass balance calculations to evaluate groundwater NO 3 – sources and transport in areas surrounding a highway construction site with documented blasting in New Hampshire. Results indicate various groundwater responses to contamination: (1) rapid breakthrough and flushing of synthetic NO 3 – (low δ 15 N, high δ 18 O) from dissolution of unexploded NH 4 NO 3 blasting agents in oxic groundwater; (2) delayed and reduced breakthrough of synthetic NO 3 – subjected to partial denitrification (high δ 15 N, high δ 18 O); (3) relatively persistent concentrations of blasting-related biogenic NO 3 – derived from nitrification of NH 4 + (low δ 15 N, low δ 18 O); and (4) stable but spatially variable biogenic NO 3 – concentrations, consistent with recharge from septic systems (high δ 15 N, low δ 18 O), variably affected by denitrification. Source characteristics of denitrified samples were reconstructed from dissolved-gas data (Ar, N 2 ) and isotopic fractionation trends associated with denitrification (Δδ 15 N/Δδ 18 O ≈ 1.31). Methods and data from this study are expected to be applicable in studies of other aquifers affected by explosives used in construction.

Environmental Science & Technology↗

USGS2016

Long-term changes in sediment and nutrient delivery from Conowingo Dam to Chesapeake Bay: Effects of reservoir sedimentation

Reduction of suspended sediment (SS), total phosphorus (TP), and total nitrogen is an important focus for Chesapeake Bay watershed management. The Susquehanna River, the bay’s largest tributary, has drawn attention because SS loads from behind Conowingo Dam (near the river’s mouth) have been rising dramatically. To better understand these changes, we evaluated histories of concentration and loading (1986–2013) using data from sites above and below Conowingo Reservoir. First, observed concentration-discharge relationships show that SS and TP concentrations at the reservoir inlet have declined under most discharges in recent decades, but without corresponding declines at the outlet, implying recently diminished reservoir trapping. Second, best estimates of mass balance suggest decreasing net deposition of SS and TP in recent decades over a wide range of discharges, with cumulative mass generally dominated by the 75&sim;99.5th percentile of daily Conowingo discharges. Finally, stationary models that better accommodate effects of riverflow variability also support the conclusion of diminished trapping of SS and TP under a range of discharges that includes those well below the literature-reported scour threshold. Overall, these findings suggest that decreased net deposition of SS and TP has occurred at subscour levels of discharge, which has significant implications for the Chesapeake Bay ecosystem.

Maryland↗

USGS2016

Copper speciation in variably toxic sediments at the Ely Copper Mine, Vermont, United States

At the Ely Copper Mine Superfund site, Cu concentrations exceed background values in both streamwater (160–1200 times) and sediments (15–79 times). Previously, these sediment samples were incubated with laboratory test organisms, and they exhibited variable toxicity for different stream sites. In this study we combined bulk- and microscale techniques to determine Cu speciation and distribution in these contaminated sediments on the basis of evidence from previous work that Cu was the most important stressor in this environment and that variable observed toxicity could have resulted from differences in Cu speciation. Copper speciation results were similar at microscopic and bulk scales. The major Cu species in the more toxic samples were sorbed or coprecipitated with secondary Mn (birnessite) and Fe minerals (jarosite and goethite), which together accounted for nearly 80% of the total Cu. The major Cu species in the less toxic samples were Cu sulfides (chalcopyrite and a covellite-like phase), making up about 80–95% of the total Cu, with minor amounts of Cu associated with jarosite or goethite. These Cu speciation results are consistent with the toxicity results, considering that Cu sorbed or coprecipitated with secondary phases at near-neutral pH is relatively less stable than Cu bound to sulfide at lower pH. The more toxic stream sediment sites were those that contained fewer detrital sulfides and were upstream of the major mine waste pile, suggesting that removal and consolidation of sulfide-bearing waste piles on site may not eliminate all sources of bioaccessible Cu.

Vermont↗

USGS2015

Implications of climate change on the heat budget of lentic systems used for power station cooling: Case study Clinton Lake, Illinois

We use a numerical model to analyze the impact of climate change--in particular higher air temperatures--on a nuclear power station that recirculates the water from a reservoir for cooling. The model solves the hydrodynamics, the transfer of heat in the reservoir, and the energy balance at the surface. We use the numerical model to (i) quantify the heat budget in the reservoir and determine how this budget is affected by the combined effect of the power station and climate change and (ii) quantify the impact of climate change on both the downstream thermal pollution and the power station capacity. We consider four different scenarios of climate change. Results of simulations show that climate change will reduce the ability to dissipate heat to the atmosphere and therefore the cooling capacity of the reservoir. We observed an increase of 25% in the thermal load downstream of the reservoir, and a reduction in the capacity of the power station of 18% during the summer months for the worst-case climate change scenario tested. These results suggest that climate change is an important threat for both the downstream thermal pollution and the generation of electricity by power stations that use lentic systems for cooling.

Illinois↗

USGS2015

Human and bovine viruses and bacteria at three Great Lakes beaches: Environmental variable associations and health risk

Waterborne pathogens were measured at three beaches in Lake Michigan, environmental factors for predicting pathogen concentrations were identified, and the risk of swimmer infection and illness was estimated. Waterborne pathogens were detected in 96% of samples collected at three Lake Michigan beaches in summer, 2010. Samples were quantified for 22 pathogens in four microbial categories (human viruses, bovine viruses, protozoa, and pathogenic bacteria). All beaches had detections of human and bovine viruses and pathogenic bacteria indicating influence of multiple contamination sources at these beaches. Occurrence ranged from 40 to 87% for human viruses, 65–87% for pathogenic bacteria, and 13–35% for bovine viruses. Enterovirus, adenovirus A, Salmonella spp. , Campylobacter jejuni , bovine polyomavirus, and bovine rotavirus A were present most frequently. Variables selected in multiple regression models used to explore environmental factors that influence pathogens included wave direction, cloud cover, currents, and water temperature. Quantitative Microbial Risk Assessment was done for C. jejuni , Salmonella spp. , and enteroviruses to estimate risk of infection and illness. Median infection risks for one-time swimming events were approximately 3 × 10 –5 , 7 × 10 –9 , and 3 × 10 –7 for C. jejuni , Salmonella spp., and enteroviruses, respectively. Results highlight the importance of investigating multiple pathogens within multiple categories to avoid underestimating the prevalence and risk of waterborne pathogens.

Wisconsin↗

USGS2016

Isotopic composition of inorganic mercury and methylmercury downstream of a historical gold mining region

We measured total mercury (THg) and monomethyl mercury (MMHg) concentrations and mercury (Hg) isotopic compositions in sediment and aquatic organisms from the Yuba River (California, USA) to identify Hg sources and biogeochemical transformations downstream of a historical gold mining region. Sediment THg concentrations and δ 202 Hg decreased from the upper Yuba Fan to the lower Yuba Fan and the Feather River. These results are consistent with the release of Hg during gold mining followed by downstream mixing and dilution. The Hg isotopic composition of Yuba Fan sediment (δ 202 Hg = −0.38 ± 0.17&permil; and Δ 199 Hg = 0.04 ± 0.03&permil;; mean ± 1 SD, n = 7) provides a fingerprint of inorganic Hg (IHg) that could be methylated locally or after transport downstream. The isotopic composition of MMHg in the Yuba River food web was estimated using biota with a range of %MMHg (the percent of THg present as MMHg) and compared to IHg in sediment, algae, and the food web. The estimated δ 202 Hg of MMHg prior to photodegradation (−1.29 to −1.07&permil;) was lower than that of IHg and we suggest this is due to mass-dependent fractionation (MDF) of up to −0.9&permil; between IHg and MMHg. This result is in contrast to net positive MDF (+0.4 to +0.8&permil;) previously observed in lakes, estuaries, coastal oceans, and forests. We hypothesize that this unique relationship could be due to differences in the extent or pathway of biotic MMHg degradation in stream environments.

California↗

USGS2016

Dietary uptake of Cu sorbed to hydrous iron oxide is linked to cellular toxicity and feeding inhibition in a benthic grazer

Whereas feeding inhibition caused by exposure to contaminants has been extensively documented, the underlying mechanism(s) are less well understood. For this study, the behavior of several key feeding processes, including ingestion rate and assimilation efficiency, that affect the dietary uptake of Cu were evaluated in the benthic grazer Lymnaea stagnalis following 4–5 h exposures to Cu adsorbed to synthetic hydrous ferric oxide (Cu–HFO). The particles were mixed with a cultured alga to create algal mats with Cu exposures spanning nearly 3 orders of magnitude at variable or constant Fe concentrations, thereby allowing first order and interactive effects of Cu and Fe to be evaluated. Results showed that Cu influx rates and ingestion rates decreased as Cu exposures of the algal mat mixture exceeded 10 4 nmol/g. Ingestion rate appeared to exert primary control on the Cu influx rate. Lysosomal destabilization rates increased directly with Cu influx rates. At the highest Cu exposure where the incidence of lysosomal membrane damage was greatest (51%), the ingestion rate was suppressed 80%. The findings suggested that feeding inhibition was a stress response emanating from excessive uptake of dietary Cu and cellular toxicity.

Environmental Science & Technology↗

USGS2016

Comparative evaluation of statistical and mechanistic models of Escherichia coli at beaches in southern Lake Michigan

Statistical and mechanistic models are popular tools for predicting the levels of indicator bacteria at recreational beaches. Researchers tend to use one class of model or the other, and it is difficult to generalize statements about their relative performance due to differences in how the models are developed, tested, and used. We describe a cooperative modeling approach for freshwater beaches impacted by point sources in which insights derived from mechanistic modeling were used to further improve the statistical models and vice versa. The statistical models provided a basis for assessing the mechanistic models which were further improved using probability distributions to generate high-resolution time series data at the source, long-term “tracer” transport modeling based on observed electrical conductivity, better assimilation of meteorological data, and the use of unstructured-grids to better resolve nearshore features. This approach resulted in improved models of comparable performance for both classes including a parsimonious statistical model suitable for real-time predictions based on an easily measurable environmental variable (turbidity). The modeling approach outlined here can be used at other sites impacted by point sources and has the potential to improve water quality predictions resulting in more accurate estimates of beach closures.

Lake Michigan, Ogden Dunes↗

USGS2016

Hydrologic controls on nitrogen cycling processes and functional gene abundance in sediments of a groundwater flow-through lake

The fate and transport of inorganic nitrogen (N) is a critically important issue for human and aquatic ecosystem health because discharging N-contaminated groundwater can foul drinking water and cause algal blooms. Factors controlling N-processing were examined in sediments at three sites with contrasting hydrologic regimes at a lake on Cape Cod, MA. These factors included water chemistry, seepage rates and direction of groundwater flow, and the abundance and potential rates of activity of N-cycling microbial communities. Genes coding for denitrification, anaerobic ammonium oxidation (anammox), and nitrification were identified at all sites regardless of flow direction or groundwater dissolved oxygen concentrations. Flow direction was, however, a controlling factor in the potential for N-attenuation via denitrification in the sediments. Potential rates of denitrification varied from 6 to 4500 pmol N/g/h from the inflow to the outflow side of the lake, owing to fundamental differences in the supply of labile organic matter. The results of laboratory incubations suggested that when anoxia and limiting labile organic matter prevailed, the potential existed for concomitant anammox and denitrification. Where oxic lake water was downwelling, potential rates of nitrification at shallow depths were substantial (1640 pmol N/g/h). Rates of anammox, denitrification, and nitrification may be linked to rates of organic N-mineralization, serving to increase N-mobility and transport downgradient.

Massachusetts↗

USGS2025

High-throughput screening identifies bisphenol P as a potent cardiotoxin, inducing cardiotoxicity through apoptosis and NF-κB Pathway

The increasing use of plastic additives, particularly bisphenols (BPs), has raised significant concerns about their potential risks to human health, especially during critical developmental stages. In this study, we developed a novel high-throughput toxicity screening platform using zebrafish ( Danio rerio ) to identify and prioritize chemicals with cardiotoxic potential, which is based on multidimensional exposure pathways ranging from environmental to human levels. The platform quantitatively assesses heart rate changes based on multilevel exposure pathways (environmental, ecological, and human), effectively prioritizing the most relevant cardiotoxic compounds with potential health risks. Using this platform, we identified bisphenol P (BPP), a widely used substitute for bisphenol A, as a potent cardiotoxic compound. BPP exposure significantly inhibited heart development and function in zebrafish, inducing abnormal heart morphology, reduced heart rate, cardiac output, and hemodynamic disturbances. Additionally, NF-κB signaling pathway analysis, including morpholino knock-down and inhibitor experiments, confirmed that BPP mediates cardiac toxicity by inducing cardiomyocyte apoptosis. Our findings underscore the toxicity that BP substitutes can have, while highlighting the potential of this multidimensional screening platform in evaluating cardiovascular toxicity and guiding future toxicological assessments during critical developmental windows.

Environmental Science & Technology↗