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USGS2008

Lead sequestration and species redistribution during soil organic matter decomposition

The turnover of soil organic matter (SOM) maintains a dynamic chemical environment in the forest floor that can impact metal speciation on relatively short timescales. Here we measure the speciation of Pb in controlled and natural organic (O) soil horizons to quantify changes in metal partitioning during SOM decomposition in different forest litters. We provide a link between the sequestration of pollutant Pb in O-horizons, estimated by forest floor Pb inventories, and speciation using synchrotron-based X-ray fluorescence and X-ray absorption spectroscopy. When Pb was introduced to fresh forest Oi samples, it adsorbed primarily to SOM surfaces, but as decomposition progressed over two years in controlled experiments, up to 60% of the Pb was redistributed to pedogenic birnessite and ferrihydrite surfaces. In addition, a significant fraction of pollutant Pb in natural soil profiles was associated with similar mineral phases (???20-35%) and SOM (???65-80%). Conifer forests have at least 2-fold higher Pb burdens in the forest floor relative to deciduous forests due to more efficient atmospheric scavenging and slower organic matter turnover. We demonstrate that pedogenic minerals play an important role in surface soil Pb sequestration, particularly in deciduous forests, and should be considered in any assessment of pollutant Pb mobility. ?? 2008 American Chemical Society.

Environmental Science & Technology↗
USGS2008

Coastal strategies to predict Escherichia coli concentrations for beaches along a 35 km stretch of southern Lake Michigan

To understand the fate and movement of Escherichia coli in beach water, numerous modeling studies have been undertaken including mechanistic predictions of currents and plumes and empirical modeling based on hydrometeorological variables. Most approaches are limited in scope by nearshore currents or physical obstacles and data limitations; few examine the issue from a larger spatial scale. Given the similarities between variables typically included in these models, we attempted to take a broader view of E. coli fluctuations by simultaneously examining twelve beaches along 35 km of Indiana's Lake Michigan coastline that includes five point-source outfalls. The beaches had similar E. coli fluctuations, and a best-fit empirical model included two variables: wave height and an interactive term comprised of wind direction and creek turbidity. Individual beach R2 was 0.32-0.50. Data training-set results were comparable to validation results (R2 = 0.48). Amount of variation explained by the model was similar to previous reports for individual beaches. By extending the modeling approach to include more coastline distance, broader-scale spatial and temporal changes in bacteria concentrations and the influencing factors can be characterized. ?? 2008 American Chemical Society.

Environmental Science & Technology↗
USGS2008

Persistence of pathogenic prion protein during simulated wastewater treatment processes

Transmissible spongiform encephalopathies (TSEs, prion diseases) are a class of fatal neurodegenerative diseases affecting a variety of mammalian species including humans. A misfolded form of the prion protein (PrP TSE) is the major, if not sole, component of the infectious agent. Prions are highly resistant to degradation and to many disinfection procedures suggesting that, if prions enter wastewater treatment systems through sewers and/or septic systems (e.g., from slaughterhouses, necropsy laboratories, rural meat processors, private game dressing) or through leachate from landfills that have received TSE-contaminated material, prions could survive conventional wastewater treatment Here, we report the results of experiments examining the partitioning and persistence of PrPTSE during simulated wastewater treatment processes including activated and mesophilic anaerobic sludge digestion. Incubation with activated sludge did not result in significant PrPTSE degradation. PrPTSE and prion infectivity partitioned strongly to activated sludge solids and are expected to enter biosolids treatment processes. A large fraction of PrPTSE survived simulated mesophilic anaerobic sludge digestion. The small reduction in recoverable PrPTSE after 20-d anaerobic sludge digestion appeared attributable to a combination of declining extractability with time and microbial degradation. Our results suggest that if prions were to enter municipal wastewater treatment systems, most would partition to activated sludge solids, survive mesophilic anaerobic digestion, and be present in treated biosolids. ?? 2008 American Chemical Society.

Environmental Science & Technology↗
USGS2008

Real-time PCR detection and quantification of nine potential sources of fecal contamination by analysis of mitochondrial Cytochrome b targets

We designed and tested real-time PCR probe/primer sets to detect and quantify Cytochrome b sequences of mitochondrial DNA (mtDNA) from nine vertebrate species of pet (dog), farm (cow, chicken, sheep, horse, pig), wildlife (Canada goose, white-tailed deer), and human. Linear ranges of the assays were from 101 to 108 copies/??l. To formally test the performance of the assays, twenty blinded fecal suspension samples were analyzed by real-time PCR to identify the source of the feces. Sixteen of the twenty samples were correctly and unambiguously identified. Average sensitivity was calculated to be 0.850, while average specificity was found to be 0.994. One beef cow sample was not detected, but mtDNA from 11 other beef cattle of both sexes and varying physiological states was found in concentrations similar (3.45 ?? 107 copies/g) to thatfound in human feces (1.1 ?? 107 copies/g). Thus, environmental conditions and sample handling are probably important factors for successful detection of fecal mtDNA. When sewage samples were analyzed, only human mtDNA (7.2 ?? 104 copies/100 mL) was detected. With a detection threshold of 250 copies/reaction, an efficient concentration and purification method resulted in a final detection limit for human feces of 1.8 mg/100 mL water.

Environmental Science & Technology↗
USGS2008

Comparison of two U.S. power-plant carbon dioxide emissions data sets

Estimates of fossil-fuel CO2 emissions are needed to address a variety of climate-change mitigation concerns over a broad range of spatial and temporal scales. We compared two data sets that report power-plant CO 2 emissions in the conterminous U.S. for 2004, the most recent year reported in both data sets. The data sets were obtained from the Department of Energy's Energy Information Administration (EIA) and the Environmental Protection Agency's eGRID database. Conterminous U.S. total emissions computed from the data sets differed by 3.5% for total plant emissions (electricity plus useful thermal output) and 2.3% for electricity generation only. These differences are well within previous estimates of uncertainty in annual U.S. fossil-fuel emissions. However, the corresponding average absolute differences between estimates of emissions from individual power plants were much larger, 16.9% and 25.3%, respectively. By statistical analysis, we identified several potential sources of differences between EIA and eGRID estimates for individual plants. Estimates that are based partly or entirely on monitoring of stack gases (reported by eGRID only) differed significantly from estimates based on fuel consumption (as reported by EIA). Differences in accounting methods appear to explain differences in estimates for emissions from electricity generation from combined heat and power plants, and for total and electricity generation emissions from plants that burn nonconventional fuels (e.g., biomass). Our analysis suggests the need for care in utilizing emissions data from individual power plants, and the need for transparency in documenting the accounting and monitoring methods used to estimate emissions.

Environmental Science & Technology↗
USGS2008

Interaction between urbanization and climate variability amplifies watershed nitrate export in Maryland

We investigated regional effects of urbanization and land use change on nitrate concentrations in approximately 1,000 small streams in Maryland during record drought and wet years in 2001-2003. We also investigated changes in nitrate-N export during the same time period in 8 intensively monitored small watersheds across an urbanization gradient in Baltimore, Maryland. Nitrate-N concentrations in Maryland were greatest in agricultural streams, urban streams, and forest streams respectively. During the period of record drought and wet years, nitrate-N exports in Baltimore showed substantial variation in 6 suburban/urban streams (2.9-15.3 kg/ha/y), 1 agricultural stream (3.4-38.9 kg/ha/y), and 1 forest stream (0.03-0.2 kg/ ha/y). Interannual variability was similar for small Baltimore streams and nearby well-monitored tributaries and coincided with record hypoxia in Chesapeake Bay. Discharge-weighted mean annual nitrate concentrations showed a variable tendency to decrease/increase with changes in annual runoff, although total N export generally increased with annual runoff. N retention in small Baltimore watersheds during the 2002 drought was 85%, 99%, and 94% for suburban, forest, and agricultural watersheds, respectively, and declined to 35%, 91%, and 41% during the wet year of 2003. Our results suggest that urban land use change can increase the vulnerability of ecosystem nitrogen retention functions to climatic variability. Further work is necessary to characterize patterns of nitrate-N export and retention in small urbanizing watersheds under varying climatic conditions to improve future forecasting and watershed scale restoration efforts aimed at improving nitrate-N retention. ?? 2008 American Chemical Society.

Environmental Science & Technology↗
USGS2008

Environmental occurrence of the enterococcal surface protein ( esp ) gene is an unreliable indicator of human fecal contamination

The enterococcal surface protein ( esp ) gene found in Enterococcus faecalis and E. faecium has recently been explored as a marker of sewage pollution in recreational waters but its occurrence and distribution in environmental enterococci has not been well-documented. If the esp gene is found in environmental samples, there are potential implications for microbial source tracking applications. In the current study, a total of 452 samples (lake water, 100; stream water, 129; nearshore sand, 96; and backshore sand, 71; Cladophora sp. (Chlorophyta), 41; and periphyton (mostly Bacillariophyceae ), 15) collected from the coastal watersheds of southern Lake Michigan were selectively cultured for enterococci and then analyzed for the esp gene by PCR, targeting E. faecalis/ E. faecium ( esp fs/fm ) and E. faecium ( esp fm ). Overall relative frequencies for esp fs/fm and esp fm were 27.4 and 5.1%. Respective percent frequency for the esp fs/fm and esp fm was 36 and 14% in lake water; 38.8 and 2.3% in stream water; 24 and 6.3% in nearshore sand; 0% in backshore sand; 24.4 and 0% in Cladophora sp.; and 33.3 and 0% in periphyton. The overall occurrence of both esp fs/fm and esp fm was significantly related ( χ 2 = 49, P < 0.0001). Post-rain incidence of esp fs/fm increased in lake and stream water and nearshore sand. Further, E. coli and enterococci cell densities were significant predictors for esp fs/fm occurrence in post-rain lake water, but esp fm was not. F + coliphage densities were not significant predictors for esp fm or esp fs/fm gene incidence. In summary, the differential occurrence of the esp gene in the environment suggests that it is not limited to human fecal sources and thus may weaken its use as a reliable tool in discriminating contaminant sources (i.e., human vs nonhuman).

Environmental Science & Technology↗
USGS2008

Removal of dissolved organic matter by anion exchange: Effect of dissolved organic matter properties

Ten isolates of aquatic dissolved organic matter (DOM) were evaluated to determine the effect that chemical properties of the DOM, such as charge density, aromaticity, and molecular weight, have on DOM removal by anion exchange. The DOM isolates were characterized as terrestrial, microbial, or intermediate humic substances or transphilic acids. All anion exchange experiments were conducted using a magnetic ion exchange (MIEX) resin. The charge density of the DOM isolates, determined by direct potentiometric titration, was fundamental to quantifying the stoichiometry of the anion exchange mechanism. The results clearly show that all DOM isolates were removed by anion exchange; however, differences among the DOM isolates did influence their removal by MIEX resin. In particular, MIEX resin had the greatest affinity for DOM with high charge density and the least affinity for DOM with low charge density and low aromaticity. This work illustrates that the chemical characteristics of DOM and solution conditions must be considered when evaluating anion exchange treatment for the removal of DOM.

Environmental Science & Technology↗
USGS2008

Evaluating regional patterns in nitrate sources to watersheds in national parks of the Rocky Mountains using nitrate isotopes

In the Rocky Mountains, there is uncertainty about the source areas and emission types that contribute to nitrate (NO 3 ) deposition, which can adversely affect sensitive aquatic habitats of high-elevation watersheds. Regional patterns in NO 3 deposition sources were evaluated using NO 3 isotopes in five National Parks, including 37 lakes and 7 precipitation sites. Results indicate that lake NO 3 ranged from detection limit to 38 μeq/L, δ 18 O (NO 3 ) ranged from −5.7 to +21.3‰, and δ 15 N (NO 3 ) ranged from −6.6 to +4.6‰. δ 18 O (NO 3 ) in precipitation ranged from +71 to +78‰. δ 15 N (NO 3 ) in precipitation and lakes overlap; however, δ 15 N (NO 3 ) in precipitation is more depleted than δ 15 N (NO 3 ) in lakes, ranging from −5.5 to −2.0‰. δ 15 N (NO 3 ) values are significantly related ( p < 0.05) to wet deposition of inorganic N, sulfate, and acidity, suggesting that spatial variability of δ 15 N (NO 3 ) over the Rocky Mountains may be related to source areas of these solutes. Regional patterns show that NO 3 and δ 15 N (NO 3 ) are more enriched in lakes and precipitation from the southern Rockies and at higher elevations compared to the northern Rockies. The correspondence of high NO 3 and enriched δ 15 N (NO 3 ) in precipitation with high NO 3 and enriched δ 15 N (NO 3 ) in lakes, suggests that deposition of inorganic N in wetfall may affect the amount of NO 3 in lakes through a combination of direct and indirect processes such as enhanced nitrification.

Environmental Science & Technology↗
USGS2009

Method development for analysis of urban dust using scanning electron microscopy with energy dispersive x-ray spectrometry to detect the possible presence of world trade center dust constituents

The collapse of the World Trade Center Towers on September 11, 2001, sent dust and debris across much of Manhattan and in the surrounding areas. Indoor and outdoor dust samples were collected and characterized by U.S. Geological Survey (USGS) scientists using scanning electron microscopy with energy-dispersive spectrometry (SEM/EDS). From this characterization, the U.S. Environmental Protection Agency and USGS developed a particulate screening method to determine the presence of residual World Trade Center dust in the indoor environment using slag wool as a primary "signature". The method describes a procedure that includes splitting, ashing, and sieving of collected dust. From one split, a 10 mg/mL dust/ isopropanol suspension was prepared and 10-30 ??L aliquots of the suspension placed on an SEM substrate. Analyses were performed using SEM/EDS manual point counting for slag wool fibers. Poisson regression was used to identify some of the sources of uncertainty, which are directly related to the small number of fibers present on each sample stub. Preliminary results indicate that the procedure is promising for screening urban background dust for the presence of WTC dust. Consistent sample preparation of reference materials and samples must be performed by each laboratory wishing to use this method to obtain meaningful and accurate results. ?? 2009 American Chemical Society.

Environmental Science & Technology↗
USGS2008

Susceptibility of synthetic long-chain alkylbenzenes to degradation in reducing marine sediments

Long-chain alkylbenzenes (LCABs) synthesized for production of alkylbenzene sulfonate surfactants have been used as molecular markers of anthropogenic waste for 25 years. Synthetic LCABs comprise two classes, the tetrapropylene-based alkylbenzenes (TABs) and the linear alkylbenzenes (LABs). LABs supplanted TABs in the mid-1960s because of improved biodegradability of their sulfonated analogs. Use of LCABs for molecular stratigraphy depends on their preservation in sediments over decadal time scales. Most laboratory and field studies suggest that LABs degrade rapidly under aerobic conditions but are resistant to degradation when oxygen is absent. However, recent work indicates that LABs may not be as persistent under reducing conditions as previously thought. To assess the potential for degradation of LCABs in reducing sediments, box cores collected in 1992 and 2003 near a submarine wastewater outfall system were analyzed using gas chromatography/mass spectrometry. The TABs were effectively preserved; differences between whole-core inventories were within analytical error. By contrast, whole-core inventories of the LABs decreased by about 50−60% during the same time interval. Based on direct comparison of chemical inventories in coeval core sections, LAB transformation rates are estimated at 0.07 ± 0.01 yr −1 . These results indicate that caution should be exercised when using synthetic LCABs for reconstruction of depositional records.

Environmental Science & Technology↗
USGS2008

Occurrence and turnover of nitric oxide in a nitrogen-impacted sand and gravel aquifer

Little is known about nitric oxide (NO) production or consumption in the subsurface, an environment which may be conducive to NO accumulation. A study conducted in a nitrogen-contaminated aquifer on Cape Cod, Massachusetts assessed the occurrence and turnover of NO within a contaminant plume in which nitrification and denitrification were known to occur. NO (up to 8.6 nM) was detected in restricted vertical zones located within a nitrate (NO 3 − ) gradient and characterized by low dissolved oxygen (<10 μM). NO concentrations correlated best with nitrite (NO 2 − ) (up to 35 μM), but nitrous oxide (N 2 O) (up to 1 μM) also was present. Single-well injection tests were used to determine NO production and consumption in situ within these zones. First-order rate constants for NO consumption were similar (0.05−0.08 h −1 ) at high and low (260 and 10 nM) NO concentrations, suggesting a turnover time at in situ concentrations of 10−20 h. Tracer tests with 15 N[NO] demonstrated that oxidation to 15 N[NO 2 − ] occurred only during the initial stages, but after 4 h reduction to 15 N[N 2 O] was the primary reaction product. Added NO 2 − (31 μM) or NO 3 − (53 μM) resulted in a linear NO accumulation at 2.4 and 1.0 nM h −1 for the first 6 h of in situ tests. These results suggest that NO was primarily produced by denitrification within this aquifer.

Environmental Science & Technology↗
USGS2008

Volatile selenium flux from the great Salt Lake, Utah

The removal mechanisms that govern Se concentrations in the Great Salt Lake are unknown despite this terminal lake being an avian habitat of hemispheric importance. However, the volatilization flux of Se from the Great Salt Lake has not been previously measured due to challenges of analysis in this hypersaline environment This paper presents results from recent field studies examining the spatial distribution of dissolved volatile Se (areally and with depth) in the south arm (main body) of the Great Salt Lake. The analyses involved collection of dissolved volatile Se in a cryofocusing trap system via sparging with helium. The cryotrapped volatile Se was digested with nitric acid and analyzed by inductively coupled plasma mass spectrometry (ICP-MS). Results show concentrations of dissolved volatile Se that increase with depth in the shallow brine, suggesting that phytoplankton in the open waters and bioherms in shallow sites (<4 m in depth) may be responsible for volatile Se production. Volatile Se flux to the atmosphere was determined using mass transport models corrected to simulate the highly saline environment of the south arm of the Great Salt Lake. The estimated annual flux of volatile Se was 1455 kg/year within a range from 560 to 3780 kg Se/year for the 95% confidence interval and from 970 to 2180 kg Se/year within the 68% confidence interval. ?? 2009 American Chemical Society.

Environmental Science & Technology↗
USGS2008

Model predictions of realgar precipitation by reaction of As(III) with synthetic mackinawite under anoxic conditions

This study investigates the removal of As(III) from solution using mackinawite, a nanoparticulate reduced iron sulfide. Mackinawite suspensions (0.1−40 g/L) effectively lower initial concentrations of 1.3×10 −5 M As(III) from pH 5−10, with maximum removal occurring under acidic conditions. Based on E h measurements, it was found that the redox state of the system depended on the mackinawite solids concentration and pH. Higher initial mackinawite concentrations and alkaline pH resulted in a more reducing redox condition. Given this, the pH edge data were modeled thermodynamically using pe (−log[e − ]) as a fitting parameter and linear pe−pH relationships within the range of measured E h values as a function of pH and mackinawite concentration. The model predicts removal of As(III) from solution by precipitation of realgar with the formation of secondary oxidation products, greigite or a mixed-valence iron oxide phase, depending on pH. This study demonstrates that mackinawite is an effective sequestration agent for As(III) and highlights the importance of incorporating redox into models describing the As−Fe−S−H 2 O system.

Environmental Science & Technology↗
USGS2008

Aquatic toxicity of airfield-pavement deicer materials and implications for airport runoff

Concentrations of airfield-pavement deicer materials (PDM) in a study of airport runoff often exceeded levels of concern regarding aquatic toxicity. Toxicity tests on Vibrio fischeri, Pimephales promelas, Ceriodaphnia dubia, and Pseudokirchneriella subcapitata (commonly known as Selenastrum capricornutum) were performed with potassium acetate (K-Ac) PDM, sodium formate (Na-For) PDM, and with freezing- point depressants (K-Ac and Na-For). Results indicate that toxicity in PDM is driven by the freezing-point depressants in all tests except the Vibrio fisheri test for Na-For PDM which is influenced by an additive. Acute toxicity end points for different organisms ranged from 298 to 6560 mg/L (as acetate) for K-Ac PDM and from 1780 to 4130 mg/L (as formate) for Na- For PDM. Chronic toxicity end points ranged from 19.9 to 336 mg/L (as acetate) for K-Ac PDM and from 584 to 1670 mg/L (as formate) for Na-For PDM. Sample results from outfalls at General Mitchell International Airport in Milwaukee, Wl (GMIA) indicated that 40% of samples had concentrations greater than the aquatic-life benchmark for K-Ac PDM. K-Ac has replaced urea during the 1990s as the most widely used PDM at GMIA and in the United States. Results of ammonia samples from airport outfalls during periods when urea-based PDM was used at GMIA indicated that41% of samples had concentrations exceeding the U.S. Environmental Protection Agency (USEPA) 1 -h water-quality criterion. The USEPA 1-h water-quality criterion for chloride was exceeded in 68% of samples collected in the receiving stream, a result of road-salt runoff from urban influence near the airport. Results demonstrate that PDM must be considered to comprehensively evaluate the impact of chemical deicers on aquatic toxicity in water containing airport runoff. ?? 2009 American Chemical Society.

Environmental Science & Technology↗
USGS2008

Summer E. coli patterns and responses along 23 Chicago beaches

Concentrations of E. coli in recreational beach water are highly variable both locally and temporally, but a broader understanding of these fluctuations may be explained through coastal observations. Currently, beach contamination study approaches tend to be site-specific underthe belief that politically delineated beaches are unique and management of beaches cannot be regionally oriented. E. coli data collected over five years from 23 Chicago beaches clearly identified ambient linked patterns at the regional scale. Temporal fluctuations were similar, with all beaches having simultaneous peaks and troughs of E. coli concentrations. Spatially, E. coli concentrations for beaches more closely situated were more closely correlated, indicating spatial autocorrelation. Julian day, wave height, and barometric pressure explained up to 40% of the variation, a value comparable to individual, less parsimonious site-specific models. Day of sampling could explain the majority of the variation in E. coli concentrations, more so than beach, depth, or time of day. Comparing beaches along a targeted coastline allows a better understanding of inherent background regional fluctuations and, ultimately, better predictions of E. coli concentrations in coastal recreational water.

Environmental Science & Technology↗
USGS2009

Geochemistry of inorganic nitrogen in waters released from coal-bed natural gas production wells in the Powder River Basin, Wyoming

Water originating from coal-bed natural gas (CBNG) production wells typically contains ammonium and is often disposed via discharge to ephemeral channels. A study conducted in the Powder River Basin, Wyoming, documented downstream changes in CBNG water composition, emphasizing nitrogen-cycling processes and the fate of ammonium. Dissolved ammonium concentrations from 19 CBNG discharge points ranged from 95 to 527 μM. Within specific channels, ammonium concentrations decreased with transport distance, with subsequent increases in nitrite and nitrate concentrations. Removal efficiency, or uptake, of total dissolved inorganic nitrogen (DIN) varied between channel types. DIN uptake was greater in the gentle-sloped, vegetated channel as compared to the incised, steep, and sparsely vegetated channel and was highly correlated with diel patterns of incident light and dissolved oxygen concentration. In a larger main channel with multiple discharge inputs ( n = 13), DIN concentrations were >300 μM, with pH > 8.5, after 5 km of transport. Ammonium represented 25−30% of the large-channel DIN, and ammonium concentrations remained relatively constant with time, with only a weak diel pattern evident. In July 2003, the average daily large-channel DIN load was 23 kg N day −1 entering the Powder River, an amount which substantially increased the total Powder River DIN load after the channel confluence. These results suggest that CBNG discharge may be an important source of DIN to western watersheds, at least at certain times of the year, and that net oxidation and/or removal is dependent upon the extent of contact with sediment and biomass, type of drainage channel, and time of day.

Wyoming↗
USGS2009

Mercury cycling in stream ecosystems. 1. Water column chemistry and transport

We studied total mercury (THg) and methylmercury (MeHg) in eight streams, located in Oregon, Wisconsin, and Florida, that span large ranges in climate, landscape characteristics, atmospheric Hg deposition, and water chemistry. While atmospheric deposition was the source of Hg at each site, basin characteristics appeared to mediate this source by providing controls on methylation and fluvial THg and MeHg transport. Instantaneous concentrations of filtered total mercury (FTHg) and filtered methylmercury (FMeHg) exhibited strong positive correlations with both dissolved organic carbon (DOC) concentrations and streamflow for most streams, whereas mean FTHg and FMeHg concentrations were correlated with wetland density of the basins. For all streams combined, whole water concentrations (sum of filtered and particulate forms) of THg and MeHg correlated strongly with DOC and suspended sediment concentrations in the water column.

Environmental Science & Technology↗