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USGS2008

Coupled effect of chemotaxis and growth on microbial distributions in organic-amended aquifer sediments: Observations from laboratory and field studies

The inter-relationship of growth and chemotactic response exhibited by two common soil-inhabiting bacteria was investigated to determine its impact on bacterial migration. Filter-chambers were used to simulate aquifer sediments characterized by vertical gradients of organic contaminants in both artificial groundwater flow systems in the laboratory and within the screened intervals of observation wells in a sandy aquifer. A labile model contaminant (acetate) was added to the top compartments of the three-part chambers, whereas bacteria with a demonstrated propensity to grow on and chemotactically respond to acetate were introduced to the lower compartments. The motility and chemotactic response of Pseudomonas putida F1 resulted in 40 to 110% greater abundances in the upper compartments and concomitant 22 to 70% depletions in the lower compartments relative to the nonchemotactic controls over 2 days. Bacteria were in greatest abundance within the sand plug that separated the upper and lower compartments where sharp acetate gradients induced a strong chemotactic response. This observation was consistent with predictions from a mathematical model. In agreement with the laboratory results, the down-well filter-chamber incubations with Pseudomonas stutzeri in the aquifer indicated that 91% fewer bacteria resided in the lower compartment than the control experiment without acetate at 15 h. The combination of chemotaxis and growth greatly accelerated the migration of bacteria toward and subsequent abundance at the higher acetate concentration.

Environmental Science & Technology↗
USGS2008

DDE in sediments of the Palos Verdes shelf, California: In situ transformation rates and geochemical fate

From 1947 to 1971 the world's largest manufacturer of DDT discharged process wastes into the sewers of Los Angeles County. Roughly 870-1450 t of DDT were released to the ocean off Palos Verdes, CA, a portion of which (???100 t) resides in sediments on the continental shelf and slope. The most abundant DDT compound in the sediments, p,p???-DDE, is degrading by reductive dechlorination, butthe rate of transformation and factors controlling it are not well understood. In order to estimate in situ transformation rates and predict the long-term fate of p,p???-DDE, box cores were collected in 1992 and 2003 from a single location on the Palos Verdes Shelf and analyzed for 8 DDT compounds and 84 polychlorinated biphenyl (PCB) congeners. The PCBs show no evidence of dechlorination, and inventories did not change between 1992 and 2003. By contrast, the inventory of p,p???-DDE decreased by 43%, whereas that of p,p???-DDMU, the putative reductive dechlorination product increased by 34%. The first-order transformation rate for p,p???-DDE at the study site is 0.051 ?? 0.006 yr-1. A multistep reaction model suggests that inventories of p,p???-DDE and p,p???-DDMU will continue to decline, whereas that of p,p???-DDNU will reach a maximum around 2014.

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

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

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

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↗
USGS2009

Mercury cycling in stream ecosystems. 3. Trophic dynamics and methylmercury bioaccumulation

Trophic dynamics (community composition and feeding relationships) have been identified as important drivers of methylmercury (MeHg) bioaccumulation in lakes, reservoirs, and marine ecosystems. The relative importance of trophic dynamics and geochemical controls on MeHg bioaccumulation in streams, however, remains poorly characterized. MeHg bioaccumulation was evaluated in eight stream ecosystems across the United States (Oregon, Wisconsin, and Florida) spanning large ranges in climate, landscape characteristics, atmospheric Hg deposition, and stream chemistry. Across all geographic regions and all streams, concentrations of total Hg (THg) in top predator fish and forage fish, and MeHg in invertebrates, were strongly positively correlated to concentrations of filtered THg (FTHg), filtered MeHg (FMeHg), and dissolved organic carbon (DOC); to DOC complexity (as measured by specific ultraviolet absorbance); and to percent wetland in the stream basins. Correlations were strongest for nonurban streams. Although regressions of log[Hg] versus δ 15 N indicate that Hg in biota increased significantly with increasing trophic position within seven of eight individual streams, Hg concentrations in top predator fish (including cutthroat, rainbow, and brown trout; green sunfish; and largemouth bass) were not strongly influenced by differences in relative trophic position. Slopes of log[Hg] versus δ 15 N, an indicator of the efficiency of trophic enrichment, ranged from 0.14 to 0.27 for all streams. These data suggest that, across the large ranges in FTHg (0.14−14.2 ng L −1 ), FMeHg (0.023−1.03 ng L −1 ), and DOC (0.50−61.0 mg L −1 ) found in this study, Hg contamination in top predator fish in streams likely is dominated by the amount of MeHg available for uptake at the base of the food web rather than by differences in the trophic position of top predator fish.

Environmental Science & Technology↗
USGS2009

Fate of sulfamethoxazole, 4-nonylphenol, and 17β-estradiol in groundwater contaminated by wastewater treatment plant effluent

Organic wastewater contaminants (OWCs) were measured in samples collected from monitoring wells located along a 4.5-km transect of a plume of groundwater contaminated by 60 years of continuous rapid infiltration disposal of wastewater treatment plant effluent. Fifteen percent of the 212 OWCs analyzed were detected, including the antibiotic sulfamethoxazole (SX), the nonionic surfactant degradation product 4-nonylphenol (NP), the solvent tetrachloroethene (PCE), and the disinfectant 1,4-dichlorobenzene (DCB). Comparison of the 2005 sampling results to data collected from the same wells in 1985 indicates that PCE and DCB are transported more rapidly in the aquifer than NP, consistent with predictions based on compound hydrophobicity. Natural gradient in situ tracer experiments were conducted to evaluate the subsurface behavior of SX, NP, and the female sex hormone 17&beta;-estradiol (E2) in two oxic zones in the aquifer: (1) a downgradient transition zone at the interface between the contamination plume and the overlying uncontaminated groundwater and (2) a contaminated zone located beneath the infiltration beds, which have not been loaded for 10 years. In both zones, breakthrough curves for the conservative tracer bromide (Br &minus; ) and SX were nearly coincident, whereas NP and E2 were retarded relative to Br &minus; and showed mass loss. Retardation was greater in the contaminated zone than in the transition zone. Attenuation of NP and E2 in the aquifer was attributed to biotransformation, and oxic laboratory microcosm experiments using sediments from the transition and contaminated zones show that uniform-ring-labeled 14 C 4-normal-NP was biodegraded more rapidly (30&minus;60% recovered as 14 CO 2 in 13 days) than 4- 14 C E2 (20&minus;90% recovered as 14 CO 2 in 54 days). There was little difference in mineralization potential between sites.

Massachusetts↗
USGS2009

Semivolatile organic compounds in residential air along the Arizona - Mexico border

Concerns about indoor air quality and the potential effects on people living in these environments are increasing as more reports about the toxicities and the potential indoor air exposure levels of household-use chemicals and chemicals fromhousingandfurnishingmanufactureinairarebeingassessed. Gas chromatography/mass spectrometry was used to confirm numerous airborne contaminants obtained from the analysis of semipermeable membrane devices deployed inside of 52 homes situated along the border between Arizona and Mexico. We also describe nontarget analytes in the organochlorine pesticide fractions of 12 of these homes; this fraction is also the most likelytocontainthebroadestscopeofbioconcentratablechemicals accumulated from the indoor air. Approximately 400 individual components were identified, ranging from pesticides to a wide array of hydrocarbons, fragrances such as the musk xylenes, flavors relating to spices, aldehydes, alcohols, esters and phthalate esters, and other miscellaneous types of chemicals. The results presented in this study demonstrate unequivocally that the mixture of airborne chemicals present indoors is far more complex than previously demonstrated. ?? 2009 American Chemical Society.

Environmental Science & Technology↗
USGS2009

Application of a rule-based model to estimate mercury exchange for three background biomes in the continental United States

Ecosystems that have low mercury (Hg) concentrations (i.e., not enriched or impactedbygeologic or anthropogenic processes) cover most of the terrestrial surface area of the earth yet their role as a net source or sink for atmospheric Hg is uncertain. Here we use empirical data to develop a rule-based model implemented within a geographic information system framework to estimate the spatial and temporal patterns of Hg flux for semiarid deserts, grasslands, and deciduous forests representing 45% of the continental United States. This exercise provides an indication of whether these ecosystems are a net source or sink for atmospheric Hg as well as a basis for recommendation of data to collect in future field sampling campaigns. Results indicated that soil alone was a small net source of atmospheric Hg and that emitted Hg could be accounted for based on Hg input by wet deposition. When foliar assimilation and wet deposition are added to the area estimate of soil Hg flux these biomes are a sink for atmospheric Hg. ?? 2009 American Chemical Society.

Environmental Science & Technology↗
USGS2009

Predicting dietborne metal toxicity from metal influxes

Dietborne metal uptake prevails for many species in nature. However, the links between dietary metal exposure and toxicity are not well understood. Sources of uncertainty include the lack of suitable tracers to quantify exposure for metals such as copper, the difficulty to assess dietary processes such as food ingestion rate, and the complexity to link metal bioaccumulation and effects. We characterized dietborne copper, nickel, and cadmium influxes in a freshwater gastropod exposed to diatoms labeled with enriched stable metal isotopes. Metal influxes in Lymnaea stagnalis correlated linearly with dietborne metal concentrations over a range encompassing most environmental exposures. Dietary Cd and Ni uptake rate constants (k uf ) were, respectively, 3.3 and 2.3 times higher than that for Cu. Detoxification rate constants (k detox ) were similar among metals and appeared 100 times higher than efflux rate constants (k e ). Extremely high Cu concentrations reduced feeding rates, causing the relationship between exposure and influx to deviate from linearity; i.e., Cu uptake rates leveled off between 1500 and 1800 nmol g -1 day -1 . L. stagnalis rapidly takes up Cu, Cd, and Ni from food but detoxifies the accumulated metals, instead of reducing uptake or intensifying excretion. Above a threshold uptake rate, however, the detoxification capabilities of L. stagnalis are overwhelmed.

Environmental Science & Technology↗
USGS2009

Emerging opportunities in management of selenium contamination

The metalloid selenium (Se) has the diverse reactivity characteristic of the chalcogens in addition to organometallic behavior. Laboratory measurements indicate that Se is an acute reproductive toxicant, which makes it a concern for the environment. Yet to date, a lack of understanding on how Se species distribute through food webs—bioaccumulation not seeming to conform to dissolved concentrations—has made for very heterogeneous regulation across jurisdictions. In this Feature, Luoma and Presser review Se’s idiosyncrasies to provide an outlook for more realistic ecotoxicologically based regulation.

Environmental Science & Technology↗
USGS2010

Federal land management, carbon sequestration, and climate change in the Southeastern U.S.: a case study with fort benning

Land use activities can have a major impact on the temporal trendsandspatialpatternsofregionalland-atmosphereexchange of carbon. Federal lands generally have substantially different land management strategies from surrounding areas, and the carbon consequences have rarely been quantified and assessed. Using the Fort Benning Installation as a case study, we used the General Ensemble biogeochemical Modeling System (GEMS) to simulate and compare ecosystem carbon sequestration between the U.S. Army's Fort Benning and surrounding areas from 1992 to 2050. Our results indicate that the military installation sequestered more carbon than surrounding areas from 1992 to 2007 (76.7 vs 18.5 g C m -2 yr -1 ), and is projected to continue sequestering more carbon from 2008 to 2050 (75.7 vs 25.6 g C m -2 yr -1 ), mostly because of the proactive management approaches adopted on military training lands. Our results suggest that federal lands might play a positive and important role in sequestering and conserving atmospheric carbon because some anthropogenic disturbances (e.g., urbanization, forest harvesting, and agriculture) can be minimized or prevented on federal lands

Georgia↗
USGS2009

Arsenite and ferrous iron oxidation linked to chemolithotrophic denitrification for the immobilization of arsenic in anoxic environments

The objective of this study was to explore a bioremediation strategy based on injecting NO 3 − to support the anoxic oxidation of ferrous iron (Fe(II)) and arsenite (As(III)) in the subsurface as a means to immobilize As in the form of arsenate (As(V)) adsorbed onto biogenic ferric (Fe(III)) (hydr)oxides. Continuous flow sand filled columns were used to simulate a natural anaerobic groundwater and sediment system with co-occurring As(III) and Fe(II) in the presence (column SF1) or absence (column SF2) of nitrate, respectively. During operation for 250 days, the average influent arsenic concentration of 567 μg L −1 was reduced to 10.6 (±9.6) μg L −1 in the effluent of column SF1. The cumulative removal of Fe(II) and As(III) in SF1 was 6.5 to 10-fold higher than that in SF2. Extraction and measurement of the mass of iron and arsenic immobilized on the sand packing of the columns were close to the iron and arsenic removed from the aqueous phase during column operation. The dominant speciation of the immobilized iron and arsenic was Fe(III) and As(V) in SF1, compared with Fe(II) and As(III) in SF2. The speciation was confirmed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The results indicate that microbial oxidation of As(III) and Fe(II) linked to denitrification resulted in the enhanced immobilization of aqueous arsenic in anaerobic environments by forming Fe(III) (hydr)oxide coated sands with adsorbed As(V).

Environmental Science & Technology↗