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Satellite-aided evaluation of population exposure to air pollution

The Clean Air Act Amendments of 1977 set schedules for states to implement regional, spatial assessments of air quality impacts. Accordingly, the U.S. Environmental Protection Agency recently published guidelines for quantifying population exposure to adverse air quality impact by using air quality and population data by census tracts. Our research complements the EPA guidelines in that it demonstrates the ability to determine population exposure to air pollution through computer processing that utilizes Landsat satellite-derived land use information. Three variables-a 1985 estimate of total suspended particulates for 2-km 2 grid cells, Landsat-derived residential land cover data for 0.45-ha cells, and population totals for census tracts-were spatially registered and cross-tabulated to produce tabular and map products illustrating relative air quality exposure for residential population by 2-km 2 cells. It would cost $20,000 to replicate our analysis for an area similar in size to the 4000-km 2 Portland area. Once completed, the spatially fine, computer-compatible air quality and population data are amenable to the timely and efficient generation of population-at-risk tabular and map information on a continuous or periodic basis.

Oregon↗

A biodynamic understanding of dietborne metal uptake by a freshwater invertebrate

Aquatic organisms accumulate metals from dissolved and particulate phases. Dietborne metal uptake likely prevails in nature, but the physiological processes governing metal bioaccumulation from diet are not fully understood. We characterize dietborne copper, cadmium, and nickel uptake by a freshwater gastropod (Lymnaea stagnalis) both in terms of biodynamics and membrane transport characteristics. We use enriched stable isotopes to trace newly accumulated metals from diet, determine food ingestion rate (IR) and estimate metal assimilation efficiency (AE). Upon 18-h exposure, dietborne metal influx was linear over a range encompassing most environmental concentrations. Dietary metal uptake rate constants (kuf) ranged from 0.104 to 0.162 g g -1 day-1, and appeared to be an expression of transmembrane transport characteristics. Although kuf values were 1000-times lower than uptake rate constants from solution, biodynamic modeling showed that diet is the major Cd, Cu, and Ni source in nature. AE varied slightly among metals and exposure concentrations (84-95%). Suppression of Cd and Cu influxes upon exposure to extreme concentrations coincided with a 10-fold decrease in food IR, suggesting that feeding inhibition could act as an end point for dietary metal toxicity in L. stagnalis.

Environmental Science & Technology↗

Cyanide speciation at four gold leach operations undergoing remediation

Analyses have been made of 81 effluents from four gold leach operations in various stages of remediation to identify the most-persistent cyanide species. Total cyanide and weak acid-dissociable (WAD) cyanide were measured using improved methods, and metals known to form stable cyanocomplexes were also measured. Typically, total cyanide greatly exceeded WAD indicating that cyanide was predominantly in strong cyanometallic complexes. Iron was generally too low to accommodate the strongly complexed cyanide as Fe(CN) 6 3- or Fe(CN) 6 4- , but cobalt was abundant enough to implicate Co(CN) 6 3- or its dissociation products (Co(CN) 6-x (H 2 O) x (3-x)- ). Supporting evidence for cobalt-cyanide complexation was found in tight correlations between cobalt and cyanide in some sample suites. Also, abundant free cyanide was produced upon UV illumination. Iron and cobalt cyanocomplexes both photodissociate; however, the iron concentration was insufficient to have carried the liberated cyanide, while the cobalt concentration was sufficient. Cobalt cyanocomplexes have not previously been recognized in cyanidation wastes. Their identification at four separate operations, which had treated ores that were not especially rich in cobalt, suggests that cobalt complexation may be a common source of cyanide persistence. There is a need for more information on the importance and behavior of cobalt cyanocomplexes in ore-processing wastes at gold mines.

California;Nevada;New Mexico↗

Mercury concentrations in salmonids from western U.S. National Parks and relationships with age and macrophage aggregates

Mercury accumulation in aquatic foodwebs and its effects on aquatic biota are of growing concern both for the health of the fish and the piscivores that prey upon them. This is of particular concern for western U.S. National Parks because it is known that mountainous and Arctic areas are sinks for some contaminants. The Western Airborne Contaminants Assessment Project seeks, in part, to ascertain mercury concentrations and evaluate effects of contaminants on biota in 14 lakes from 8 National Parks or Preserves. In this paper we report that mercury has accumulated to concentrations in trout that may negatively impact some piscivorous wildlife, indicating potential terrestrial ecosystem effects. Additionally, we show that mercury concentrations increase with age in 4 species of trout, providing evidence of bioaccumulation. Finally, we demonstrate that mercury is associated with tissue damage in the kidney and spleen, as indicated by increases in macrophage aggregates. This finding suggests that mercury, and possibly other contaminants, are negatively affecting the trout that inhabit these remote and protected ecosystems. Our results indicate that mercury is indeed a concern for the U.S. National Parks, from an organismic and potentially an ecosystem perspective. ?? 2008 American Chemical Society.

Environmental Science & Technology↗

Atmospherically deposited PBDEs, pesticides, PCBs, and PAHs in western U.S. National Park fish: Concentrations and consumption guidelines

Concentrations of polybrominated diphenyl ethers (PBDEs), pesticides, polychlorinated biphenyls (PCBs), and polycyclic aromatic hydrocarbons were measured in 136 fish from 14 remote lakes in 8 western U.S. National Parks/Preserves between 2003 and 2005 and compared to human and wildlife contaminant health thresholds. A sensitive (median detection limit, -18 pg/g wet weight), efficient (61% recovery at 8 ng/g), reproducible (4.1% relative standard deviation (RSD)), and accurate (7% deviation from standard reference material (SRM)) analytical method was developed and validated for these analyses. Concentrations of PCBs, hexachlorobenzene, hexachlorocyclohexanes, DDTs, and chlordanes in western U.S. fish were comparable to or lower than mountain fish recently collected from Europe, Canada, and Asia. Dieldrin and PBDE concentrations were higher than recent measurements in mountain fish and Pacific Ocean salmon. Concentrations of most contaminants in western U.S. fish were 1-6 orders of magnitude below calculated recreational fishing contaminant health thresholds. However, lake average contaminant concentrations in fish exceeded subsistence fishing cancer thresholds in 8 of 14 lakes and wildlife contaminant health thresholds for piscivorous birds in 1of 14 lakes. These results indicate that atmospherically deposited organic contaminants can accumulate in high elevation fish, reaching concentrations relevant to human and wildlife health. ?? 2008 American Chemical Society.

Environmental Science & Technology↗

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↗

Ecohydrological factors affecting nitrate concentrations in a phreatic desert aquifer in northwestern China

Aerobic conditions in desert aquifers commonly allow high nitrate (NO 3-) concentrations in recharge to persist for long periods of time, an important consideration for N-cycling and water quality. In this study, stable isotopes of NO3- (??15N NO3 and ??18ONO3) were used to trace NO3- cycling processes which affect concentrations in groundwater and unsaturated zone moisture in the arid Badain Jaran Oesert in northwestern China. Most groundwater NO3- appears to be depleted relative to Cl- in rainfall concentrated by evapotranspiration, indicating net N losses. Unsaturated zone NO 3- is generally higher than groundwater NO 3- in terms of both concentration (up to 15 476 ??M, corresponding to 3.6 mg NO3--N per kg sediment) and ratios with Cl-. Isotopic data indicate that the NO3- derives primarily from nitrification, with a minor direct contribution of atmospheric NO3- inferred for some samples, particularly in the unsaturated zone. Localized denitrification in the saturated zone is suggested by isotopic and geochemical indicators in some areas. Anthropogenic inputs appear to be minimal, and variability is attributed to environmental factors. In comparison to other arid regions, the sparseness of vegetation in the study area appears to play an important role in moderating unsaturated zone NO3- accumulation by allowing solute flushing and deterring extensive N2 fixation. ?? 2008 American Chemical Society.

Environmental Science & Technology↗

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↗

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↗

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↗

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↗

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↗

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↗

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↗

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↗

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↗

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↗