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USGS2009

Spatial pattern of groundwater arsenic occurrence and association with bedrock geology in greater augusta, maine

In New England, groundwater arsenic occurrence has been linked to bedrock geology on regional scales. To ascertain and quantify this linkage at intermediate (10 0 -10 1 km) scales, 790 groundwater samples from fractured bedrock aquifers in the greater Augusta, Maine area are analyzed, and 31% of the sampled wells have arsenic concentrations >10 ??g/L. The probability of [As] exceeding 10 ??g/L mapped by indicator kriging is highest in Silurian pelite-sandstone and pelite-limestone units (???40%). This probability differs significantly (p < 0.001) from those in the Silurian - Ordovician sandstone (24%), the Devonian granite (15%), and the Ordovician - Cambrian volcanic rocks (9%). The spatial pattern of groundwater arsenic distribution resembles the bedrock map. Thus, bedrock geology is associated with arsenic occurrence in fractured bedrock aquifers of the study area at intermediate scales relevant to water resources planning. The arsenic exceedance rate for each rock unit is considered robust because low, medium, and high arsenic occurrences in four cluster areas (3-20 km 2 ) with a low sampling density of 1-6 wells per km 2 are comparable to those with a greater density of 5-42 wells per km 2 . About 12,000 people (21% of the population) in the greater Augusta area (???1135 km 2 ) are at risk of exposure to >10 ??g/L arsenic in groundwater. ?? 2009 American Chemical Society.

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 17β-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 − ) and SX were nearly coincident, whereas NP and E2 were retarded relative to Br − 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 (30−60% recovered as 14 CO 2 in 13 days) than 4- 14 C E2 (20−90% recovered as 14 CO 2 in 54 days). There was little difference in mineralization potential between sites.

Massachusetts↗

USGS2009

Using oxygen isotopes of phosphate to trace phosphorus sources and cycling in lake Erie

Water samples collected during three sampling trips to Lake Erie displayed oxygen isotopic values of dissolved phosphate (δ 18 O p ) that were largely out of equilibrium with ambient conditions, indicating that source signatures may be discerned. δ 18 O p values in the Lake ranged from +10‰ to +17‰, whereas the equilibrium value was expected to be around +14‰. The riverine weighted average δ 18 O p value was +11‰ and may represent one source of phosphate to the Lake. The lake δ 18 O p values indicated that there must be one or more as yet uncharacterized source(s) of phosphate with a high δ 18 O p value. Potential sources other than rivers are not yet well-characterized with respect to δ 18 O of phosphate, but we speculate that a likely source may be the release of phosphate from sediments under reducing conditions created during anoxic events in the hypolimnion of the central basin of Lake Erie. Identifying potential phosphorus sources to the Lake is vital for designing effective management plans for reducing nutrient inputs and associated eutrophication.

Environmental Science & Technology↗

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

Regional nutrient trends in streams and rivers of the United States, 1993-2003

Trends in flow-adjusted concentrations (indicators of anthropogenic changes) and observed concentrations (indicators of natural and anthropogenic changes) of total phosphorus and total nitrogen from 1993 to 2003 were evaluated in the eastern, central, and western United States by adapting the Regional Kendall trend test to account for seasonality and spatial correlation. The only significant regional trend was an increase in flow-adjusted concentrations of total phosphorus in the central United States, which corresponded to increases in phosphorus inputs from fertilizer in the region, particularly west of the Mississippi River. A similar upward regional trend in observed total phosphorus concentrations in the central United States was not found, likely because precipitation and runoff decreased during drought conditions in the region, offsetting the increased source loading on the land surface. A greater number of regional trends would have been significant if spatial correlation had been disregarded, indicating the importance of spatial correlation modifications in regional trend assessments when sites are not spatially independent.

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

PCBs and DDE in tree swallow ( Tachycineta bicolor ) eggs and nestlings from an estuarine PCB superfund site, New Bedford Harbor, MA, U.S.A.

While breeding tree swallows ( Tachycineta bicolor ) have been used as biomonitors for freshwater sites, we report the first use of this species to assess contaminant bioaccumulation from estuarine breeding grounds into these aerial insectivores. Eggs and nestlings were collected from nest boxes in a polychlorinated biphenyl (PCB) contaminated estuary, the New Bedford Harbor Superfund site (NBH, Massachusetts, USA), and a reference salt marsh, Fox Hill (FH, Jamestown, Rhode Island, USA). Sediments, eggs, and nestlings were compared on a ng g −1 wet weight basis for total PCBs and DDE (1,1- bis -(4-chlorophenyl)-2,2-dichloroethene), metabolite of DDT (1,1,1-trichloro-2,2- bis -(p-chlorophenyl)ethane). NBH samples contained high concentrations of PCBs compared to FH for sediment (36,500 and 0.2), eggs (11,200 and 323), and nestlings (16,800 and 26). PCB homologue patterns linked tree swallow contamination to NBH sediment. NBH samples were also contaminated with DDE compared to FH for sediment (207 and 0.9) and nestlings (235 and 30) but not for eggs (526 and 488), suggesting both NBH and nonbreeding ground sources for DDE. The relationships between sediment and tree swallow egg and nestling PCBs were similar to those reported for freshwater sites. Like some highly contaminated freshwater sites, NBH PCB bioaccumulation had little apparent effect on reproductive success.

Massachusetts↗

USGS2009

Characterizing the oxygen isotopic composition of phosphate sources to aquatic ecosystems

The oxygen isotopic composition of dissolved inorganic phosphate (δ 18 O p ) in many aquatic ecosystems is not in isotopic equilibrium with ambient water and, therefore, may reflect the source δ 18 O p . Identification of phosphate sources to water bodies is critical for designing best management practices for phosphate load reduction to control eutrophication. In order for δ 18 O p to be a useful tool for source tracking, the δ 18 O p of phosphate sources must be distinguishable from one another; however, the δ 18 O p of potential sources has not been well characterized. We measured the δ 18 O p of a variety of known phosphate sources, including fertilizers, semiprocessed phosphorite ore, particulate aerosols, detergents, leachates of vegetation, soil, animal feces, and wastewater treatment plant effluent. We found a considerable range of δ 18 O p values (from +8.4 to +24.9‰) for the various sources, and statistically significant differences were found between several of the source types. δ 18 O p measured in three different fresh water systems was generally not in equilibrium with ambient water. Although there is overlap in δ 18 O p values among the groups of samples, our results indicate that some sources are isotopically distinct and δ 18 O p can be used for identifying phosphate sources to aquatic systems.

Environmental Science & Technology↗

USGS2009

Inputs of fossil carbon from wastewater treatment plants to U.S. Rivers and oceans

Every day more than 500 million cubic meters of treated wastewater are discharged into rivers, estuaries, and oceans, an amount slightly less than the average flow of the Danube River. Typically, wastewaters have high organic carbon (OC) concentrations and represent a large fraction of total river flow and a higher fraction of river OC in densely populated watersheds. Here, we report the first direct measurements of radiocarbon ( 14 C) in municipal wastewater treatment plant (WWTP) effluent. The radiocarbon ages of particulate and dissolved organic carbon (POC and DOC) in effluent are old and relatively uniform across a range of WWTPs in New York and Connecticut. Wastewater DOC has a mean radiocarbon age of 1630 ?? 500 years B.P. and a mean ?? 13 C of -26.0 ?? 1???. Mass balance calculations indicate that 25% of wastewater DOC is fossil carbon, which is likely derived from petroleumbased household products such as detergents and pharmaceuticals. Thesefindings warrant reevaluation of the "apparent age" of riverine DOC, the total flux of petroleum carbon to U.S. oceans, and OC source assignments in waters impacted by sewage. ?? 2009 American Chemical Society.

Environmental Science & Technology↗

USGS2009

Isotopic variability of mercury in ore, mine-waste calcine, and leachates of mine-waste calcine from areas mined for mercury

The isotopic composition of mercury (Hg) was determined in cinnabar ore, mine-waste calcine (retorted ore), and leachates obtained from water leaching experiments of calcine from two large Hg mining districts in the U.S. This study is the first to report significant mass-dependent Hg isotopic fractionation between cinnabar ore and resultant calcine. Data indicate that ?? 202 Hg values relative to NIST 3133 of calcine (up to 1.52???) in the Terlingua district, Texas, are as much as 3.24??? heavier than cinnabar (-1.72???) prior to retorting. In addition, ?? 202 Hg values obtained from leachates of Terlingua district calcines are isotopically similar to, or as much as 1.17??? heavier than associated calcines, most likely due to leaching of soluble, byproduct Hg compounds formed during ore retorting that are a minor component in the calcines. As a result of the large fractionation found between cinnabar and calcine, and because calcine is the dominant source of Hg contamination from the mines studied, ?? 202 Hg values of calcine may be more environmentally important in these mined areas than the primary cinnabar ore. Measurement of the Hg isotopic composition of calcine is necessary when using Hg isotopes for tracing Hg sources from areas mined for Hg, especially mine water runoff. ?? 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↗

USGS2009

Chlorine-36 as a tracer of perchlorate origin

Perchlorate (ClO 4 − ) is ubiquitous in the environment. It is produced naturally by atmospheric photochemical reactions, and also is synthesized in large quantities for military, aerospace, and industrial applications. Nitrate-enriched salt deposits of the Atacama Desert (Chile) contain high concentrations of natural ClO 4 − , and have been exported worldwide since the mid-1800s for use in agriculture. The widespread introduction of synthetic and agricultural ClO 4 − into the environment has contaminated numerous municipal water supplies. Stable isotope ratio measurements of Cl and O have been applied for discrimination of different ClO 4 − sources in the environment. This study explores the potential of 36 Cl measurements for further improving the discrimination of ClO 4 − sources. Groundwater and desert soil samples from the southwestern United States (U.S.) contain ClO 4 − having high 36 Cl abundances ( 36 Cl/Cl = 3100 × 10 −15 to 28,800 × 10 −15 ), compared with those from the Atacama Desert ( 36 Cl/Cl = 0.9 × 10 −15 to 590 × 10 −15 ) and synthetic ClO 4 − reagents and products ( 36 Cl/Cl = 0.0 × 10 −15 to 40 × 10 −15 ). In conjunction with stable Cl and O isotope ratios, 36 Cl data provide a clear distinction among three principal ClO 4 − source types in the environment of the southwestern U.S.

Environmental Science & Technology↗

USGS2009

Fipronil and its degradates in indoor and outdoor dust

Fipronil is a potent insecticide used for control of termites, fleas, roaches, ants, and other pests. We measured fipronil, fipronil sulfide, and desulfinyl fipronil concentrations in indoor and outdoor dust from 24 residences in Austin, Texas. At least one of these three fipronil compounds was detected in every sample. Fipronil accounted for most of the total fipronil (T-fipronil; fipronil+desulfinyl fipronil+fipronil sulfide), followed by desulfinyl fipronil and fipronil sulfide. Nineteen of 24 samples of indoor dust had T-fipronil concentrations less than 270 ??g/kg; the remaining five had concentrations from 1320 to 14,200 ??g/kg. All three of the residences with a dog on which a flea-control product containing fipronil was used were among the five residences with elevated fipronil concentrations. In outdoor dust, all concentrations of T-fipronil were less than 70??g/kg with one exception (430??g/kg). For every residence, the concentration of T-fipronil in indoor dust exceeded that in outdoor dust, and the median concentration of T-fipronil was 15 times higher indoors than outdoors.

Environmental Science & Technology↗

USGS2009

Surface complexation of carboxylate adheres Cryptosporidium parvum öocysts to the hematite-water interface

The interaction of viable Cryptosporidium parvum öocysts at the hematite (α-Fe 2 O 3 )−water interface was examined over a wide range in solution chemistry using in situ attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy. Spectra for hematite-sorbed öocysts showed distinct changes in carboxylate group vibrations relative to spectra obtained in the absence of hematite, indicative of direct chemical bonding between carboxylate groups and Fe metal centers of the hematite surface. The data also indicate that complexation modes vary with solution chemistry. In NaCl solution, öocysts are bound to hematite via monodentate and binuclear bidentate complexes. The former predominates at low pH, whereas the latter becomes increasingly prevalent with increasing pH. In a CaCl 2 solution, only binuclear bidentate complexes are observed. When solution pH is above the point of zero net proton charge (PZNPC) of hematite, öocyst surface carboxylate groups are bound to the mineral surface via outer-sphere complexes in both electrolyte solutions.

Environmental Science & Technology↗

USGS2009

Rapid changes in small fish mercury concentrations in estuarine wetlands: Implications for wildlife risk and monitoring programs

Small fish are commonly used to assess mercury (Hg) risk to wildlife and monitor Hg in wetlands. However, limited research has evaluated short-term Hg variability in small fish, which can have important implications for monitoring programs and risk assessment. We conducted a time-series study of Hg concentrations in two small fish species representing benthic (longjaw mudsuckers [Gillichthys mirabilis]) and pelagic (threespine sticklebacks [Gasterosteus aculeatus]) food-webs within three wetland habitats in San Francisco Bay Estuary. We simultaneously monitored prey deliveries, nest initiation, and chick hatching dates of breeding Forster's terns (Sterna forsteri), the most abundant nesting piscivore in the region. Mudsuckers and sticklebacks were the predominant prey fish, comprising 36% and 25% of tern diet, and Hg concentrations averaged (geometric mean ?? SE, ??g/g dw) 0.44 ?? 0.01 and 0.68 ?? 0.03, respectively. Fish Hg concentrations varied substantially over time following a quadratic form in both species, increasing 40% between March and May then decreasing 40% between May and July. Importantly, Forster's terns initiated 68% of nests and 31% of chicks hatched during the period of peak Hg concentrations in prey fish. These results illustrate the importance of short-term temporal variation in small fish Hg concentrations for both Hg monitoring programs and assessing wildlife risk.

Environmental Science & Technology↗