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USGS2005

Trends in hydrophobic organic contaminants in urban and reference lake sediments across the United States, 1970-2001

A shift in national policy toward stronger environmental protection began in the United States in about 1970. Conversely, urban land use, population, energy consumption, and vehicle use have increased greatly since then. To assess the effects of these changes on water quality, the U.S. Geological Survey used sediment cores to reconstruct water-quality histories for38 urban and reference lakes across the United States. Cores were age-dated, and concentration profiles of polycyclic aromatic hydrocarbons (PAHs) and chlorinated hydrocarbons were tested statistically. Significant trends in total DDT, p,p???-DDE, and total PCBs were all downward. Trends in chlordane were split evenly between upward and downward, and trends in PAHs were mostly upward. Significant trends did not occur in about one-half of cases tested. Concentrations of p,p???-DDE, p,p???-DDD, and PCBs were about one-half as likely to exceed the probable effect concentration (PEC), a sediment quality guideline, in sediments deposited in the 1990s as in 1965-1975, whereas PAHs were twice as likely to exceed the PEC in the more recently deposited sediments. Concentrations of all contaminants evaluated correlated strongly with urban land use. Upward trends in PAH concentrations, the strong association of PAH with urban settings, and rapid urbanization occurring in the United States suggest that PAHs could surpass chlorinated hydrocarbons in the threat they pose to aquatic biota in urban streams and lakes.

Environmental Science & Technology↗
USGS2005

Inhibition of calcite precipitation by natural organic material: Kinetics, mechanism, and thermodynamics

The inhibition of calcite precipitation by natural organic material (NOM) in solutions seeded with calcite was investigated using a pH-stat system. Experiments were carried out using three NOMs with different physical/chemical properties. For each of the materials, inhibition was found to be more effective at lower carbonate/calcium ratios and lower pH values. The reduction in the precipitation rate could be explained by a Langmuir adsorption model using a conditional equilibrium constant. By identification of the type of site on the NOM molecules that is involved in the adsorption reaction, the "conditional" equilibrium constants obtained at different solution compositions converged to a single "nonconditional" value. The thermodynamic data determined at 25??C and 1 atm suggest that the interaction between NOM molecules and the calcite surface is chemisorptive in nature and that adsorption is an endothermic reaction driven by the entropy change. The greatest degree of inhibition was observed for the NOM with the highest molecular weight and aromatic carbon content. For a given type of NOM, the degree of inhibition of calcite precipitation was dictated by the balance between the enthalpy change and the entropy change of the adsorption reaction. ?? 2005 American Chemical Society.

Environmental Science & Technology↗
USGS2005

Sorption of aromatic organic pollutants to grasses from water

The influence of plant lipids on the equilibrium sorption of three aromatic solutes from water was studied. The plant-water sorption isotherms of benzene, 1,2-dichlorobenzene, and phenanthrene were measured over a large range of solute concentrations using sealed vessels containing water, dried plant material, and solute. The plant materials studied include the shoots of annual rye, tall fescue, red fescue, and spinach as well as the roots of annual rye. Seven out of eight sorption isotherms were linear with no evidence of competitive effects between the solutes. For a given plant type, the sorption coefficient increased with decreasing solute water solubility. For a given solute, sorption increased with increasing plant lipid content. The estimated lipid-water partition coefficients of individual solutes were found to be significantly greater than the corresponding octanol-water partition coefficients. This indicates that plant lipids are a more effective partition solvent than octanol for the studied aromatic compounds. As expected, the solute lipid-water partition coefficients were log-linearly related to the respective water solubilities. For the compounds studied, partitioning into the lipids is believed to be the primary sorption mechanism. ?? 2005 American Chemical Society.

Environmental Science & Technology↗
USGS2005

Mass balance assessment for mercury in Lake Champlain

A mass balance model for mercury in Lake Champlain was developed in an effort to understand the sources, inventories, concentrations, and effects of mercury (Hg) contamination in the lake ecosystem. To construct the mass balance model, air, water, and sediment were sampled as a part of this project and other research/monitoring projects in the Lake Champlain Basin. This project produced a STELLA-based computer model and quantitative apportionments of the principal input and output pathways of Hg for each of 13 segments in the lake. The model Hg concentrations in the lake were consistent with measured concentrations. Specifically, the modeling identified surface water inflows as the largest direct contributor of Hg into the lake. Direct wet deposition to the lake was the second largest source of Hg followed by direct dry deposition. Volatilization and sedimentation losses were identified as the two major removal mechanisms. This study significantly improves previous estimates of the relative importance of Hg input pathways and of wet and dry deposition fluxes of Hg into Lake Champlain. It also provides new estimates of volatilization fluxes across different lake segments and sedimentation loss in the lake. ?? 2006 American Chemical Society.

Environmental Science & Technology↗
USGS2005

Biogeochemical controls on diel cycling of stable isotopes of dissolved 02 and dissolved inorganic carbon in the Big Hole River, Montana

Rivers with high biological productivity typically show substantial increases in pH and dissolved oxygen (DO) concentration during the day and decreases at night, in response to changes in the relative rates of aquatic photosynthesis and respiration. These changes, coupled with temperature variations, may impart diel (24-h) fluctuations in the concentration of trace metals, nutrients, and other chemical species. A better understanding of diel processes in rivers is needed and will lead to improved methods of data collection for both monitoring and research purposes. Previous studies have used stable isotopes of dissolved oxygen (DO) and dissolved inorganic carbon (DIC) as tracers of geochemical and biological processes in streams, lakes, and marine systems. Although seasonal variation in δ 18 O of DO in rivers and lakes has been documented, no study has investigated diel changes in this parameter. Here, we demonstrate large (up to 13‰) cycles in δ 18 O-DO for two late summer sampling periods in the Big Hole River of southwest Montana and illustrate that these changes are correlated to variations in the DO concentration, the C-isotopic composition of DIC, and the primary productivity of the system. The magnitude of the diel cycle in δ 18 O-DO was greater in August versus September because of the longer photoperiod and warmer water temperatures. This study provides another biogeochemical tool for investigating the O 2 and C budgets in rivers and may also be applicable to lake and groundwater systems.

Montana↗
USGS2005

Assessing the potential for re-emission of mercury deposited in precipitation from arid soils using a stable isotope

A solution containing 198 Hg in the form of HgCl 2 was added to a 4 m 2 area of desert soils in Nevada, and soil Hg fluxes were measured using three dynamic flux chambers. There was an immediate release of 198 Hg after it was applied, and then emissions decreased exponentially. Within the first 6 h after the isotope was added to the soil, ∼12 ng m - 2 of 198 Hg was emitted to the atmosphere, followed by a relatively steady flux of the isotope at 0.2 ± 0.2 ng m - 2 h - 1 for the remainder of the experiment (62 days). Over this time, ∼200 ng m - 2 or 2% of the 198 Hg isotope was emitted from the soil, and we estimate that ∼6% of the isotope would be re-emitted in a year's time. During the experiment, dry deposition of elemental Hg from the atmosphere was measured with an average deposition rate of 0.2 ± 0.1 ng m - 2 h - 1 . Emission of ambient Hg from the soil was observed after soil wetting with the isotope solution and after a storm event. However, the added moisture from the storm event did not affect 198 Hg flux. Results suggest that in this desert environment, where there is limited precipitation, Hg deposited by wet processes is not readily re-emitted and that dry deposition of elemental Hg may be an important process.

Environmental Science & Technology↗
USGS2005

Murre eggs ( Uria aalge and Uria lomvia ) as indicators of mercury contamination in the Alaskan marine environment

Sixty common murre ( Uria aalge ) and 27 thick-billed murre ( Uria lomvia ) eggs collected by the Seabird Tissue Archival and Monitoring Project (STAMP) in 1999−2001 from two Gulf of Alaska and three Bering Sea nesting colonies were analyzed for total mercury (Hg) using isotope dilution cold vapor inductively coupled mass spectrometry. Hg concentrations (wet mass) ranged from 0.011 μg/g to 0.357 μg/g (relative standard deviation = 76%), while conspecifics from the same colonies and years had an average relative standard deviation of 33%. Hg levels in eggs from the Gulf of Alaska (0.166 μg/g ± 0.011 μg/g) were significantly higher ( p < 0.0001) than in the Bering Sea (0.047 μg/g ± 0.004 μg/g). Within the Bering Sea, Hg was significantly higher ( p = 0.0007) in eggs from Little Diomede Island near the arctic than at the two more southern colonies. Although thick-billed and common murres are ecologically similar, there were significant species differences in egg Hg concentrations within each region ( p < 0.0001). In the Bering Sea, eggs from thick-billed murres had higher Hg concentrations than eggs from common murres, while in the Gulf of Alaska, common murre eggs had higher concentrations than those of thick-billed murres. A separate one-way analysis of variance on the only time−trend data currently available for a colony (St. Lazaria Island in the Gulf of Alaska) found significantly lower Hg concentrations in common murre eggs collected in 2001 compared to 1999 ( p = 0.017). Results from this study indicate that murre eggs may be effective monitoring units for detecting geographic, species, and temporal patterns of Hg contamination in marine food webs. The relatively small intracolony variation in egg Hg levels and the ability to consistently obtain adequate sample sizes both within and among colonies over a large geographic range means that monitoring efforts using murre eggs will have suitable statistical power for detecting environmental patterns of Hg contamination. The potential influences of trophic effects, physical transport patterns, and biogeochemical processes on these monitoring efforts are discussed, and future plans to investigate the sources of the observed variability are presented.

Environmental Science & Technology↗
USGS2005

Chemical loading into surface water along a hydrological, biogeochemical, and land use gradient: A holistic watershed approach

Identifying the sources and impacts of organic and inorganic contaminants at the watershed scale is a complex challenge because of the multitude of processes occurring in time and space. Investigation of geochemical transformations requires a systematic evaluation of hydrologic, landscape, and anthropogenic factors. The 1160 km 2 Boulder Creek Watershed in the Colorado Front Range encompasses a gradient of geology, ecotypes, climate, and urbanization. Streamflow originates primarily as snowmelt and shows substantial annual variation. Water samples were collected along a 70-km transect during spring-runoff and base-flow conditions, and analyzed for major elements, trace elements, bulk organics, organic wastewater contaminants (OWCs), and pesticides. Major-element and trace-element concentrations were low in the headwaters, increased through the urban corridor, and had a step increase downstream from the first major wastewater treatment plant (WWTP). Boron, gadolinium, and lithium were useful inorganic tracers of anthropogenic inputs. Effluent from the WWTP accounted for as much as 75% of the flow in Boulder Creek and was the largest chemical input. Under both hydrological conditions, OWCs and pesticides were detected in Boulder Creek downstream from the WWTP outfall as well as in the headwater region, and loads of anthropogenic-derived contaminants increased as basin population density increased. This report documents a suite of potential endocrine-disrupting chemicals in a reach of stream with native fish populations showing indication of endocrine disruption.

Environmental Science & Technology↗
USGS2005

Accumulation of contaminants in fish from wastewater treatment wetlands

Increasing demands on water resources in arid environments make reclamation and reuse of municipal wastewater an important component of the water budget. Treatment wetlands can be an integral part of the water-reuse cycle providing both water-quality enhancement and habitat functions. When used for habitat, the bioaccumulation potential of contaminants in the wastewater is a critical consideration. Water and fish samples collected from the Tres Rios Demonstration Constructed Wetlands near Phoenix, Arizona, which uses secondary-treated wastewater to maintain an aquatic ecosystem in a desert environment, were analyzed for hydrophobic organic compounds (HOC) and trace elements. Semipermeable membrane devices (SPMD) were deployed to investigate uptake of HOC. The wetlands effectively removed HOC, and concentrations of herbicides, pesticides, and organic wastewater contaminants decreased 40−99% between inlet and outlet. Analysis of Tilapia mossambica and Gambusia affinis indicated accumulation of HOC, including p,p ‘-DDE and trans -nonachlor. The SPMD accumulated the HOC detected in the fish tissue as well as additional compounds. Trace-element concentrations in whole-fish tissue were highly variable, but were similar between the two species. Concentrations of HOC and trace elements varied in different fish tissue compartments, and concentrations in Tilapia liver tissue were greater than those in the whole organism or filet tissue. Bioconcentration factors for the trace elements ranged from 5 to 58 000 and for the HOC ranged from 530 to 150 000.

Environmental Science & Technology↗
USGS2006

Long-term natural attenuation of carbon and nitrogen within a groundwater plume after removal of the treated wastewater source

Disposal of treated wastewater for more than 60 years onto infiltration beds on Cape Cod, Massachusetts produced a groundwater contaminant plume greater than 6 km long in a surficial sand and gravel aquifer. In December 1995 the wastewater disposal ceased. A long-term, continuous study was conducted to characterize the post-cessation attenuation of the plume from the source to 0.6 km downgradient. Concentrations and total pools of mobile constituents, such as boron and nitrate, steadily decreased within 1-4 years along the transect. Dissolved organic carbon loads also decreased, but to a lesser extent, particularly downgradient of the infiltration beds. After 4 years, concentrations and pools of carbon and nitrogen in groundwater were relatively constant with time and distance, but substantially elevated above background. The contaminant plume core remained anoxic for the entire 10-year study period; temporal patterns of integrated oxygen deficit decreased slowly at all sites. In 2004, substantial amounts of total dissolved carbon (7 mol C m-2) and fixed (dissolved plus sorbed) inorganic nitrogen (0.5 mol N m-2) were still present in a 28-m vertical interval at the disposal site. Sorbed constituents have contributed substantially to the dissolved carbon and nitrogen pools and are responsible for the long-term persistence of the contaminant plume. Natural aquifer restoration at the discharge location will take at least several decades, even though groundwater flow rates and the potential for contaminant flushing are relatively high.

Environmental Science & Technology↗
USGS2006

Evaluation of the factors controlling the time-dependent inactivation rate coefficients of bacteriophage MS2 and PRD1

Static and dynamic batch experiments were conducted to study the effects of temperature and the presence of sand on the inactivation of bacteriophage MS2 and PRD1. The experimental data suggested that the inactivation process can be satisfactorily represented by a pseudo-first-order expression with time-dependent rate coefficients. The time-dependent rate coefficients were used to determine pertinent thermodynamic properties required for the analysis of the molecular processes involved in the inactivation of each bacteriophage. A combination of high temperature and the presence of sand appears to produce the greatest disruption to the surrounding protein coat of MS2. However, the lower activation energies for PRD1 indicate a weaker dependence of the inactivation rate on temperature. Instead, the presence of air-liquid and air-solid interfaces appears to produce the greatest damage to specific viral components that are related to infection. These results indicate the importance of using thermodynamic parameters based on the time-dependent inactivation model to better predict the inactivation of viruses in groundwater. ?? 2006 American Chemical Society.

Environmental Science & Technology↗
USGS2006

Regional Kendall test for trend

Trends in environmental variables are often investigated within a study region at more than one site. At each site, a trend analysis determines whether a trend has occurred. Yet often also of interest is whether a consistent trend is evident throughout the entire region. This paper adapts the Seasonal Kendall trend test to determine whether a consistent regional trend occurs in environmental variables.

Environmental Science & Technology↗
USGS2006

Perchlorate in pleistocene and holocene groundwater in North-Central New Mexico

Groundwater from remote parts of the Middle Rio Grande Basin in north-central New Mexico has perchlorate (ClO 4 - ) concentrations of 0.12−1.8 μg/L. Because the water samples are mostly preanthropogenic in age (0−28 000 years) and there are no industrial sources in the study area, a natural source of the ClO 4 - is likely. Most of the samples have Br - , Cl - , and SO 4 2 - concentrations that are similar to those of modern bulk atmospheric deposition with evapotranspiration (ET) factors of about 7−40. Most of the ET values for Pleistocene recharge were nearly twice that for Holocene recharge. The NO 3 - /Cl - and ClO 4 - /Cl - ratios are more variable than those of Br - /Cl - or SO 4 2 - /Cl - . Samples thought to have recharged under the most arid conditions in the Holocene have relatively high NO 3 - /Cl - ratios and low δ 15 N values (+1 per mil (‰)) similar to those of modern bulk atmospheric N deposition. The δ 18 O values of the NO 3 - (−4 to 0 ‰) indicate that atmospheric NO 3 - was not transmitted directly to the groundwater but may have been cycled in the soils before infiltrating. Samples with nearly atmospheric NO 3 - /Cl - ratios have relatively high ClO 4 - concentrations (1.0−1.8 μg/L) with a nearly constant ClO 4 - /Cl - mole ratio of (1.4 ± 0.1) × 10 - 4 , which would be consistent with an average ClO 4 - concentration of 0.093 ± 0.005 μg/L in bulk atmospheric deposition during the late Holocene in north-central NM. Samples thought to have recharged under wetter conditions have higher δ 15 N values (+3 to +8 ‰), lower NO 3 - /Cl - ratios, and lower ClO 4 - /Cl - ratios than the ones most likely to preserve an atmospheric signal. Processes in the soils that may have depleted atmospherically derived NO 3 - also may have depleted ClO 4 - to varying degrees prior to recharge. If these interpretations are correct, then ClO 4 - concentrations of atmospheric origin as high as 4 μg/L are possible in preanthropogenic groundwater in parts of the Southwest where ET approaches a factor of 40. Higher ClO 4 - concentrations in uncontaminated groundwater could occur in recharge beneath arid areas where ET is greater than 40, where long-term accumulations of atmospheric salts are leached suddenly from dry soils, or where other (nonatmospheric) natural sources of ClO 4 - exist.

Environmental Science & Technology↗
USGS2006

Evidence for the aquatic binding of arsenate by natural organic matter-suspended Fe(III)

Dialysis experiments with arsenate and three different NOM samples amended with Fe(III) showed evidence confirming the formation of aquatic arsenate-Fe(III)-NOM associations. A linear relationship was observed between the amount of complexed arsenate and the Fe(III) content of the NOM. The dialysis results were consistent with complex formation through ferric iron cations acting as bridges between the negatively charged arsenate and NOM functional groups and/or a more colloidal association, in which the arsenate is bound by suspended Fe(III)-NOM colloids. Sequential filtration experiments confirmed that a significant proportion of the iron present at all Fe/C ratios used in the dialysis experiments was colloidal in nature. These colloids may include larger NOM species that are coagulated by the presence of chelated Fe(III) and/or NOM-stabilized ferric (oxy)hydroxide colloids, and thus, the solution-phase arsenate-Fe(III)-NOM associations are at least partially colloidal in nature. ?? 2006 American Chemical Society.

Environmental Science & Technology↗
USGS2006

Modeling the probability of arsenic in groundwater in New England as a tool for exposure assessment

We developed a process-based model to predict the probability of arsenic exceeding 5 ??g/L in drinking water wells in New England bedrock aquifers. The model is being used for exposure assessment in an epidemiologic study of bladder cancer. One important study hypothesis that may explain increased bladder cancer risk is elevated concentrations of inorganic arsenic in drinking water. In eastern New England, 20-30% of private wells exceed the arsenic drinking water standard of 10 micrograms per liter. Our predictive model significantly improves the understanding of factors associated with arsenic contamination in New England. Specific rock types, high arsenic concentrations in stream sediments, geochemical factors related to areas of Pleistocene marine inundation and proximity to intrusive granitic plutons, and hydrologic and landscape variables relating to groundwater residence time increase the probability of arsenic occurrence in groundwater. Previous studies suggest that arsenic in bedrock groundwater may be partly from past arsenical pesticide use. Variables representing historic agricultural inputs do not improve the model, indicating that this source does not significantly contribute to current arsenic concentrations. Due to the complexity of the fractured bedrock aquifers in the region, well depth and related variables also are not significant predictors. ?? 2006 American Chemical Society.

Environmental Science & Technology↗
USGS2006

Anaerobic biotransformation of roxarsone and related N-substituted phenylarsonic acids

Large quantities of arsenic are introduced into the environment through land application of poultry litter containing the organoarsenical feed additive roxarsone (3-nitro-4-hydroxyphenylarsonic acid). The objective of this study was to evaluate the bioconversion of roxarsone and related N-substituted phenylarsonic acid derivatives under anaerobic conditions. The results demonstrate that roxarsone is rapidly transformed in the absence of oxygen to the corresponding aromatic amine, 4-hydroxy-3-aminophenylarsonic acid (HAPA). The formation of HAPA is attributable to the facile reduction of the nitro group. Electron-donating substrates, such as hydrogen gas, glucose, and lactate, stimulated the rate of nitro group reduction, indicating a microbial role. During long-term incubations, HAPA and the closely related 4-aminophenylarsonic acid (4-APA) were slowly biologically eliminated by up to 99% under methanogenic and sulfate-reducing conditions, whereas little or no removal occurred in heat-killed inoculum controls. Arsenite and, to a lesser extent, arsenate were observed as products of the degradation. Freely soluble forms of the inorganic arsenical species accounted for 19-28% of the amino-substituted phenylarsonic acids removed. This constitutes the first report of a biologically catalyzed rupture of the phenylarsonic group under anaerobic conditions. ?? 2006 American Chemical Society.

Environmental Science & Technology↗
USGS2006

Characterization of aircraft deicer and anti-icer components and toxicity in airport snowbanks and snowmelt runoff

Snowbank samples were collected from snowbanks within a medium-sized airport for four years to characterize aircraft deicer and anti-icer (ADAF) components and toxicity. Concentrations of ADAF components varied with median glycol concentrations from individual sampling periods ranging from 65 to 5940 mg/L. Glycol content in snowbanks ranged from 0.17 to 11.4% of that applied to aircraft. Glycol, a freezing point depressant, was selectively removed during melt periods before snow and ice resulting in lower glycol concentrations after melt periods. Concentrations of ADAF components in airport runoff were similar during periods of snowmelt as compared to active ADAF application periods; however, due to the long duration of snowmelt events, greater masses of glycol were transported during snowmelt events. Alkylphenol ethoxylates (APEO), selected APEO degradation products, and 4- and 5-methyl-1H-benzotriazole were detected in snowbank samples and airport snowmelt. Concentrations of APEO parent products were greater in snowbank samples than in runoff samples. Relative abundance of APEO degradation products increased in the downstream direction from the snowbank to the outfalls and the receiving stream with respect to APEO parent compounds and glycol. Toxicity in Microtox assays remained in snowbanks after most glycol had been removed during melt periods. Increased toxicity in airport snowbanks as compared to other urban snowbanks was not explained by additional combustion or fuel contribution in airport snow. Organic markers suggest ADAF additives as a possible explanation for this increased toxicity. Results indicate that glycol cannot be used as a surrogate for fate and transport of other ADAF components. ?? 2006 American Chemical Society.

Environmental Science & Technology↗
USGS2006

Widespread presence of naturally occurring perchlorate in high plains of Texas and New Mexico

Perchlorate (ClO4-) occurrence in groundwater has previously been linked to industrial releases and the historic use of Chilean nitrate fertilizers. However, recently a number of occurrences have been identified for which there is no obvious anthropogenic source. Groundwater from an area of 155 000 km2 in 56 counties in northwest Texas and eastern New Mexico is impacted by the presence of ClO4-. Concentrations were generally low (<4 ppb), although some areas are impacted by concentrations up to 200 ppb. ClO4- distribution is not related to well type (public water system, domestic, agricultural, or water-table monitoring) or aquifer (Ogallala, Edward Trinity High Plains, Edwards Trinity Plateau, Seymour, or Cenozoic). Results from vertically nested wells strongly indicate a surface source. The source of ClO4- appears to most likely be atmospheric deposition. Evidence supporting this hypothesis primarily relates to the presence of ClO 4- in tritium-free older water, the lack of relation between land use and concentration distribution, the inability of potential anthropogenic sources to account for the estimated mass of ClO4-, and the positive relationship between conserved anions (e.g., IO3-, Cl-, SO4-2) and ClO4-. The ClO4- distribution appears to be mainly related to evaporative concentration and unsaturated transport. This process has led to higher ClO4- and other ion concentrations in groundwater where the water table is relatively shallow, and in areas with lower saturated thickness. Irrigation may have accelerated this process in some areas by increasing the transport of accumulated salts and by increasing the number of evaporative cycles. Results from this study highlight the potential for ClO4- to impact groundwater in arid and semiarid areas through long-term atmospheric deposition. ?? 2006 American Chemical Society.

Environmental Science & Technology↗