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At least 1,135 records · Page 63Linked to original sources
USGS1997

Enhancement and inhibition of microbial activity in hydrocarbon- contaminated arctic soils: Implications for nutrient-amended bioremediation

Bioremediation is being used or proposed as a treatment option at many hydrocarbon-contaminated sites. One such site is a former bulk-fuel storage facility near Barrow, AK, where contamination persists after approximately 380 m3 of JP-5 was spilled in 1970. The soil at the site is primarily coarse sand with low organic carbon (<1%) end low moisture (1-3%) contents. We examined the effects of nutrient additions on microorganisms in contaminated soil from this site in laboratory microcosms and in mesocosms incubated for 6 weeks in the field. Nitrogen was the major limiting nutrient in this system, but microbial populations and activity were maximally enhanced by additions of both nitrogen and phosphorus. When nutrients were added to soil in the field at three levels of N:P (100:45, 200:90, and 300:135 mg/kg soil), the greatest stimulation in microbial activity occurred at the lowest, rather than the highest, level of nutrient addition. The total soil-water potentials ranged from -2 to -15 bar with increasing levels of fertilizer. Semivolatile hydrocarbon concentrations declined significantly only in the soils treated at the low fertilizer level. These results indicate that an understanding of nutrient effects at a specific site is essential for successful bioremediation.Bioremediation is being used or proposed as a treatment option at many hydrocarbon-contaminated sites. One such site is a former bulk-fuel storage facility near Barrow, AK, where contamination persists after approximately 380 m3 of JP-5 was spilled in 1970. The soil at the site is primarily coarse sand with low organic carbon (<1%) and low moisture (1-3%) contents. We examined the effects of nutrient additions on microorganisms in contaminated soil from this site in laboratory microcosms and in mesocosms incubated for 6 weeks in the field. Nitrogen was the major limiting nutrient in this system, but microbial populations and activity were maximally enhanced by additions of both nitrogen and phosphorus. When nutrients were added to soil in the field at three levels of N:P (100:45, 200:90, and 300:135 mg/kg soil), the greatest stimulation in microbial activity occurred at the lowest, rather than the highest, level of nutrient addition. The total soil-water potentials ranged from -2 to -15 bar with increasing levels of fertilizer. Semi-volatile hydrocarbon concentrations declined significantly only in the soils treated at the low fertilizer level. These results indicate that an understanding of nutrient effects at a specific site is essential for successful bioremediation.

Environmental Science & Technology↗
USGS1997

Historical trends in organochlorine compounds in river basins identified using sediment cores from reservoirs

This study used chemical analyses of dated sediment cores from reservoirs to define historical trends in water quality in the influent river basins. This work applies techniques from paleolimnology to reservoirs, and in the process, highlights differences between sediment-core interpretations for reservoirs and natural lakes. Sediment cores were collected from six reservoirs in the central and southeastern United States, sectioned, and analyzed for 137Cs and organochlorine compounds. 137Cs analyses were used to demonstrate limited post-depositional mixing, to indicate sediment deposition dates, and to estimate sediment focusing factors. Relative lack of mixing, high sedimentation rates, and high focusing factors distinguish reservoir sediment cores from cores collected in natural lakes. Temporal trends in concentrations of PCBs, total DDT (DDT + DDD + DDE), and chlordane reflect historical use and regulation of these compounds and differences in land use between reservoir drainages. PCB and total DDT core burdens, normalized for sediment focusing, greatly exceed reported cumulative regional atmospheric fallout of PCBs and total DDT estimated using cores from peat hogs and natural lakes, indicating the dominance of fluvial inputs of both groups of compounds to the reservoirs.This study used chemical analyses of dated sediment cores from reservoirs to define historical trends in water quality in the influent river basins. This work applies techniques from paleolimnology to reservoirs, and in the process, highlights differences between sediment-core interpretations for reservoirs and natural lakes. Sediment cores were collected from six reservoirs in the central and southeastern United States, sectioned, and analyzed for 137Cs and organochlorine compounds. 137Cs analyses were used to demonstrate limited post-depositional mixing, to indicate sediment deposition dates, and to estimate sediment focusing factors. Relative lack of mixing, high sedimentation rates, and high focusing factors distinguish reservoir sediment cores from cores collected in natural lakes. Temporal trends in concentrations of PCBs, total DOT (DDT+DDD+DDE), and chlordane reflect historical use and regulation of these compounds and differences in land use between reservoir drainages. PCB and total DDT core burdens, normalized for sediment focusing, greatly exceed reported cumulative regional atmospheric fallout of PCBs and total DDT estimated using cores from peat bogs and natural lakes, indicating the dominance of fluvial inputs of both groups of compounds to the reservoirs.

Environmental Science & Technology↗
USGS1997

The urban atmosphere as a non-point source for the transport of MTBE and other volatile organic compounds (VOCS) to shallow groundwater

Infiltration and dispersion (including molecular diffusion) can transport volatile organic compounds (VOCs) from urban air into shallow groundwater. The gasoline additive methyl- tert -butyl ether (MTBE) is of special interest because of its (1) current levels in some urban air, (2) strong partitioning from air into water, (3) resistance to degradation, (4) use as an octane-booster since the 1970s, (5) rapidly increasing use in the 1990s to reduce CO and O 3 in urban air, and (6) its frequent detection at low microgram per liter levels in shallow urban groundwater in Denver, New England, and elsewhere. Numerical simulations were conducted using a 1-D model domain set in medium sand (depth to water table = 5 m) to provide a test of whether MTBE and other atmospheric VOCs could move to shallow groundwater within the 10−15 y time frame over which MTBE has now been used in large amounts. Degradation and sorption were assumed negligible. In case 1 (no infiltration, steady atmospheric source), 10 y was not long enough to permit significant VOC movement by diffusion into shallow groundwater. Case 2 considered a steady atmospheric source plus 36 cm/y of net infiltration; groundwater at 2 m below the water table became nearly saturated with atmospheric levels of VOC within 5 y. Case 3 was similar to case 2, but considered the source to be seasonal, being “on” for only 5 of 12 months each year, as with the use of MTBE during the winter fuel-oxygenate season; groundwater at 2 m below the water table became equilibrated with 5 / 12 of the “source-on” concentration within 5 y. Cases 4 and 5 added an evapotranspiration (ET) loss of 36 cm/y, resulting in no net recharge. Case 4 took the ET from the surface, and case 5 took the ET from the capillary fringe at a depth of 3.5 m. Net VOC mass transfer to shallow groundwater after 5 y was less for both cases 4 and 5 than for case 3. However, it was significantly greater for cases 4 and 5 than for case 1, even though cases 1, 4, and 5 were all no-net recharge cases. The mechanism responsible for this effect was the dispersion acting on each downward infiltration event, and also on the ET-induced flow. The ability of MTBE to reach groundwater in cases 2−5 is taken as evidence of the potential importance of urban air as a non-point source for VOCs in shallow urban groundwater. Two subcases were run for both case 4 and case 5: subcase a (water and VOCs move with ET) and subcase b (water only moves with ET).

Environmental Science & Technology↗
USGS1997

Marine bacterial degradation of brominated methanes

Brominated methanes are ozone-depleting compounds whose natural sources include marine algae such as kelp. Brominated methane degradation by bacteria was investigated to address whether bacterial processes might effect net emission of these compounds to the atmosphere. Bacteria in seawater collected from California kelp beds degraded CH2Br2 but not CHBr3. Specific inhibitors showed that methanotrophs and nitrifiers did not significantly contribute to CH2Br2 removal. A seawater enrichment culture oxidized 14CH2Br2 to 14CO2 as well as 14CH3Br to 14CO2. The rates of CH2Br2 degradation in laboratory experiments suggest that bacterial degradation of CH2Br2 in a kelp bed accounts for <1% of the CH2Br2 produced by the kelp. However, the half-life of CH2Br2 due to bacterial removal appears faster than hydrolysis and within an order of magnitude of volatilization to the atmosphere.Brominated methanes are ozone-depleting compounds whose natural sources include marine algae such as kelp. Brominated methane degradation by bacteria was investigated to address whether bacterial processes might effect net emission of these compounds to the atmosphere. Bacteria in seawater collected from California kelp beds degraded CH2Br2 but not CHBr3. Specific inhibitors showed that methanotrophs and nitrifiers did not significantly contribute to CH2Br2 removal. A seawater enrichment culture oxidized 14CH2Br2 to 14CO2 as well as 14CH3Br to 14CO2. The rates of CH2Br2 degradation in laboratory experiments suggest that bacterial degradation of CH2Br2 in a kelp bed accounts for <1% of the CH2Br2 produced by the kelp. However, the half-life of CH2Br2 due to bacterial removal appears faster than hydrolysis and within an order of magnitude of volatilization to the atmosphere.

Environmental Science & Technology↗
USGS1997

Organic carbon and nitrogen content associated with colloids and suspended particulates from the Mississippi River and some of its tributaries

Suspended material samples were collected at 16 sites along the Mississippi River and some of its tributaries during July-August 1991, October-November 1991, and April-May 1992, and separated into colloid and particulate fractions to determine the organic carbon content of these two fractions of suspended material. Sample collection involved centrifugation to isolate the suspended particulate fraction and ultrafiltration to isolate the colloid fraction. For the first time, particulate and colloid concentrations and organic carbon and nitrogen content were investigated along the entire reach of the Mississippi River from above Minneapolis, Minnesota, to below New Orleans, Louisiana. Organic carbon content of the colloid (15.2 percent) was much higher than organic carbon content of the particulate material (4.8 percent). Carbon/nitrogen ratios of colloid and particulate phases were more similar to ratios for microorganisms than to ratios for soils, humic materials, or plants.Suspended material samples were collected at 16 sites along the Mississippi River and some of its tributaries during July-August 1991, October-November 1991, and April-May 1992, and separated into colloid and particulate fractions to determine the organic carbon content of these two fractions of suspended material. Sample collection involved centrifugation to isolate the suspended particulate fraction and ultrafiltration to isolate the colloid fraction. For the first time, particulate and colloid concentrations and organic carbon and nitrogen content were investigated along the entire reach of the Mississippi River from above Minneapolis, Minnesota, to below New Orleans, Louisiana. Organic carbon content of the colloid (15.2 percent) was much higher than organic carbon content of the particulate material (4.8 percent). Carbon/nitrogen ratios of colloid and particulate phases were more similar to ratios for microorganisms than to ratios for soils, humic materials, or plants.

Environmental Science & Technology↗
USGS1997

Groundwater record of halocarbon transport by the Danube River

Groundwater dating studies have supported the concept that aquifers with low coefficients of dispersion may contain coherent records of past conditions in recharge areas. Groundwater records can provide unique information about natural or anthropogenic changes in the atmosphere and hydrosphere where long-term monitoring data are not available. Here we describe a 40-year record of halocarbon contamination in the Danube River that was retrieved from a shallow aquifer in northwest Hungary. The time scale is based on 3H and He isotope dating of groundwaters that were recharged by the Danube River and moved horizontally away from the river in a surficial gravel aquifer with minor dispersion at a maximum rate of at least 500 m/yr. Analyses of dated groundwaters along a flow path indicate that the river loads of selected compounds (including CFC-12, CFC-113, and trichloroethane) were negligible before about 1950, rose rapidly to peak values in the 1960s and 1970s, and then decreased by varying degrees to the present. Peak concentrations are tentatively attributed to point sources in upstream urban-industrial centers; while recent decreases presumably resulted from declining manufacturing rates and(or) improvements in control of urban- industrial runoff and sewage effluent entering the river in upstream areas.

Danube River↗
USGS1998

Occurrence of pesticides in shallow groundwater of the United States: initial results from the National Water-Quality Assessment program

The first phase of intensive data collection for the National Water-Quality Assessment (NAWQA) was completed during 1993&minus;1995 in 20 major hydrologic basins of the United States. Groundwater land-use studies, designed to sample recently recharged groundwater (generally within 10 years) beneath specific land-use and hydrogeologic settings, are a major component of the groundwater quality as sessment for NAWQA. Pesticide results from the 41 land-use studies conducted during 1993&minus;1995 indicate that pesticides were commonly detected in shallow groundwater, having been found at 54.4% of the 1034 sites sampled in agricultural and urban settings across the United States. Pesticide concentrations were generally low, with over 95% of the detections at concentrations less than 1 &mu;g/L. Of the 46 pesticide compounds examined, 39 were detected. The compounds detected most frequently were atrazine (38.2%), deethylatrazine (34.2%), simazine (18.0%), metolachlor (14.6%), and prometon (13.9%). Statistically significant relations were observed between frequencies of detection and the use, mobility, and persistence of these compounds. Pesticides were commonly detected in both agricultural (56.4%; 813 sites) and urban (46.6%; 221 sites) settings. Frequent detections of pesticides in urban areas indicate that, as is the case with agricultural pesticide use in agricultural areas, urban and suburban pesticide use significantly contribute to pesticide occurrence in shallow groundwater. Although pesticides were detected in groundwater sampled in urban areas and all nine of the agricultural land-use categories examined, significant variations in occurrence were observed among these categories. Maximum contaminant levels (MCLs) established by the U.S. Environmental Protection Agency for drinking water were exceeded for only one pesticide (atrazine, 3 &mu;g/L) at a single location. However, MCLs have been established for only 25 of the 46 pesticide compounds examined, do not cover pesticide degradates, and, at present, do not take into account additive or synergistic effects of combinations of pesticide compounds or potential effects on nearby aquatic ecosystems.

Environmental Science & Technology↗
USGS1998

Contribution of hydroxylated atrazine degradation products to the total atrazine load in midwestern streams

The contribution of hydroxylated atrazine degradation products (HADPs) to the total atrazine load (i.e., atrazine plus stable metabolites) in streams needs to be determined in order to fully assess the impact of atrazine contamination on stream ecosystems and human health. The objectives of this study were (1) to determine the contribution of HADPs to the total atrazine load in streams of nine midwestern states and (2) to discuss the mechanisms controlling the concentrations of HADPs in streams. Stream samples were collected from 95 streams in northern Missouri at preplant and postplant of 1994 and 1995, and an additional 46 streams were sampled in eight midwestern states at postplant of 1995. Samples were analyzed for atrazine, deethylatrazine (DEA), deisopropylatrazine (DIA), and three HADPs. Overall, HADP prevalence (i.e., frequency of detection) ranged from 87 to 100% for hydroxyatrazine (HA), 0 to 58% for deethylhydroxyatrazine (DEHA), and 0% for deisopropylhydroxyatrazine (DIHA) with method detection limits of 0.04−0.10 μg L -1 . Atrazine metabolites accounted for nearly 60% of the atrazine load in northern Missouri streams at preplant, with HA the predominant metabolite present. Data presented in this study and a continuous monitoring study are used to support the hypothesis that a combination of desorption from stream sediments and dissolved-phase transport control HADP concentrations in streams.

Environmental Science & Technology↗
USGS1998

Evaluation of microtiter-plate enzyme-linked immunosorbent assay for the analysis of triazine and chloroacetanilide herbicides in rainfall

Triazine and chloroacetanilide concentrations in rainfall samples collected from a 23-state region of the United States were analyzed with microtiter-plate enzyme-linked immunosorbent assay (ELISA). Thirty-six percent of rainfall samples (2072 out of 5691) were confirmed using gas chro matography/mass spectrometry (GC/MS) to evaluate the operating performance of ELISA as a screening test. Comparison of ELISA to GC/MS results showed that the two ELISA methods accurately reported GC/MS results ( m = 1), but with more variability evident with the triazine than with the chloroacetanilide ELISA. Bayes's rule, a standardized method to report the results of screening tests, indicated that the two ELISA methods yielded comparable predictive values (80%), but the triazine ELISA yielded a false-positive rate of 11.8% and the chloroacetanilide ELISA yielded a false-negative rate of 23.1%. The false-positive rate for the triazine ELISA may arise from cross reactivity with an unknown triazine or metabolite. The false-negative rate of the chloroacetanilide ELISA probably resulted from a combination of low sensitivity at the reporting limit of 0.15 μg/L and a distribution characterized by 75% of the samples at or below the reporting limit of 0.15 μg/L.

Environmental Science & Technology↗
USGS1998

Anaerobic benzene oxidation in the Fe(III) reduction zone of petroleum-contaminated aquifers

The potential for anaerobic benzene oxidation in the Fe(III)-reduction zone of petroleum-contaminated aquifers was evaluated. Sediments were incubated under strict anaerobic conditions without any amendments in order to simulate in situ conditions. [ 14 C]Benzene was not oxidized to 14 CO 2 at most sites examined, which is consistent with previous studies that have found that benzene tends to persist in unamended, anaerobic aquifer materials and/or long periods of time are required in order to adapt the microbial population for benzene degradation. However, at one site located in Bemidji, MN, [ 14 C]benzene was oxidized to 14 CO 2 in unamended sediments without an apparent lag, suggesting that benzene was anaerobically degraded in situ. Benzene was not significantly oxidized in sediments from nearby Fe(III)-reducing sites nor in sediments collected from an uncontaminated background site in the same aquifer. Culturing and 16S rRNA-based molecular studies of the Bemidji aquifer demonstrated that while all sites contained similar numbers of Fe(III)-reducing microorganisms closely related to Geothrix fermentens , the site at which anaerobic benzene degradation was observed was greatly enriched with microorganisms in the family Geobacteraceae . This study provides the first data consistent with in situ anaerobic oxidation of benzene to carbon dioxide in the Fe(III)-reducing zone of a petroleum-contaminated aquifer and suggests that comparative studies on the size of the Geobacteraceae community in petroleum-contaminated aquifers might aid in the location of zones in which benzene degradation coupled to Fe(III) reduction is taking place.

Environmental Science & Technology↗
USGS1998

Effect of contaminant concentration on aerobic microbial mineralization of DCE and VC in stream-bed sediments

Discharge of DCE and VC to an aerobic surface water system simultaneously represents a significant environmental concern and, potentially, a non-engineered opportunity for efficient contaminant bioremediation. The potential for bioremediation, however, depends on the ability of the stream-bed microbial community to efficiently and completely degrade DCE and VC over a range of contaminant concentrations. The purposes of the studies reported here were to assess the potential for aerobic DCE and VC mineralization by stream-bed microorganisms and to evaluate the effects of DCE and VC concentrations on the apparent rates of aerobic mineralization. Bed-sediment microorganisms indigenous to a creek, where DCE-contaminated groundwater continuously discharges, demonstrated rapid mineralization of DCE and VC under aerobic conditions. Over 8 days, the recovery of [1,2-14C]DCE radioactivity as 14CO2 ranged from 17% to 100%, and the recovery of [1,2- 14C]VC radioactivity as 14CO2 ranged from 45% to 100%. Rates of DCE and VC mineralization increased significantly with increasing contaminant concentration, and the response of apparent mineralization rates to changes in DCE and VC concentrations was adequately described by Michaelis-Menten kinetics.Discharge of DCE and VC to an aerobic surface water system simultaneously represents a significant environmental concern and, potentially, a non-engineered opportunity for efficient contaminant bioremediation. The potential for bioremediation, however, depends on the ability of the stream-bed microbial community to efficiently and completely degrade DCE and VC over a range of contaminant concentrations. The purposes of the studies reported here were to assess the potential for aerobic DCE and VC mineralization by stream-bed microorganisms and to evaluate the effects of DCE and VC concentrations on the apparent rates of aerobic mineralization. Bed-sediment microorganisms indigenous to a creek, where DCE-contaminated groundwater continuously discharges, demonstrated rapid mineralization of DCE and VC under aerobic conditions. Over 8 days, the recovery of [1,2-14C]DCE radioactivity as 14CO2 ranged from 17% to 100%, and the recovery of [1,2-14C]VC radioactivity as 14CO2 ranged from 45% to 100%. Rates of DCE and VC mineralization increased significantly with increasing contaminant concentration, and the response of apparent mineralization rates to changes in DCE and VC concentrations was adequately described by Michaelis-Menten kinetics.

Environmental Science & Technology↗
USGS1997

Sequestration of hydrophobic organic contaminants by geosorbents

The chemical interactions of hydrophobic organic contaminants (HOCs) with soils and sediments (geosorbents) may result in strong binding and slow subsequent release rates that significantly affect remediation rates and endpoints. The underlying physical and chemical phenomena potentially responsible for this apparent sequestration of HOCs by geosorbents are not well understood. This challenges our concepts for assessing exposure and toxicity and for setting environmental quality criteria. Currently there are no direct observational data revealing the molecular-scale locations in which nonpolar organic compounds accumulate when associated with natural soils or sediments. Hence macroscopic observations are used to make inferences about sorption mechanisms and the chemical factors affecting the sequestration of HOCs by geosorbents. Recent observations suggest that HOC interactions with geosorbents comprise different inorganic and organic surfaces and matrices, and distinctions may be drawn along these lines, particularly with regard to the roles of inorganic micropores, natural sorbent organic matter components, combustion residue particulate carbon, and spilled organic liquids. Certain manipulations of sorbates or sorbent media may help reveal sorption mechanisms, but mixed sorption phenomena complicate the interpretation of macroscopic data regarding diffusion of HOCs into and out of different matrices and the hysteretic sorption and aging effects commonly observed for geosorbents. Analytical characterizations at the microscale, and mechanistic models derived therefrom, are needed to advance scientific knowledge of HOC sequestration, release, and environmental risk.

Environmental Science & Technology↗
USGS1997

Method for determination of methyl tert-butyl ether and its degradation products in water

An analytical method is described that can detect the major alkyl ether compounds that are used as gasoline oxygenates (methyl tert-butyl ether, MTBE; ethyl tert-butyl ether, ETBE; and tert-amyl methyl ether, TAME) and their most characteristic degradation products (tert-butyl alcohol, TBA; tert-butyl formate, TBF; and tert-amyl alcohol, TAA) in water at sub-ppb concentrations. The new method involves gas chromatography (GC) with direct aqueous injection (DAI) onto a polar column via a splitless injector, coupled with detection by mass spectrometry (MS). DAI-GC/MS gives excellent agreement with conventional purge-and-trap methods for MTBE over a wide range of environmentally relevant concentrations. The new method can also give simultaneous identification of polar compounds that might occur as degradation products of gasoline oxygenates, such as TBA, TBF, TAA, methyl acetate, and acetone. When the method was applied to effluent from a column microcosm prepared with core material from an urban site in New Jersey, conversion of MTBE to TBA was observed after a lag period of 35 days. However, to date, analyses of water samples from six field sites using the DAI-GC/MS method have not produced evidence for the expected products of in situ degradation of MTBE.An analytical method is described that can detect the major alkyl ether compounds that are used as gasoline oxygenates (methyl tert-butyl ether, MTBE; ethyl tert-butyl ether, ETBE; and tert-amyl methyl ether, TAME) and their most characteristic degradation products (tert-butyl alcohol, TBA; tert-butyl formate, TBF; and tert-amyl alcohol, TAA) in water at sub-ppb concentrations. The new method involves gas chromatography (GC) with direct aqueous injection (DAI) onto a polar column via a splitless injector, coupled with detection by mass spectrometry (MS). DAI-GC/MS gives excellent agreement with conventional purge-and-trap methods for MTBE over a wide range of environmentally relevant concentrations. The new method can also give simultaneous identification of polar compounds that might occur as degradation products of gasoline oxygenates, such as TBA, TBF, TAA, methyl acetate, and acetone. When the method was applied to effluent from a column microcosm prepared with core material from an urban site in New Jersey, conversion of MTBE to TBA was observed after a lag period of 35 days. However, to date, analyses of water samples from six field sites using the DAI-GC/MS method have not produced evidence for the expected products of in situ degradation of MTBE.

Environmental Science & Technology↗
USGS1998

Polychlorinated dibenzo-p-dioxin and dibenzofuran concentration profiles in sediment and fish tissue of the Willamette Basin, Oregon

Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/F) are highly hydrophobic compounds that have been implicated as carcinogens and, more recently, as estrogen disrupters. An occurrence and distribution study of these compounds in the Willamette Basin, Oregon, was conducted by the U.S. Geological Survey as part of the National Water-Quality Assessment Program. Bed sediment was collected from 22 sites; fish tissue was collected from eight sites. PCDD/F were found to be ubiquitous in Willamette Basin sediment. A distinct homolog profile, dominated by octachlorodibenzo-p-dioxin, was observed in sediment throughout the basin. The PCDD homolog profile was consistent at all sites, regardless of total PCDD/F concentration, presence of point sources, subbasin size, geographic location or land use. Principal components analysis revealed a gradient among the homolog profiles that showed increasing dominance of highly chlorinated congeners where human and industrial activity increased. Tissue and bed sediment obtained from the same site did not have similar PCDD/F concentrations or homolog profiles. Fish tissue showed enrichment in less chlorinated congeners and congeners with chlorine substitutions in the 2, 3, 7 and 8 positions.

Environmental Science & Technology↗
USGS1998

Partition characteristics of polycyclic aromatic hydrocarbons on soils and sediments

The partition behavior was determined for three polycyclic aromatic hydrocarbons (PAHs), i.e., naphthalene, phenanthrene, and pyrene, from water to a range of soil and sediment samples. The measured partition coefficients of the individual PAHs between soil/sediment organic matter (SOM) and water (i.e., K(oc) values) are relatively invariant either for the 'clean' (uncontaminated) soils or for the clean sediments; however, the mean K(oc) values on the sediments are about twice the values on the soils. This disparity is similar to the earlier observation for other nonpolar solutes and reflects the compositional differences between soil and sediment organic matters. No significant differences in K(oc) are observed between a clean coastal marine sediment and freshwater sediments. The coastal sediments that are significantly impacted by organic contaminants exhibit higher K(oc) values. At given K(ow) values (octanol-water), the PAHs exhibit much higher K(oc) values than other relatively nonpolar solutes (e.g., chlorinated hydrocarbons). This effect is shown to result from the enhanced partition of PAHs to SOM rather than from lower K(ow) values of PAHs at given supercooled liquid solute solubilities in water. The enhanced partition of PAHs over other nonpolar solutes in SOM provides an account of the markedly different correlations between log K(oc) and log K(ow) for PAHs and for other nonpolar solutes. The improved partition of PAHs in SOM stems apparently from the enhanced compatibility of their cohesive energy densities with those of the aromatic components in SOM. The approximate aromatic fraction in soil/sediment organic matter has been assessed by solid-state 13C-NMR spectroscopy.The partition behavior was determined for three polycyclic aromatic hydrocarbons (PAHs), i.e., naphthalene, phenanthrene, and pyrene, from water to a range of soil and sediment samples. The measured partition coefficients of the individual PAHs between soil/sediment organic matter (SOM) and water (i.e., Koc values) are relatively invariant either for the `clean' (uncontaminated) soils or for the clean sediments; however, the mean Koc values on the sediments are about twice the values on the soils. This disparity is similar to the earlier observation for other nonpolar solutes and reflects the compositional differences between soil and sediment organic matters. No significant differences in Koc are observed between a clean coastal marine sediment and freshwater sediments. The coastal sediments that are significantly impacted by organic contaminants exhibit higher Koc values. At given Kow values (octanol-water), the PAHs exhibit much higher Koc values than other relatively nonpolar solutes (e.g., chlorinated hydrocarbons). This effect is shown to result from the enhanced partition of PAHs to SOM rather than from lower Kow values of PAHs at given supercooled liquid solute solubilities in water. The enhanced partition of PAHs over other nonpolar solutes in SOM provides an account of the markedly different correlations between log Koc and log Kow for PAHs and for other nonpolar solutes. The improved partition of PAHs in SOM stems apparently from the enhanced compatibility of their cohesive energy densities with those of the aromatic components in SOM. The approximate aromatic fraction in soil/sediment organic matter has been assessed by solid-state 13C-NMR spectroscopy.

Environmental Science & Technology↗
USGS1998

Rapid oxidation of geothermal arsenic(III) in streamwaters of the eastern Sierra Nevada

Arsenic redox cycling was examined in source waters of the Los Angeles Aqueduct, specifically at Hot Creek, a tributary of the Owens River. Elevated arsenic concentrations in Hot Creek result from geothermal inputs. Total arsenic and As(III) concentrations were determined in the creek and in hot spring pools along its banks. Samples were processed in the field using anion-exchange columns to separate inorganic As(III) and As(V) species. Downstream of the geothermal inputs, decreasing contributions of As(III) to total arsenic concentrations indicated rapid in-stream oxidation of As(III) to As(V) with almost complete oxidation occurring within 1200 m. Based on assumed plug flow transport and a flow velocity of about 0.4 m/s, the pseudo- first-order half-life calculated for this reaction was approximately 0.3 h. Conservative transport of total dissolved arsenic was observed over the reach. Pseudo-first-order reaction rates determined for As(III) oxidation in batch studies conducted in the field with aquatic macrophytes and/or macrophyte surface matter were comparable to the in-stream oxidation rate observed along Hot Creek. In batch kinetic studies, oxidation was not observed after sterile filtration or after the addition of antibiotics, which indicates that bacteria attached to submerged macrophytes are mediating the rapid As(III) oxidation reaction.Arsenic redox cycling was examined in source waters of the Los Angeles Aqueduct, specifically at Hot Creek, a tributary of the Owens River. Elevated arsenic concentrations in Hot Creek result from geothermal inputs. Total arsenic and As(III) concentrations were determined in the creek and in hot spring pools along its banks. Samples were processed in the field using anion-exchange columns to separate inorganic As(III) and As(V) species. Downstream of the geothermal inputs, decreasing contributions of As(III) to total arsenic concentrations indicated rapid in-stream oxidation of As(III) to As(V) with almost complete oxidation occurring within 1200 m. Based on assumed plug flow transport and a flow velocity of about 0.4 m/s, the pseudo-first-order half-life calculated for this reaction was approximately 0.3 h. Conservative transport of total dissolved arsenic was observed over the reach. Pseudo-first-order reaction rates determined for As(III) oxidation in batch studies conducted in the field with aquatic macrophytes and/or macrophyte surface matter were comparable to the in-stream oxidation rate observed along Hot Creek. In batch kinetic studies, oxidation was not observed after sterile filtration or after the addition of antibiotics, which indicates that bacteria attached to submerged macrophytes are mediating the rapid As(III) oxidation reaction.

Environmental Science & Technology↗
USGS1998

Partitioning and transport of total and methyl mercury in the Lower Fox River, Wisconsin

To investigate transport and partitioning processes of Hg(T) in the Fox River, we coupled detailed time series data of total mercury (Hg(T)) at the river mouth with transect sampling in the Lower Fox River. Unfiltered Hg(T) concentrations in the Fox River during the study period (April 1994-October 1995) ranged from 1.8 to 182 ng L(-1) with a median of 24.8 ng L-1, predominantly (93.6%) in the particulate phase. These levels were significantly elevated compared with other large tributaries to Lake Michigan (Hurley, J. P.; Shafer, M. M.; Cowell, S. E.; Overdier, J. T.; Hughes, P. E.; Armstrong, D. E. Environ. Sci. Technol. 1996, 30, 20932098). Transect sampling revealed progressively increasing water column Hg(T) concentrations and Hg(T) particulate enrichment downstream, which were consistent with trends in sediment Hg(T) levels in the river. Resuspended sediments are likely the predominant source of Hg from the Fox River into Green Bay. Despite elevated Hg(T) concentrations, methyl mercury (MeHg) concentrations were relatively low, suggesting limited bioavailability of Hg(T) associated with sediments.To investigate transport and partitioning processes of HgT in the Fox River, we coupled detailed time series data of total mercury (HgT) at the river mouth with transect sampling in the Lower Fox River. Unfiltered HgT concentrations in the Fox River during the study period (April 1994-October 1995) ranged from 1.8 to 182 ng L-1 with a median of 24.8 ng L-1, predominantly (93.6%) in the particulate phase. These levels were significantly elevated compared with other large tributaries to Lake Michigan. Transect sampling revealed progressively increasing water column HgT concentrations and HgT particulate enrichment downstream, which were consistent with trends in sediment HgT levels in the river. Resuspended sediments are likely the predominant source of Hg from the Fox River into Green Bay. Despite elevated HgT concentrations, methyl mercury (MeHg) concentrations were relatively low, suggesting limited bioavailability of HgT associated with sediments.

Environmental Science & Technology↗