Trace metal assessment of Lake Michigan tributaries using low-level techniques
No abstract available.
Indiana, Michigan, Wisconsin↗
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Comparison of denitrification activity measurements in groundwater using cores and natural-gradient tracer tests
The transport of many solutes in groundwater is dependent upon the relative rates of physical flow and microbial metabolism. Quantifying rates of microbial processes under subsurface conditions is difficult and is most commonly approximated using laboratory studies with aquifer materials. In this study, we measured in situ rates of denitrification in a nitrate-contaminated aquifer using small-scale, natural-gradient tracer tests and compared the results with rates obtained from laboratory incubations with aquifer core material. Activity was measured using the acetylene block technique. For the tracer tests, co-injection of acetylene and bromide into the aquifer produced a 30 μM increase in nitrous oxide after 10 m of transport (23−30 days). An advection−dispersion transport model was modified to include an acetylene-dependent nitrous oxide production term and used to simulate the tracer breakthrough curves. The model required a 4-day lag period and a relatively low sensitivity to acetylene to match the narrow nitrous oxide breakthrough curves. Estimates of in situ denitrification rates were 0.60 and 1.51 nmol of N 2 O produced cm - 3 aquifer day - 1 for two successive tests. Aquifer core material collected from the tracer test site and incubated as mixed slurries in flasks and as intact cores yielded rates that were 1.2−26 times higher than the tracer test rate estimates. Results with the coring-dependent techniques were variable and subject to the small-scale heterogeneity within the aquifer, while the tracer tests integrated the heterogeneity along a flow path, giving a rate estimate that is more applicable to transport at the scale of the aquifer.
Environmental Science & Technology↗
Anaerobic hydrocarbon degradation in petroleum-contaminated harbor sediments under sulfate-reducing and artificially imposed iron-reducing conditions
The potential use of iron(III) oxide to stimulate in-situ hydrocarbon degradation in anaerobic petroleum-contaminated harbor sediments was investigated. Previous studies have indicated that Fe(III)-reducing bacteria (FeRB) can oxidize some electron donors more effectively than sulfate- reducing bacteria (SRB). In contrast to previous results in freshwater sediments, the addition of Fe(III) to marine sediments from San Diego Bay, CA did not switch the terminal electron-accepting process (TEAP) from sulfate reduction to Fe-(III) reduction. Addition of Fe(III) also did not stimulate anaerobic hydrocarbon oxidation. Exposure of the sediment to air [to reoxidize Fe(II) to Fe(III)] followed by anaerobic incubation of the sediments, resulted in Fe-(III) reduction as the TEAP, but contaminant degradation was not stimulated and in some instances was inhibited. The difference in the ability of FeRB to compete with the SRB in the different sediment treatments was related to relative population sizes. Although the addition of Fe(III) did not stimulate hydrocarbon degradation, the results presented here as well as other recent studies demonstrate that there may be significant anaerobic hydrocarbon degradation under sulfate-reducing conditions in harbor sediments.
Environmental Science & Technology↗
Reactive solute transport in an acidic stream: Experimental pH increase and simulation of controls on pH, aluminum, and iron
Solute transport simulations quantitatively constrained hydrologic and geochemical hypotheses about field observations of a pH modification in an acid mine drainage stream. Carbonate chemistry, the formation of solid phases, and buffering interactions with the stream bed were important factors in explaining the behavior of pH, aluminum, and iron. The precipitation of microcrystalline gibbsite accounted for the behavior of aluminum; precipitation of Fe(OH)3 explained the general pattern of iron solubility. The dynamic experiment revealed limitations on assumptions that reactions were controlled only by equilibrium chemistry. Temporal variation in relative rates of photoreduction and oxidation influenced iron behavior. Kinetic limitations on ferrous iron oxidation and hydrous oxide precipitation and the effects of these limitations on field filtration were evident. Kinetic restraints also characterized interaction between the water column and the stream bed, including sorption and desorption of protons from iron oxides at the sediment-water interface and post-injection dissolution of the precipitated aluminum solid phase.
Environmental Science & Technology↗
Chemical factors influencing colloid-facilitated transport of contaminants in porous media
The effects of colloids on the transport of two strongly sorbing solutes a hydrophobic organic compound, phenanthrene, and a metal ion, Ni 2+ were studied in sand-packed laboratory columns under different pH and ionic strength conditions. Two types of column experiments were performed as follows: (i) sorption/mobilization experiments where the contaminant was first sorbed in the column under conditions where no colloids were released and mobilized under conditions where colloids were released as a result of ionic strength reduction in the influent; and (ii) transport experiments where the contaminant, dissolved or sorbed on colloids, was injected into columns packed with a strongly sorbing porous medium. In the first type of experiment, contaminant mobilization was significant only when all releasable colloids were flushed from the column. In all other cases, although high colloid particle concentrations were encountered, there was no marked effect on total contaminant concentrations. In the second type of experiment, colloid deposition efficiencies were shown to control the enhancement of transport. The deposition efficiency was a function of the pH (for a high organic content sand) and of the contaminant concentration (for a charged species such as Ni 2+ ).
Environmental Science & Technology↗
Hydrologic and microbiological factors affecting persistence and migration of petroleum hydrocarbons spilled in a continuous-permafrost region
Fuel spills, totaling about 1300 m3, occurred between 1976 and 1978 adjacent to Imikpuk Lake, a drinking water source near Barrow, AK. Substantial contamination of soils and groundwater near the lake persists. We examined the magnitude and direction of groundwater flux and the microbial activity at this site to understand the persistence of contamination and its effect on the lake. We found that groundwater flux is small due to shallow permafrost, which restricts the cross-sectional area available for flow, and to the short annual thaw season (ca. 90 days). The small flux and limited depth also constrain contaminant transport and dispersion, resulting in persistent, shallow contamination. The numbers of hydrocarbon-oxidizing microorganisms and their laboratory mineralization potentials for benzene (at 10 ??C) were higher in samples from contaminated areas than in reference samples. Benzene mineralization potentials in groundwater samples were comparable to more temperate systems (0.1-0.5 mg of benzene mineralized L-1 day-1) and were stimulated by nutrient additions. Field measurements of dissolved oxygen, nitrate, ferrous iron, and sulfide in groundwater provided evidence that biodegradation of petroleum hydrocarbons is occurring in situ. Despite evidence of an active microbial population, microbial processes, like contaminant transport, are likely limited at this site by the short annual thaw season.
Environmental Science & Technology↗
Processes affecting the fate of monoaromatic hydrocarbons in an aquifer contaminated by crude oil
Crude oil spilled from a subsurface pipeline in north-central Minnesota has dissolved in the groundwater, resulting in the formation of a plume of aliphatic, aromatic, and alicyclic hydrocarbons. Comparison of paired oil and groundwater samples collected along the central axis of the residual oil body shows that the trailing edge of the oil is depleted in the more soluble aromatic hydrocarbons (e.g., benzene, toluene, etc.) when compared with the leading edge. At the same time, concentrations of monoaromatic hydrocarbons in groundwater beneath the oil increase as the water moves toward the leading edge of the oil. Immediately downgradient from the leading edge of the oil body, certain aromatic hydrocarbons (e.g., benzene) are found at concentrations near those expected of a system at equilibrium, and the concentrations exhibit little variation over time (???8-20%). Other compounds (e.g., toluene) appear to be undersaturated, and their concentrations show considerably more temporal variation (???20-130%). The former are persistent within the anoxic zone downgradient from the oil, whereas concentrations of the latter decrease rapidly. Together, these observations suggest that the volatile hydrocarbon composition of the anoxic groundwater near the oil body is controlled by a balance between dissolution and removal rates with only the most persistent compounds reaching saturation. Examination of the distributions of homologous series and isomeric assemblages of alkylbenzenes reveals that microbial degradation is the dominant process controlling the fate of these compounds once groundwater moves away from the oil. For all but the most persistent compounds, the distal boundary of the plume at the water table extends no more than 10-15 m down-gradient from the oxic/anoxic transition zone. Thus, transport of the monoaromatic hydrocarbons is limited by redox conditions that are tightly coupled to biological degradation processes.
Environmental Science & Technology↗
Comparison of Eh and H2 measurements for delineating redox processes in a contaminated aquifer
Measurements of oxidation-reduction potential ( E h ) and concentrations of dissolved hydrogen (H 2 ) were made in a shallow groundwater system contaminated with solvents and jet fuel to delineate the zonation of redox processes. E h measurements ranged from +69 to -158 mV in a cross section of the contaminated plume and accurately delineated oxic from anoxic groundwater. Plotting measured E h and pH values on an equilibrium stability diagram indicated that Fe(III) reduction was the predominant redox process in the anoxic zone and did not indicate the presence of methanogenesis and sulfate reduction. In contrast, measurements of H 2 concentrations indicated that methanogenesis predominated in heavily contaminated sediments near the water table surface (H 2 ∼ 7.0 nM) and that the methanogenic zone was surrounded by distinct sulfate-reducing (H 2 ∼ 1-4 nM) and Fe(III)-reducing (H 2 ∼ 0.1-0.8 nM) zones. The presence of methanogenesis, sulfate reduction, and Fe(III) reduction was confirmed by the distribution of dissolved oxygen, sulfate, Fe(II), and methane in groundwater. These results show that H 2 concentrations were more useful for identifying anoxic redox processes than E h measurements in this groundwater system. However, H 2 -based redox zone delineations are more reliable when H 2 concentrations are interpreted in the context of electron-acceptor (oxygen, nitrate, sulfate) availability and the presence of final products [Fe(II), sulfide, methane] of microbial metabolism.
Environmental Science & Technology↗
Comment on "Problems associated with using filtration to define dissolved trace element concentrations in natural water samples"
No abstract available.
Environmental Science & Technology↗
Binding of pyrene to aquatic and commercial humic substances: The role of molecular weight and aromaticity
The binding of pyrene to a number of humic substances isolated from various aquatic sources and a commercial humic acid was measured using the solubility enhancement method. The humic materials used in this study were characterized by various spectroscopic and liquid chromatography methods. A strong correlation was observed between the pyrene binding coefficient, K(doc), and the molecular weights, molar absorptivities at 280 nm, and aromaticity of the aquatic humic substances. Binding of pyrene to the commercial humic acid, however, was significantly stronger and did not obey the relationships observed between K(doc) and the chemical properties of the aquatic humic substrates. These results suggest that the molecular weight and the aromatic content of the humic substrates exert influences on the binding of nonpolar and planar aromatic molecules and that the physicochemical properties of both humic materials and organic solutes are important in controlling the speciation of nonpolar organic contaminants in natural waters.
Environmental Science & Technology↗
Physiological considerations in applying laboratory-determined buoyant densities to predictions of bacterial and protozoan transport in groundwater: Results of in-situ and laboratory tests
Buoyant densities were determined for groundwater bacteria and microflagellates (protozoa) from a sandy aquifer (Cape Cod, MA) using two methods: (1) density-gradient centrifugation (DGC) and (2) Stoke's law approximations using sedimentation rates observed during natural-gradient injection and recovery tests. The dwarf (average cell size, 0.3 μm), unattached bacteria inhabiting a pristine zone just beneath the water table and a majority (∼80%) of the morphologically diverse community of free-living bacteria inhabiting a 5-km-long plume of organically-contaminated groundwater had DGC-determined buoyant densities <1.019 g/cm 3 before culturing. In the aquifer, sinking rates for the uncultured 2-μm size class of contaminant plume bacteria were comparable to that of the bromide tracer (1.9 × 10 - 3 M), also suggesting a low buoyant density. Culturing groundwater bacteria resulted in larger (0.8−1.3 μm), less neutrally-buoyant (1.043−1.081 g/cm 3 ) cells with potential sedimentation rates up to 64-fold higher than those predicted for the uncultured populations. Although sedimentation generally could be neglected in predicting subsurface transport for the community of free-living groundwater bacteria, it appeared to be important for the cultured isolates, at least until they readapt to aquifer conditions. Culturing-induced alterations in size of the contaminant-plume microflagellates (2−3 μm) were ameliorated by using a lower nutrient, acidic (pH 5) porous growth medium. Buoyant densities of the cultured microflagellates were low, i.e., 1.024−1.034 g/cm 3 (using the DGC assay) and 1.017−1.039 g/cm 3 (estimated from in-situ sedimentation rates), sug gesting good potential for subsurface transport under favorable conditions.
Environmental Science & Technology↗
Anaerobic degradation of benzene in diverse anoxic environments
Benzene has often been observed to be resistant to microbial degradation under anoxic conditions. A number of recent studies, however, have demonstrated that anaerobic benzene utilization can occur. This study extends the previous reports of anaerobic benzene degradation to sediments that varied with respect to contamination input, predominant redox condition, and salinity. In spite of differences in methodology, microbial degradation of benzene was noted in slurries constructed with sediments from various geographical locations and range from aquifer sands to fine-grained estuarine muds, under methanogenic, sulfate-reducing, and iron-reducing conditions. In aquifer sediments under methanogenic conditions, benzene loss was concomitant with methane production, and microbial utilization of [ 14 C]benzene yielded 14 CO 2 and 14 CH 4 . In slurries with estuarine and aquifer sediments under sulfate-reducing conditions, the loss of sulfate in amounts consistent with the stoichiometric degradation of benzene or the conversion of [ 14 C]benzene to 14 CO 2 indicates that benzene was mineralized. Benzene loss also occurred in the presence of Fe(III) in sediments from freshwater environments. Microbial benzene utilization, however, was not observed under denitrifying conditions. These results indicate that the potential for the anaerobic degradation of benzene, which was once thought to be resistant to non-oxygenase attack, exists in a variety of aquatic sediments from widely distributed locations.
Environmental Science & Technology↗
From the 1988 drought to the 1993 flood: Transport of halogenated organic compounds with the Mississippi river suspended sediment at Thebes, Illinois
Suspended sediment was isolated from water samples collected from the Mississippi River at Thebes, IL, eight times over a 5-year period from May 1988 through September 1993 in order to evaluate the transport of lipophilic halogenated organic compounds associated with the suspended sediment. Two hydrologic extremes were included-the 1988 drought and the 1993 flood. Halogenated organic compounds included polychlorinated biphenyls (PCBs), hexachlorobenzene, pentachloroanisole, DCPA (dacthal), trifluralin, aldrin, dieldrin, and chlordane components. Sediment transport of most of these organic compounds was substantially higher during the 1993 flood then at other sampling times. The extreme transports during the flood were due to unusually high concentrations of some contaminants on the suspended sediment, low to average concentrations of suspended sediment being transported, and unusually high water discharges.
Illinois↗
Lack of correlation between organic acid concentrations and predominant electron-accepting processes in a contaminated aquifer
Long-term (1992-1995) monitoring data from a petroleum hydrocarbon- contaminated aquifer were used to examine the hypothesis that concentrations of low molecular weight (LMW) aliphatic organic acids reflect terminal electron-accepting processes. During the period of study, concentrations of dissolved hydrogen (H2) indicated that methanogenic, sulfate-reducing, and iron(III)-reducing conditions predominated at the site. However, there was no correlation between LMW organic acid concentrations and concentrations of dissolved H2. These results indicate that organic acid concentrations are not a reliable indicator of local redox conditions at this site.
Environmental Science & Technology↗
Transport and recovery of bacteriophage PRD1 in a sand and gravel aquifer: Effect of sewage-derived organic matter
To test the effects of sewage-derived organic matter on virus attachment, 32P-labeled bacteriophage PRD1, linear alkylbenzene sulfonates (LAS), and tracers were injected into sewage-contaminated (suboxic, elevated organic matter) and uncontaminated (oxic, low organic matter) zones of an iron oxide-coated quartz sand and gravel aquifer on Cape Cod, MA. In the uncontaminated zone, 83% of the PRD1 were attenuated over the first meter of transport by attachment to aquifer grains. In the contaminated zone, 42% of the PRD1 were attenuated over the first meter of transport. Sewage-derived organic matter contributed to the difference in PRD1 attenuation by blocking attachment sites in the contaminated zone. At greater distances down gradient (to a total transport distance of 3.6 m), a near-constant amount of PRD1 continued to break through, suggesting that aquifer grain heterogeneities allowed a small amount of reversible attachment. Injection of an LAS mixture (25 mg L-1), a common sewage constituent, remobilized 87% of the attached PRD1 in the contaminated zone, but only 2.2% in the uncontaminated zone. LAS adsorption promoted virus recovery in the contaminated zone by altering the PRD1-surface interactions; however, the amount of LAS adsorbed was not sufficient to promote release of the attached PRD1 in the uncontaminated zone.
Environmental Science & Technology↗
Matrix-enhanced degradation of p,p'-DDT during gas chromatographic analysis: A consideration
Analysis of p,p ‘-DDT in environmental samples requires monitoring the GC-derived breakdown of this insecticide, which produces p,p ‘-DDD and/or p,p ‘-DDE, both also primary environmental degradation products. A performance evaluation standard (PES) containing p,p ‘-DDT but not p,p ‘-DDD or p,p ‘-DDE can be injected at regular intervals throughout an analytical sequence to monitor GC degradation. Some U.S. EPA methods limit GC breakdown of DDT in the PES to ≤20%. GC/MS analysis of large-volume natural water samples fortified with deuterium- and 13 C-labeled p,p ‘-DDT exhibited up to 65% DDT breakdown by the GC inlet. These matrix-enhanced GC degradation amounts substantially exceeded the <20% breakdown levels indicated by bracketing injections of the PES containing unlabeled and labeled DDT. Substantial matrix-enhanced GC degradation was not observed during analysis of a limited number of fractionated bed-sediment extracts containing labeled DDT. Use of isotopically labeled DDT seems to provide an effective tool for monitoring sample-specific DDT breakdown during GC/MS analysis. However, analyte co-elutions render impractical their use in GC/ECD analysis. The oc currence of matrix-enhanced GC degradation might have important implications on data quality and the resultant interpretations of the environmental degradation of DDT and other thermolabile contaminants.
Environmental Science & Technology↗
Analysis of environmental data with censored observations
The potential threats to humans and to terrestrial and aquatic ecosystems from environmental contamination could depend on the sum of the concentrations of different chemicals. However, direct summation of environmental data is not generally feasible because it is common for some chemical concentrations to be recorded as being below the analytical reporting limit. This creates special problems in the analysis of the data. A new model selection procedure, named forward censored regression, is introduced for selecting an appropriate model for environmental data with censored observations. The procedure is demonstrated using concentrations of atrazine (2-chloro-4-ethylamino-6-isopropylamino- s -triazine), deethylatrazine (DEA, 2-amino-4-chloro-6-isopropylamino- s -triazine), and deisopropylatrazine (DIA, 2-amino-4-chloro-6-ethylamino- s -triazine) in groundwater in the midwestern United States by using the data derived from a previous study conducted by the U.S. Geological Survey. More than 80% of the observations for each compound for this study were left censored at 0.05 μg/L. The values for censored observations of atrazine, DEA, and DIA are imputed with the selected models. The summation of atrazine residue (atrazine + DEA + DIA) can then be calculated using the combination of observed and imputed values to generate a pseudo-complete data set. The all-subsets regression procedure is applied to the pseudo-complete data to select the final model for atrazine residue. The methodology presented can be used to analyze similar cases of environmental contamination involving censored data.
Environmental Science & Technology↗
Bacterial oxidation of methyl bromide in Mono Lake, California
The oxidation of methyl bromide (MeBr) in the water column of Mono Lake, CA, was studied by measuring the formation of H14CO3 from [14C]MeBr. Potential oxidation was detected throughout the water column, with highest rates occurring in the epilimnion (5-12 m depth). The oxidation of MeBr was eliminated by filter-sterilization, thereby demonstrating the involvement of bacteria. Vertical profiles of MeBr activity differed from those obtained for nitrification and methane oxidation, indicating that MeBr oxidation is not simply a co-oxidation process by either nitrifiers or methanotrophs. Furthermore, specific inhibitors of methane oxidation and/or nitrification (e.g., methyl fluoride, acetylene, allyl sulfide) had no effect upon the rate of MeBr oxidation in live samples. Of a variety of potential electron donors added to Mono Lake water, only trimethylamine resulted in the stimulation of MeBr oxidation. Cumulatively, these results suggest that the oxidation of MeBr in Mono Lake waters is attributable to trimethylamine-degrading methylotrophs. Neither methyl chloride nor methanol inhibited the oxidation of [14C]MeBr in live samples, indicating that these bacteria directly oxidized MeBr rather than the products of MeBr nucleophilic substitution reactions.
Environmental Science & Technology↗