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USGS1992

Geochemical heterogeneity in a sand and gravel aquifer: Effect of sediment mineralogy and particle size on the sorption of chlorobenzenes

The effect of particle size, mineralogy and sediment organic carbon (SOC) on sorption of tetrachlorobenzene and pentachlorobenzene was evaluated using batch-isotherm experiments on sediment particle-size and mineralogical fractions from a sand and gravel aquifer, Cape Cod, Massachusetts. Concentration of SOC and sorption of chlorobenzenes increase with decreasing particle size. For a given particle size, the magnetic fraction has a higher SOC content and sorption capacity than the bulk or non-magnetic fractions. Sorption appears to be controlled by the magnetic minerals, which comprise only 5–25% of the bulk sediment. Although SOC content of the bulk sediment is <0.1%, the observed sorption of chlorobenzenes is consistent with a partition mechanism and is adequately predicted by models relating sorption to the octanol/water partition coefficient of the solute and SOC content. A conceptual model based on preferential association of dissolved organic matter with positively-charged mineral surfaces is proposed to describe micro-scale, intergranular variability in sorption properties of the aquifer sediments.

Journal of Contaminant Hydrology↗

USGS1992

Identification of persistent anionic surfactant-derived chemicals in sewage effluent and groundwater

Preparative isolation and fractionation procedures coupled with spectrometric analyses were used to identify surfactant-derived contaminants in sewage effluent and sewage-contaminated groundwater from a site located on Cape Cod, Massachusetts. Anionic surfactants and their biodegradation intermediates were isolated from field samples by ion exchange and fractionated by solvent extraction and adsorption chromatography. Fractions were analyzed by 13 C nuclear magnetic resonance spectrometry and gas chromatography-mass spectrometry. Carboxylated residues of alkylphenol polyethoxylate surfactants were detected in sewage effluent and contaminated groundwater. Linear alkylbenzenesulfonates (LAS) were identified in sewage effluent and groundwater. Groundwater LAS composition suggested preferential removal of select isomers and homologs due to processes of biodegradation and partitioning. Tetralin and indane sulfonates (DATS), alicyclic analogs of LAS, were also identified in field samples. Although DATS are a minor portion of LAS formulations, equivalent concentrations of LAS and DATS in groundwater suggested persistence of alicyclic contaminant structures over those of linear structure. Sulfophenyl-carboxylated (SPC) LAS biodegradation intermediates were determined in sewage effluent and groundwater. Homolog distributions suggested that SPC containing 3–10 alkyl-chain carbons persist during infiltration and groundwater transport. Surfactant-derived residues detected in well F 300-50 groundwater have a minimum residence time in the range of 2.7–4.6 yr. LAS detected in groundwater at 500 m from infiltration has been stable over an estimated 50–500 half lives.

Journal of Contaminant Hydrology↗

USGS1992

The aqueous photolysis of α-pinene in solution with humic acid

Terpenes are produced abundantly by environmental processes but are found in very low concentrations in natural waters. Aqueous photolysis of solutions containing α-pinene, a representative terpene, in the presence of humic acid resulted in degradation of the pinene. Comparison of this reaction to photolysis of α-pinene in the presence of methylene blue leads to the conclusion that the reactive pathway for the abiotic degradation of α-pinene is due to reaction with singlet oxygen produced by irradiation of the humic material. The initial product of single oxygen and α-pinene is a hydroperoxide. Since humic materials are prevalent in most natural waters, this mechanism of photodecomposition for α-pinene probably also applies to other terpenes in surface waters and may be reasonably considered to contribute to their low environmental concentration.

Journal of Contaminant Hydrology↗

USGS1992

Associations of free-living bacteria and dissolved organic compounds in a plume of contaminated groundwater

Associations of free-living bacteria (FLB) and dissolved organic contaminants in a 4-km-long plume of sewage-contaminated groundwater were investigated. Abundance of FLB in the core of the plume (as delineated by maximum specific conductance) steadily decreased in the direction of flow from a point 0.25 km downgradient from the source to the toe of the plume. At 0.25 km downgradient, FLB comprised up to 31% of the total bacterial population, but constituted <7% of the population at 2 km downgradient. Abundance of FLB correlated strongly (r = 0.80, n = 23) with total dissolved organic carbon (DOC) in contaminated groundwater between 0.64 and 2.1 km downgradient, although distributions of individual contaminants such as di-, tri- and tetrachloroethene were highly variable, and their association with FLB less clear. Numbers of FLB in the downgradient portion of the plume which is contaminated with branched-chain alkylbenzenesulfonate (ABS) surfactants were low (<5 · 10 8 /L) in spite of relatively high levels of DOC (up to 4 mg/L). However, abundance of FLB correlated strongly with non-surfactant DOC along vertical transects through the plume. The ratio of FLB to DOC and the ratio of FLB to attached bacteria generally decreased in the direction of flow and, consequently, with the age of the organic contaminants.

Journal of Contaminant Hydrology↗

USGS1993

Modeling steady-state methanogenic degradation of phenols in groundwater

Field and microcosm observations of methanogenic phenolic compound degradation indicate that Monod kinetics governs the substrate disappearance but overestimates the observed biomass. In this paper we present modeling results from an ongoing multidisciplinary study of methanogenic biodegradation of phenolic compounds in a sand and gravel aquifer contaminated by chemicals and wastes used in wood treatment. Field disappearance rates of four phenols match those determined in batch microcosm studies previously performed by E.M. Godsy and coworkers. The degradation process appears to be at steady-state because even after a sustained influx over several decades, the contaminants still are disappearing in transport downgradient. The existence of a steady-state degradation profile of each substrate together with a low biomass density in the aquifer indicate that the bacteria population is exhibiting no net growth. This may be due to the oligotrophic nature of the biomass population in which utilization and growth are approximately independent of concentration for most of the concentration range. Thus a constant growth rate should exist over much of the contaminated area which may in turn be balanced by an unusually high decay or maintenance rate due to hostile conditions or predation.

Journal of Contaminant Hydrology↗

USGS1993

Effect of pH on bacteriophage transport through sandy soils

Effects of pH and hydrophobicity on attachment and detachment of PRD- 1 and MS- 2 in three different sandy soils were investigated in a series of laboratory-column experiments. Concentrations of the lipid-containing phage PRD- 1 decreased 3–4 orders of magnitude during passage through the 10–15-cm-long columns. Attachment of the lipid-containing phage PRD- 1 was insensitive to pH and was apparently controlled by hydrophobic interactions in soil media. The less-hydrophobic phage MS-2 acted conservatively; it was not removed in the columns at pH's 5.7–8.0. The sticking efficiency (α) in a colloid-filtration model was between 0.1 and 1 for PRD- 1 , indicating a relatively high removal efficiency. Phage attachment was reversible, but detachment under steady-state conditions was slow. An increase in pH had a moderate effect on enhancing detachment. Still, these soils should continue to release phage to virus-free water for days to weeks following exposure to virus-containing water. In sandy soils with a mass-fraction organic carbon as low as a few hundredths of a percent, pH changes in the range 5.7–8.0 should have little effect on retention of more-hydrophobic virus (e.g., PRD- 1 ), in that retardation will be dominated by hydrophobic effects. Sharp increases in pH should enhance detachment and transport of virus previously deposited on soil grains. A more hydrophilic virus (e.g., MS- 2 ) will transport as a conservative tracer in low-carbon sandy soil.

Journal of Contaminant Hydrology↗

USGS1994

Distribution and transport of selected anthropogenic organic compounds on Mississippi River suspended sediment (U.S.A.), May/June 1988

The distribution and transport of selected hydrophobic halogenated organic compounds on suspended sediment from the lower Mississippi River were determined using discharge-weighted sampling with concurrent discharge measurements. Trends in compound concentration from upstream to downstream and the effects of selected tributaries were determined. The compounds identified on the suspended sediment include pentachlorobenzene, hexachlorobenzene, pentachloroanisole, dacthal, chlordane (trans-), nonachlor (trans-), chlorthalonil, and penta-, hexa-, hepta- and octachlorobiphenyls. Loads of most of the compounds increased from upstream to downstream on the main stem of the Mississippi River. Of the tributaries studied, the Ohio River had the most significant effect on the loads.The distribution and transport of selected hydrophobic halogenated organic compounds on suspended sediment from the lower Mississippi River were determined using discharge-weighted sampling with concurrent discharge measurements. Trends in compound concentration from upstream to downstream and the effects of selected tributaries were determined. The compounds identified on the suspended sediment include pentachlorobenzene, hexachlorobenzene, pentachloroanisole, dacthal, chlordane (trans-), nonachlor (trans-), chlorthalonil, and penta-, hexa-, hepta- and octachlorobiphenyls. Loads of most of the compounds increased from upstream to downstream on the main stem of the Mississippi River. Of the tributaries studied, the Ohio River had the most significant effect on the loads.

Journal of Contaminant Hydrology↗

USGS1996

A top specified boundary layer (TSBL) approximation approach for the simulation of groundwater contamination processes

This paper presents improvements in the 'classical boundary layer' (CBL) approximation method to obtain simple but robust initial characterization of aquifer contamination processes. Contaminants are considered to penetrate into the groundwater through the free surface of the aquifer. The improved method developed in this study is termed the 'top specified boundary layer' (TSBL) approach. It involves the specification of the contaminant concentration at the top of the contaminated 'region of interest' (ROI), which is simulated as a boundary layer. the TSBL modification significantly improves the ability of the boundary layer method to predict the development of concentration profiles over both space and time. The TSBL method can be useful for the simulation of cases in which the contaminant concentration is prescribed at the aquifer's free surface as well as for cases in which the contaminant mass flux is prescribed at the surface.

Journal of Contaminant Hydrology↗

USGS1996

Characterization of metal adsorption variability in a sand and gravel aquifer, Cape Cod, Massachusetts, U.S.A

Several geochemical properties of an aquifer sediment that control metal-ion adsorption were investigated to determine their potential use as indicators of the spatial variability of metal adsorption. Over the length of a 4.5-m-long core from a sand and gravel aquifer, lead (Pb2+) and zinc (Zn2+) adsorption at constant chemical conditions (pH 5.3) varied by a factor of 2 and 4, respectively. Pb2+ and Zn2+ were adsorbed primarily by Fe- and Al-oxide coatings on quartz-grain surfaces. Per unit surface area, both Pb2+ and Zn2+ adsorption were significantly correlated with the amount of Fe and Al that dissolved from the aquifer material in a partial chemical extraction. The variability in conditional binding constants for Pb2+ and Zn2+ adsorption (log KADS) derived from a simple non-electrostatic surface complexation model were also predicted by extracted Fe and Al normalized to surface area. Because the abundance of Fe- and Al-oxide coatings that dominate adsorption does not vary inversely with grain size by a simple linear relationship, only a weak, negative correlation was found between the spatial variability of Pb2+ adsorption and grain size in this aquifer. The correlation between Zn2+ adsorption and grain size was not significant. Partial chemical extractions combined with surface-area measurements have potential use for estimating metal adsorption variability in other sand and gravel aquifers of negligible carbonate and organic carbon content.

Massachusetts↗

USGS2004

Effect of cell physicochemical characteristics and motility on bacterial transport in groundwater

The influence of physicochemical characteristics and motility on bacterial transport in groundwater were examined in flow-through columns. Four strains of bacteria isolated from a crystalline rock groundwater system were investigated, with carboxylate-modified and amidine-modified latex microspheres and bromide as reference tracers. The bacterial isolates included a gram-positive rod (ML1), a gram-negative motile rod (ML2), a nonmotile mutant of ML2 (ML2m), and a gram-positive coccoid (ML3). Experiments were repeated at two flow velocities, in a glass column packed with glass beads, and in another packed with iron-oxyhydroxide coated glass beads. Bacteria breakthrough curves were interpreted using a transport equation that incorporates a sorption model from microscopic observation of bacterial deposition in flow-cell experiments. The model predicts that bacterial desorption rate will decrease exponentially with the amount of time the cell is attached to the solid surface. Desorption kinetics appeared to influence transport at the lower flow rate, but were not discernable at the higher flow rate. Iron-oxyhydroxide coatings had a lower-than-expected effect on bacterial breakthrough and no effect on the microsphere recovery in the column experiments. Cell wall type and shape also had minor effects on breakthrough. Motility tended to increase the adsorption rate, and decrease the desorption rate. The transport model predicts that at field scale, desorption rate kinetics may be important to the prediction of bacteria transport rates. ?? 2003 Elsevier B.V. All rights reserved.

Journal of Contaminant Hydrology↗

USGS2004

Direct-push geochemical profiling for assessment of inorganic chemical heterogeneity in aquifers

Discrete-depth sampling of inorganic groundwater chemistry is essential for a variety of site characterization activities. Although the mobility and rapid sampling capabilities of direct-push techniques have led to their widespread use for evaluating the distribution of organic contaminants, complementary methods for the characterization of spatial variations in geochemical conditions have not been developed. In this study, a direct-push-based approach for high-resolution inorganic chemical profiling was developed at a site where sharp chemical contrasts and iron-reducing conditions had previously been observed. Existing multilevel samplers (MLSs) that span a fining-upward alluvial sequence were used for comparison with the direct-push profiling. Chemical profiles obtained with a conventional direct-push exposed-screen sampler differed from those obtained with an adjacent MLS because of sampler reactivity and mixing with water from previous sampling levels. The sampler was modified by replacing steel sampling components with stainless-steel and heat-treated parts, and adding an adapter that prevents mixing. Profiles obtained with the modified approach were in excellent agreement with those obtained from an adjacent MLS for all constituents and parameters monitored (Cl, NO3, Fe, Mn, DO, ORP, specific conductance and pH). Interpretations of site redox conditions based on field-measured parameters were supported by laboratory analysis of dissolved Fe. The discrete-depth capability of this approach allows inorganic chemical variations to be described at a level of detail that has rarely been possible. When combined with the mobility afforded by direct-push rigs and on-site methods of chemical analysis, the new approach is well suited for a variety of interactive site-characterization endeavors. ?? 2003 Elsevier B.V. All rights reserved.

Journal of Contaminant Hydrology↗

USGS2004

Degradation of 1,1,2,2-tetrachloroethane and accumulation of vinyl chloride in wetland sediment microcosms and in situ porewater: Biogeochemical controls and associations with microbial communities

The biodegradation pathways of 1,1,2,2-tetrachloroethane (TeCA) and 1,1,2-trichloroethane (112TCA) and the associated microbial communities in anaerobic wetland sediments were evaluated using concurrent geochemical and genetic analyses over time in laboratory microcosm experiments. Experimental results were compared to in situ porewater data in the wetland to better understand the factors controlling daughter product distributions in a chlorinated solvent plume discharging to a freshwater tidal wetland at Aberdeen Proving Ground, Maryland. Microcosms constructed with wetland sediment from two sites showed little difference in the initial degradation steps of TeCA, which included simultaneous hydrogenolysis to 112TCA and dichloroelimination to 1,2-dichloroethene (12DCE). The microcosms from the two sites showed a substantial difference, however, in the relative dominance of subsequent dichloroelimination of 112TCA. A greater dominance of 112TCA dichloroelimination in microcosms constructed with sediment that was initially iron-reducing and subsequently simultaneously iron-reducing and methanogenic caused approximately twice as much vinyl chloride (VC) production as microcosms constructed with sediment that was methanogenic only throughout the incubation. The microcosms with higher VC production also showed substantially more rapid VC degradation. Field measurements of redox-sensitive constituents, TeCA, and its anaerobic degradation products along flowpaths in the wetland porewater also showed greater production and degradation of VC with concurrent methanogenesis and iron reduction. Molecular fingerprinting indicated that bacterial species [represented by a peak at a fragment size of 198 base pairs (bp) by MnlI digest] are associated with VC production from 112TCA dichloroelimination, whereas methanogens (190 and 307 bp) from the Methanococcales or Methanobacteriales family are associated with VC production from 12DCE hydrogenolysis. Acetate-utilizing methanogens (acetotrophs) appear to be involved in the biodegradation of VC. The relative abundance of Methanosarcinaceae, the only methanogen group with acetotrophic members, doubled in microcosms in which degradation of VC was observed. In addition, molecular analyses using primers specific for known dehalorespiring bacteria in the Dehalococcoides and Desulfuromonas groups showed the presence of these bacteria in microcosm slurry from the site that showed the highest VC production and degradation. Determination of biogeochemical controls and microbial consortia involved in TeCA degradation is leading to a better understanding of the heterogeneity in biodegradation rates and daughter product distribution in the wetland, improving capabilities for developing remediation and monitoring plans.

Journal of Contaminant Hydrology↗

USGS2004

Mechanisms of electron acceptor utilization: Implications for simulating anaerobic biodegradation

Simulation of biodegradation reactions within a reactive transport framework requires information on mechanisms of terminal electron acceptor processes (TEAPs). In initial modeling efforts, TEAPs were approximated as occurring sequentially, with the highest energy-yielding electron acceptors (e.g. oxygen) consumed before those that yield less energy (e.g., sulfate). Within this framework in a steady state plume, sequential electron acceptor utilization would theoretically produce methane at an organic-rich source and Fe(II) further downgradient, resulting in a limited zone of Fe(II) and methane overlap. However, contaminant plumes often display much more extensive zones of overlapping Fe(II) and methane. The extensive overlap could be caused by several abiotic and biotic processes including vertical mixing of byproducts in long-screened monitoring wells, adsorption of Fe(II) onto aquifer solids, or microscale heterogeneity in Fe(III) concentrations. Alternatively, the overlap could be due to simultaneous utilization of terminal electron acceptors. Because biodegradation rates are controlled by TEAPs, evaluating the mechanisms of electron acceptor utilization is critical for improving prediction of contaminant mass losses due to biodegradation. Using BioRedox-MT3DMS, a three-dimensional, multi-species reactive transport code, we simulated the current configurations of a BTEX plume and TEAP zones at a petroleum- contaminated field site in Wisconsin. Simulation results suggest that BTEX mass loss due to biodegradation is greatest under oxygen-reducing conditions, with smaller but similar contributions to mass loss from biodegradation under Fe(III)-reducing, sulfate-reducing, and methanogenic conditions. Results of sensitivity calculations document that BTEX losses due to biodegradation are most sensitive to the age of the plume, while the shape of the BTEX plume is most sensitive to effective porosity and rate constants for biodegradation under Fe(III)-reducing and methanogenic conditions. Using this transport model, we had limited success in simulating overlap of redox products using reasonable ranges of parameters within a strictly sequential electron acceptor utilization framework. Simulation results indicate that overlap of redox products cannot be accurately simulated using the constructed model, suggesting either that Fe(III) reduction and methanogenesis are occurring simultaneously in the source area, or that heterogeneities in Fe(III) concentration and/or mineral type cause the observed overlap. Additional field, experimental, and modeling studies will be needed to address these questions. ?? 2004 Elsevier B.V. All rights reserved.

Journal of Contaminant Hydrology↗

USGS2004

Field investigation into unsaturated flow and transport in a fault: Model analyses

Results of a fault test performed in the unsaturated zone of Yucca Mountain, Nevada, were analyzed using a three-dimensional numerical model. The fault was explicitly represented as a discrete feature and the surrounding rock was treated as a dual-continuum (fracture-matrix) system. Model calibration against seepage and water-travel-velocity data suggests that lithophysal cavities connected to fractures can considerably enhance the effective fracture porosity and therefore retard water flow in fractures. Comparisons between simulation results and tracer concentration data also indicate that matrix diffusion is an important mechanism for solute transport in unsaturated fractured rock. We found that an increased fault-matrix and fracture-matrix interface areas were needed to match the observed tracer data, which is consistent with previous studies. The study results suggest that the current site-scale model for the unsaturated zone of Yucca Mountain may underestimate radionuclide transport time within the unsaturated zone, because an increased fracture-matrix interface area and the increased effective fracture porosity arising from lithophysal cavities are not considered in the current site-scale model. ?? 2004 Published by Elsevier B.V.

Journal of Contaminant Hydrology↗

USGS2005

Numerical methods for improving sensitivity analysis and parameter estimation of virus transport simulated using sorptive-reactive processes

Using one- and two-dimensional homogeneous simulations, this paper addresses challenges associated with sensitivity analysis and parameter estimation for virus transport simulated using sorptive-reactive processes. Head, flow, and conservative- and virus-transport observations are considered. The paper examines the use of (1) observed-value weighting, (2) breakthrough-curve temporal moment observations, and (3) the significance of changes in the transport time-step size. The results suggest that (1) sensitivities using observed-value weighting are more susceptible to numerical solution variability, (2) temporal moments of the breakthrough curve are a more robust measure of sensitivity than individual conservative-transport observations, and (3) the transport-simulation time step size is more important than the inactivation rate in solution and about as important as at least two other parameters, reflecting the ease with which results can be influenced by numerical issues. The approach presented allows more accurate evaluation of the information provided by observations for estimation of parameters and generally improves the potential for reasonable parameter-estimation results. ?? 2004 Elsevier B.V. All rights reserved.

Journal of Contaminant Hydrology↗

USGS2005

Reply to “Commentary: Assessment of past infiltration fluxes through Yucca Mountain on the basis of the secondary mineral record—Is it a viable methodology?” by Y.V. Dublyansky and S.Z. Smirnov

Many of the comments by Dublyansky and Smirnov (2005) on Marshall et al. (2003) reflect a longstanding debate over the origin of secondary calcite and opal deposits found in cavities and on fracture surfaces at Yucca Mountain, Nevada, site of a proposed high-level nuclear waste repository (US Department of Energy, 2001). These comments require consideration of data and interpretations beyond the scope of Marshall et al. (2003). Dublyansky et al. (2004) and Dublyansky et al. (2005) also have commented on papers published by Whelan et al. (2002) and Wilson et al. (2003), and we will refer to the replies to those comments (Whelan et al., 2004, Wilson and Cline, 2005) in addressing the comments that go beyond the scope of Marshall et al. (2003).

Nevada↗

USGS2005

Parameter and observation importance in modelling virus transport in saturated porous media - Investigations in a homogenous system

This paper evaluates the importance of seven types of parameters to virus transport: hydraulic conductivity, porosity, dispersivity, sorption rate and distribution coefficient (representing physical-chemical filtration), and in-solution and adsorbed inactivation (representing virus inactivation). The first three parameters relate to subsurface transport in general while the last four, the sorption rate, distribution coefficient, and in-solution and adsorbed inactivation rates, represent the interaction of viruses with the porous medium and their ability to persist. The importance of four types of observations to estimate the virus-transport parameters are evaluated: hydraulic heads, flow, temporal moments of conservative-transport concentrations, and virus concentrations. The evaluations are conducted using one- and two-dimensional homogeneous simulations, designed from published field experiments, and recently developed sensitivity-analysis methods. Sensitivity to the transport-simulation time-step size is used to evaluate the importance of numerical solution difficulties. Results suggest that hydraulic conductivity, porosity, and sorption are most important to virus-transport predictions. Most observation types provide substantial information about hydraulic conductivity and porosity; only virus-concentration observations provide information about sorption and inactivation. The observations are not sufficient to estimate these important parameters uniquely. Even with all observation types, there is extreme parameter correlation between porosity and hydraulic conductivity and between the sorption rate and in-solution inactivation. Parameter estimation was accomplished by fixing values of porosity and in-solution inactivation.

Journal of Contaminant Hydrology↗

USGS2006

Simulation of solute transport across low-permeability barrier walls

Low-permeability, non-reactive barrier walls are often used to contain contaminants in an aquifer. Rates of solute transport through such barriers are typically many orders of magnitude slower than rates through the aquifer. Nevertheless, the success of remedial actions may be sensitive to these low rates of transport. Two numerical simulation methods for representing low-permeability barriers in a finite-difference groundwater-flow and transport model were tested. In the first method, the hydraulic properties of the barrier were represented directly on grid cells and in the second method, the intercell hydraulic-conductance values were adjusted to approximate the reduction in horizontal flow, allowing use of a coarser and computationally efficient grid. The alternative methods were tested and evaluated on the basis of hypothetical test problems and a field case involving tetrachloroethylene (PCE) contamination at a Superfund site in New Hampshire. For all cases, advective transport across the barrier was negligible, but preexisting numerical approaches to calculate dispersion yielded dispersive fluxes that were greater than expected. A transport model (MODFLOW-GWT) was modified to (1) allow different dispersive and diffusive properties to be assigned to the barrier than the adjacent aquifer and (2) more accurately calculate dispersion from concentration gradients and solute fluxes near barriers. The new approach yields reasonable and accurate concentrations for the test cases.

Journal of Contaminant Hydrology↗