The velocity of DNAPL fingering in water-saturated porous media: laboratory experiments and a mobile–immobile–zone model

Dense nonaqueous phase liquids (DNAPLs) are immiscible with water and can give rise to highly fingered fluid distributions when infiltrating through water-saturated porous media. In this paper, a conceptual mobile–immobile–zone (MIZ) model is presented to describe the structure of a DNAPL finger in water-saturated porous media and the velocity of finger propagation. A finger is composed of a finger body and a tip. The finger body has a mobile core and an immobile sheath. All the DNAPL within the tip of a finger is mobile. Lab experiments utilizing image analyses of a DNAPL (PCE) penetrating into water-saturated homogeneous glass beads were carried out in a two-dimensional transparent chamber. The results show that the fingers elongated almost linearly with time. The fingers did not grow laterally after the tip of the finger had passed. The average finger diameters were between 3.9 and 5.4 mm for PCE propagation in water-saturated glass bead porous media with mean particle diameters from 0.32 to 1.36 mm. The estimated mobile core diameters were 51–60% of the average finger diameters.     

Determining effective interfacial tension and predicting finger spacing for DNAPL penetration into water-saturated porous media

The difficulty in determining the effective interfacial tension limits the prediction of the wavelength of fingering of immiscible fluids in porous media. A method to estimate the effective interfacial tension using fractal concepts was presented by Chang et al. [Water Resour. Res. 30 (1994) 125]. We modified the method in that the macroscopic interface length was used instead of the system width. Methods to determine the macroscopic and the microscopic interface length are given. Lab experiments of dense nonaqueous phase liquid (DNAPL) penetrating into water-saturated glass beads were carried out in a two-dimensional (2-D) transparent chamber. The displacement processes were recorded using a 35-mm camera or a video camera, which was directly connected to and controlled by a computer. Unlike the method of Chang et al. (1994), the modified method used here gives a constant value of the effective interfacial tension over time. The predicted wavelengths of fingering are relatively close to those observed except for the fine beads.     

Multidimensional validation of a numerical model for simulating a DNAPL release in heterogeneous porous media

A fixed-volume release of 1,2-DCE, tracked in space and time with a light transmission/image analysis system, provided a data set for the infiltration, redistribution, and immobilisation of a dense non-aqueous phase liquid (DNAPL) in a heterogeneous porous medium. The two-dimensional bench scale flow cell was packed with a spatially correlated, random heterogeneous distribution of six sand types. In order to provide the necessary modelling parameters, detailed constitutive relationships were measured at the local scale for the six sands. These experiments revealed that nonwetting phase (NWP) relative permeability-saturation (k(rN)-S(W)) relationships are strongly correlated to sand type. Trends in the best-fit k(rN)-S(W) parameters reflected a positive correlation between mean grain diameter and the maximum NWP relative permeability, k(rN)(max). Multiphase flow simulations of the bench scale experiment best reproduced the experimental observations, producing excellent matches in both time and space, when the measured, correlated local scale k(rN)-S(W) relationships were employed.     

Quantitative imaging of contaminant distributions in heterogeneous porous media laboratory experiments

Intermediate-scale laboratory experiments on heterogeneous porous media have been increasingly used for the study of saturated and unsaturated ground water systems. While the ability to reproduce field-scale heterogeneity in these experiments has advanced, the use of visualization or image analysis methods to characterize the spatial distribution of solute concentrations has largely remained at the homogeneous media level. To advance these imaging techniques we developed a generic image analysis package that, for the first time, automatically segments regions in photographic images that require unique concentration calibration curves due to varying porous media properties or lighting nonuniformities. As a robust test, our image analysis package was applied to an intermediate-scale flow tank experiment characterized by a correlated random permeability field with unprecedented resolution. Twenty-five distinct classes of porous media were developed and binned to the synthetic permeability field, creating an experimental field of 3456 rectangular cells and thereby ensuring the emplaced field closely matched the statistics of the original continuous distribution. Concentration distributions were determined for an experimental tracer run and the corresponding dispersion parameters were calculated. The closeness of the experimental, image-processed longitudinal dispersivity (4.6 x 10(-2) m) to that obtained from the field statistics (9.1 x 10(-2) m) verifies our image analysis technique.     

The effect of entrapped nonaqueous phase liquids on tracer transport in heterogeneous porous media: laboratory experiments at the intermediate scale

This work considers the applicability of conservative tracers for detecting high-saturation nonaqueous-phase liquid (NAPL) entrapment in heterogeneous systems. For this purpose, a series of experiments and simulations was performed using a two-dimensional heterogeneous system (10x1.2 m), which represents an intermediate scale between laboratory and field scales. Tracer tests performed prior to injecting the NAPL provide the baseline response of the heterogeneous porous medium. Two NAPL spill experiments were performed and the entrapped-NAPL saturation distribution measured in detail using a gamma-ray attenuation system. Tracer tests following each of the NAPL spills produced breakthrough curves (BTCs) reflecting the impact of entrapped NAPL on conservative transport. To evaluate significance, the impact of NAPL entrapment on the conservative-tracer breakthrough curves was compared to simulated breakthrough curve variability for different realizations of the heterogeneous distribution. Analysis of the results reveals that the NAPL entrapment has a significant impact on the temporal moments of conservative-tracer breakthrough curves.     

Microbial growth and transport in porous media under denitrification conditions: experiments and simulations

Soil column experiments were conducted to study bacterial growth and transport in porous media under denitrifying conditions. The study used a denitrifying microbial consortium isolated from aquifer sediments sampled at the U.S. Department of Energy's Hanford site. One-dimensional, packed-column transport studies were conducted under two substrate loading conditions. A detailed numerical model was developed to predict the measured effluent cell and substrate concentration profiles. First-order attachment and detachment models described the interphase exchange processes between suspended and attached biomass. Insignificantly different detachment coefficient values of 0.32 and 0.43 day⁻¹, respectively, were estimated for the high and low nitrate loading conditions (48 and 5 mg l⁻¹ NO₃, respectively). Comparison of these values with those calculated from published data for aerobically growing organisms shows that the denitrifying consortium had lower detachment rate coefficients. This suggests that, similar to detachment rates in reactor-grown biofilms, detachment in porous media may increase with microbial growth rate. However, available literature data are not sufficient to confirm a specific analytical model for predicting this growth dependence.     

Miscible fluid displacement stability in unconfined porous media:: Two-dimensional flow experiments and simulations

In situ flushing groundwater remediation technologies, such as cosolvent flushing, rely on the stability of the interface between the resident and displacing fluids for efficient removal of contaminants. Contrasts in density and viscosity between the resident and displacing fluids can adversely affect the stability of the displacement front. Petroleum engineers have developed techniques to describe these types of processes; however, their findings do not necessarily translate directly to aquifer remediation. The purpose of this laboratory study was to investigate how density and viscosity contrasts affected cosolvent displacements in unconfined porous media characterized by the presence of a capillary fringe. Two-dimensional flow laboratory experiments, which were partially scaled to a cosolvent flushing field experiment, were conducted to determine potential implications of flow instabilities in homogeneous sand packs. Numerical simulations were also conducted to investigate the differential impact of fluid property contrasts in unconfined and confined systems. The results from these experiments and simulations indicated that the presence of a capillary fringe was an important factor in the displacement efficiency. Buoyant forces can act to carry a lighter-than-water cosolvent preferentially into the capillary fringe during displacement of the resident groundwater. During subsequent water flooding, buoyancy forces can act to effectively trap the cosolvent in the capillary fringe, contributing to the inefficient removal of cosolvent from the aquifer.     

Variable-density flow in heterogeneous porous media — Laboratory experiments and numerical simulations

Konz, M., Ackerer, P., Younes, A., Huggenberger, P., Zechner, E., 2009a. 2D Stable Layered Laboratory-scale Experiments for Testing Density-coupled Flow Models. Water Resources Research, 45. doi:10.1029/2008WR007118., a series of laboratory-scale 2D tank experiments were conducted and accurately simulated for density driven flow problems on homogeneous porous media. In the present work, we extended the numerical and experimental studies to heterogeneous problems. The heterogeneous porous medium was constructed with a low permeability zone in the centre of the tank and had well-defined parameters and boundary conditions. Concentration distributions were measured in high resolution using a photometric method and an image analysis technique. The numerical model used for the simulations was based on efficient advanced approximations for both spatial and temporal discretizations. The Method Of Lines (MOL) was used to allow higher-order temporal discretization. Three different boundary conditions, corresponding to different localizations of the inflow and the outflow openings at the opposite edges of the tank, were applied to investigate different flow scenarios in the heterogeneous porous medium flow tank. Simulation results of all three density coupled experiments revealed a density-dependent behavior of dispersion. Thus, a reduction of dispersivites was required to obtain a good matching of the experimental data. The high quality of the experiments enabled a detailed testing of numerical variable-density flow codes under heterogeneous conditions. Therefore, the experiments were considered to be reliable benchmark tests.     

Cesium migration in Hanford sediment: a multisite cation exchange model based on laboratory transport experiments

Cs+ transport experiments carried out in columns packed with uncontaminated Hanford formation sediment from the SX tank farm provide strong support for the use of a multisite, multicomponent cation exchange model to describe Cs+ migration in the Hanford vadose zone. The experimental results indicate a strong dependence of the effective Cs+ Kd on the concentrations of other cations, including Na+ that is present at high to extremely high concentrations in fluids leaking from the Hanford SX tanks. A strong dependence of the Cs+ Kd on the aqueous Cs+ concentration is also apparent, with retardation of Cs+ increasing from a value of 41 at a Cs+ concentration of 10(-4) M in the feed solution to as much as 282 at a Cs+ concentration of 5x10(-7) M, all in a background of 1 M NaNO3. The total cation exchange capacity (CEC) of the Hanford sediment was determined using 22Na isotopic equilibrium exchange in a flow-through column experiment. The value for the CEC of 120 microeq/g determined with this method is compatible with a value of 121.9 microeq/g determined by multi-cation elution. While two distinct exchange sites were proposed by Zachara et al. [Geochim. Cosmochim. Acta 66 (2002) 193] based on binary batch exchange experiments, a third site is proposed in this study to improve the fit of the Cs+-Na+ and Cs+-Ca+ exchange data and to capture self-sharpened Cs+ breakthrough curves at low concentrations of Cs+. Two of the proposed exchange sites represent frayed edge sites (FES) on weathered micas and constitute 0.02% and 0.22% of the total CEC. Both of the FES show a very strong selectivity for Cs+ over Na+ (K(Na-Cs)=10(7.22) and 10(4.93), respectively). The third site, accounting for over 99% of the total CEC, is associated with planar sites on expansible clays and shows a smaller Na+-Cs+ selectivity coefficient of 10(1.99). Parameters derived from a fit of binary batch experiments alone tend to under predict Cs+ retardation in the column experiments. The transport experiments indicate 72-90% of the Cs+ sorbed in experiments targeting exchange on FES was desorbed over a 10- and 24-day period, respectively. At high Cs+ concentrations, where sorption is controlled primarily by exchange on planar sites, 95% of the Cs+ desorption was desorbed. Most of the difficulty in desorbing Cs+ from FES is a result of the extremely high selectivity of these sites for Cs+, although truly irreversible sorption as high as 23% was suggested in one experiment. The conclusion that Cs+ exchange is largely reversible in a thermodynamic sense is supported by the ability to match Cs+ desorption curves almost quantitatively with an equilibrium reactive transport simulation. The model for Cs+ retardation developed here qualitatively explains the behavior of Cs+ in the Hanford vadose zone underneath a variety of leaking tanks with differing salt concentrations. The high selectivity of FES for Cs+ implies that future desorption and migration is very unlikely to occur under natural recharge conditions.     

Illuminating reactive microbial transport in saturated porous media: demonstration of a visualization method and conceptual transport model

We demonstrate a method to study reactive microbial transport in saturated translucent porous media using the bacteria Pseudomonas fluorescens 5RL genetically engineered to carry a plasmid with bioluminescence genes inducible by salicylate. Induced bacteria were injected into a cryolite grain filled chamber saturated with a sterile non-growth-promoting (phosphorus limited) chemical mixture containing salicylate as an aromatic hydrocarbon analogue. The amount of light produced by the bacteria serves as an estimator of the relative efficiency of aerobic biodegradation since bioluminescence is dependent on both salicylate and oxygen but only consumes oxygen. Bioluminescence was captured with a digital camera and analyzed to study the evolving spatial pattern of the bulk oxygen consuming reactions. As fluid flow transported the bacteria through the chamber, bioluminescence was observed to initially increase until an oxygen depletion zone developed behind the advective front. Bacterial transport was modeled with the advection dispersion equation and oxygen concentration was modeled assuming bacterial consumption via Monod kinetics with consideration of additional effects of rate-limited mass transfer from residual gas bubbles. Consistent with previous measurements, bioluminescence was considered proportional to oxygen consumed. Using the observed bioluminescence, model parameters were fit that were consistent with literature values and produced results in good agreement with the experimental data. These findings demonstrate potential for using this method to investigate the complex spatial and temporal dynamics of reactive microbial transport in saturated porous media.     

Stochastic-convective transport with nonlinear reaction and mixing: application to intermediate-scale experiments in aerobic biodegradation in saturated porous media

Aerobic biodegradation of benzoate by Pseudomonas cepacia sp. in a saturated heterogeneous porous medium was simulated using the stochastic-convective reaction (SCR) approach. A laboratory flow cell was randomly packed with low permeability silt-size inclusions in a high permeability sand matrix. In the SCR upscaling approach, the characteristics of the flow field are determined by the breakthrough of a conservative tracer. Spatial information on the actual location of the heterogeneities is not used. The mass balance equations governing the nonlinear and multicomponent reactive transport are recast in terms of reactive transports in each of a finite number of discrete streamtubes. The streamtube ensemble members represent transport via a steady constant average velocity per streamtube and a conventional Fickian dispersion term, and their contributions to the observed breakthroughs are determined by flux-averaging the streamtube solute concentrations. The resulting simulations were compared to those from a high-resolution deterministic simulation of the reactive transport, and to alternative ensemble representations involving (i) effective Fickian travel time distribution function, (ii) purely convective streamtube transport, and (iii) streamtube ensemble subset simulations. The results of the SCR simulation compare favorably to that of a sophisticated high-resolution deterministic approach.     

The effect of a biofilm on solute diffusion in fractured porous media

At sites in fractured rock where contamination has been exposed to the rock matrix for extended periods of time, the amount of contaminant mass residing in the matrix can be considerable. Even though it may be possible to diminish concentrations by the advection of clean water through the fracture features, back diffusion from mass held in the matrix will lead to a continuing source of contamination. In such an event, the development of a biofilm (a thin film of microbial mass) on the wall of the fractures may act to limit or prevent the back diffusion process. The objective of this preliminary study is to explore the influence imparted by the presence of a biofilm on the process of matrix diffusion. The investigation was conducted using radial diffusion cells constructed from rock core in which biofilm growth was stimulated in a central reservoir. Once biofilms were developed, forward diffusion experiments were conducted in which a conservative solute migrated from the central reservoir into the intact rock sample. Diffusion experiments were performed in a total of 11 diffusion cell pairs where biofilm growth was stimulated in one member of the pair and inhibited in the other. The effect of the presence of a biofilm on tracer diffusion was determined by comparison of the diffusion curves produced by each cell pair. A semi-analytical model that accounts for the presence of a biofilm was used to investigate the effect of the biofilm on mass transfer due to changes in the effective porosity, effective diffusion coefficient, and the depth of penetration of the biofilm into the intact rock. The results show that the biofilm acted to plug the rock matrix, rather than forming a discrete layer on the reservoir surface. The reduction in effective porosity due to the biofilm ranged from 6% to 52% with the majority of the samples in the 30% to 50% range. Based on the present results, with more efficient biofilm stimulation, it is reasonable to assume that a more complete plugging of the microcrack porosity might be possible, leaving a much thicker and efficient barrier than could be achieved via a surface biofilm.     

A review on reactive transport model and porosity evolution in the porous media

Environmental Science and Pollution Research - This work comprehensively reviews the equations governing multicomponent flow and reactive transport in porous media on the pore-scale, mesoscale and...     

A numerical model for transient-hysteretic flow and solute transport in unsaturated porous media

A two-dimensional flow and transport model was developed for simulating transient water flow and nonreactive solute transport in heterogeneous, unsaturated porous media containing air and water. The model is composed of a unique combination of robust and accurate numerical algorithms for solving the Richards', Darcy flux, and advection-dispersion equations. The mixed form of Richards' equation is solved using a finite-element formulation and a modified Picard iteration scheme. Mass lumping is employed to improve solution convergence and stability behavior. The flow algorithm accounts for hysteresis in the pressure head-water content relationship. Darcy fluxes are approximated with a Galerkin and Petrov-Galerkin finite-element method developed for random heterogeneous porous media. The transport equation is solved using an Eulerian-Lagrangian method. A multi-step, fourth-order Runge-Kutta, reverse particle tracking technique and a quadratic-linear interpolation scheme are shown to be superior for determining the advective concentration. A Galerkin finite-element method is used for approximating the dispersive flux. The unsaturated flow and transport model was applied to a variety of rigorous problems and was found to produce accurate, mass-conserving solutions when compared to analytical solutions and published numerical results.     

Transport of a decay chain in homogenous porous media: analytical solutions

With the aid of integral transforms, analytical solutions for the transport of a decay chain in homogenous porous media are derived. Unidirectional steady-state flow and radial steady-state flow in single and multiple porosity media are considered. At least in Laplace domain, all solutions can be written in closed analytical formulae. Partly, the solutions can also be inverted analytically. If not, analytical calculation of the steady-state concentration distributions, evaluation of temporal moments and numerical inversion are still possible. Formulae for several simple boundary conditions are given and visualized in this paper. The derived novel solutions are widely applicable and are very useful for the validation of numerical transport codes.     

Nonideal transport of contaminants in heterogeneous porous media: 10. Impact of co-solutes on sorption by porous media with low organic-carbon contents

The impact of co-solutes on sorption of tetrachloroethene (PCE) by two porous media with low organic-carbon contents was examined by conducting batch experiments. The two media (Borden and Eustis) have similar physical properties, but significantly different organic-carbon (OC) contents. Sorption of PCE was nonlinear for both media, and well-described by the Freundlich equation. For the Borden aquifer material (OC = 0.03%), the isotherms measured with a suite of co-solutes present (1,2-dichlorobenzene, bromoform, carbon tetrachloride, and hexachloroethane) were identical to the isotherms measured for PCE alone. These results indicate that there was no measurable impact of the co-solutes on PCE sorption for this system. In contrast to the Borden results, there was a measurable reduction in sorption of PCE by the Eustis soil (OC = 0.38%) in the presence of the co-solutes. The organic-carbon fractions of both media contain hard-carbon components, which have been associated with the manifestation of nonideal sorption phenomena. The disparity in results observed for the two media may relate to relative differences in the magnitude and geochemical nature of these hard-carbon components.     

Dechlorination after thermal treatment of a TCE-contaminated aquifer: laboratory experiments

A microcosm study was conducted to evaluate dechlorination of trichloroethene (TCE) to ethene and survival of dechlorinating bacteria after a thermal treatment in order to explore the potential for post-thermal bioremediation. Unamended microcosms containing groundwater and aquifer material from a contaminated site dechlorinated TCE to cis-1,2-dichloroethene (cDCE), while lactate-amended microcosms dechlorinated TCE to cDCE or ethene. A thermal treatment was simulated by heating a sub-set of microcosms to 100 degrees C for 10d followed by cooling to 10 degrees C over 150 d. The heated microcosms demonstrated no dechlorination when unamended. However, when amended with lactate, cDCE was produced in 2 out of 6 microcosms within 300 d after heating. Dechlorination of TCE to cDCE thus occurred in fewer heated (2 out of 12) than unheated (10 out of 12) microcosms. In unheated microcosms, the presence of dechlorinating microorganisms, including Dehalococcoides, was confirmed using nested PCR of 16S rRNA genes. Dechlorinating microorganisms were detected in fewer microcosms after heating, and Dehalococcoides were not detected in any microcosms after heating. Dechlorination may therefore be limited after a thermal treatment in areas that have been heated to 100 degrees C. Thus, inflow of groundwater containing dechlorinating microorganisms and/or bioaugmention may be needed for anaerobic dechlorination to occur after a thermal treatment.     

Bacteriophage transport through a fining-upwards sedimentary sequence: laboratory experiments and simulation

A column containing four concentric layers of progressively finer-grained glass beads (graded column) was used to study the transport of the bacteriophage T7 in water flowing parallel to layering through a fining-upwards (FU) sedimentary structure. By passing a pulse of T7, and a conservative solute tracer upwards through a column packed with a single bead size (uniform column), the capacity of each bead type to attenuate the bacteriophage was determined. Solute and bacteriophage responses were modelled using an analytical solution to the advection-dispersion equation, with first-order kinetic deposition simulating bacteriophage attenuation. Resulting deposition constants for different flow velocities indicated that filtration theory-determined values differed from experimentally determined values by less than 10%. In contrast, the responses of solute and bacteriophage tracers passing upwards through graded columns could not be reproduced with a single analytical solution. However, a flux-weighted summation of four one-dimensional advective-dispersive analytical terms approximated solute breakthrough curves. The prolonged tailing observed in the resulting curve resembled that typically generated from field-based tracer test data, reflecting the potential importance of textural heterogeneity in the transport of dissolved substances in groundwater. Moreover, bacteriophage deposition terms, determined from filtration theory, reproduced the T7 breakthrough curve once desorption and inactivation on grain surfaces were incorporated. To evaluate the effect of FU sequences on mass transport processes in more detail, bacteriophage passage through sequences resembling those sampled from a FU bed in a fluvioglacial gravel pit were carried out using an analogous approach to that employed in the laboratory. Both solute and bacteriophage breakthrough responses resembled those generated from field-based test data and in the graded column experiments. Comparisons with the results of simulations using averaged hydraulic conductivities show that simulations employing averaged parameters overestimate bacteriophage travel times and underestimate masses recovered and peak concentrations.     

Mobilization and entry of DNAPL pools into finer sand media by cosolvents: two-dimensional chamber studies

Two-dimensional chamber studies were conducted to determine qualitative and quantitative performance of cosolvents targeted at pooled dense non-aqueous phase liquid (DNAPL) (perchlorethylene, PCE) residing above a fine-grain capillary barrier. Downward mobilization of DNAPL, up gradient along an overriding cosolvent front, was observed. This produced significant pooling above a fine-grain layer that in some cases lead to entry into the capillary barrier beneath. Entry pressure calculations using physical and hydrogeologic parameters provided an excellent prediction of breakthrough of DNAPL into the capillary barrier. Calculations predict approximately 0.5 m of DNAPL would be necessary to enter a Beit Netofa clay, under extreme cosolvent flooding conditions (100% ethanol). Gradient injection of cosolvent did not appear to provide any benefit suggesting a rapid decrease in interfacial tension (IFT) compared to the rate of DNAPL solubilization. Use of a partitioning alcohol (tertiary butyl alcohol, TBA) resulted in DNAPL swelling and reduced entry into the capillary barrier. However, the trapping of flushing solution, containing PCE, could potentially lead to longer remediation times.