Analysis of colloid and tracer breakthrough curves

We consider the dispersion and elution of colloids and dissolved nonsorbing tracers within saturated heterogeneous porous media. Since flow path geometry in natural systems is often ill-characterized macroscopic (mean) flow rates and dispersion tensors are utilized in order to account for the sub-model scale microscopic fluctuations in media structure (and the consequent hydrodynamic profile). Even for tracer migration and dispersal this issue is far from settled.Here we consider how colloid and tracer migration phenomena can be treated consistently. Theoretical calculations for model flow geometries yield two quantitative predictions for the transport of free (not yet captured) colloids with reference to a non-sorbing dissolved tracer within the same medium: the average migration velocity of the free colloids is higher than that of the tracer; and that the ratio of the equivalent hydrodynamic dispersion rates of colloids and tracer is dependent only upon properties of the colloids and the porous medium, it is independent of pathlengths and fluid flux, once length scales are large enough.The first of these is well known, since even in simple flow paths free colloids must stay more centre stream. The second, if validated suggests how solute and colloid dispersion may be dealt with consistently in macroscopic migration models. This is crucial since dispersion is usually ill-characterized and unaddressed by the experimental literature. In this paper we present evidence based upon an existing Drigg field injection test for the validity of these predictions.We show that starting from experimental data the fitted dispersion rates of both colloids and non-sorbing tracers increase with the measured elution rates (obeying slightly different rules for tracers and colloids); and that the ratio of colloid and nonsorbing tracer elution rates, and the ratio of colloid and nonsorbing tracer dispersion rates may be dependent upon properties of the colloids and the medium (not the flow regime).It is important to realize that even for unretarded species, an earlier peak in the breakthrough curve does not necessarily correspond to a faster mean elution rate, or vice versa. But rather that a colloid may elute faster but disperse less than an equivalent tracer. Hence its peak may be retarded compared to that of the tracer, even assuming no retardation. Hence one must consider a combination of mean elution rate and mean dispersion rate, and not rely on “peak times” to corroborate chromatographic effects. The importance of this lies in the fact that these processes are not independent and yet upscale differently. Thus realistic estimates of effective colloid dispersion rates should be upscaled in a way consistent with that adopted for tracers within the same system.     

Effects of sorption on transverse mixing in transient flows

Transverse mixing has been identified as a potentially limiting factor for natural attenuation of plumes originating from continuously emitting sources. Under steady-state flow conditions, dispersion is the only process leading to lateral mixing. This process is very slow and cannot explain the lateral spread of plumes observed in the field. When the flow direction fluctuates with time, transverse dispersion is slightly enhanced, but not very pronounced. Under these flow conditions, however, sorption can contribute to mixing into the mean transverse direction. If the reacting compounds differ in their strength of sorption, chromatographic mixing and separation alternate in time-periodic flows. For instantaneous sorption, the plumes may overlap within a stripe of fixed width. In contrast to sorption in local equilibrium, kinetic sorption contributes to mixing also for compounds with identical sorption strength. I derive an analytical expression for the equivalent transverse dispersion coefficient of a kinetically sorbing compound in a spatially uniform flow field undergoing sinusoidal fluctuations in time. This expression may be used for reactive transport calculations in an equivalent domain with constant flow. The effects are the strongest for compounds with a dimensionless partitioning coefficient of about unity, slow sorption kinetics, and slowly fluctuating velocities. For realistic parameters, kinetic sorption contributes to transverse mixing in the same range as heterogeneity.     

Monte Carlo simulation of nitrogen oxides dispersion from a vehicular exhaust plume and its sensitivity studies

The pollutant dispersion behavior from the vehicular exhaust plume has a direct impact on human health, particularly to the drivers, bicyclists, motorcyclists, pedestrians, people working nearby and vehicle passengers. A two-dimensional pollutant dispersion numerical model was developed based on the joint-scalar probability density function (PDF) approach coupled with a k–ε turbulence model to simulate the initial dispersion process of nitrogen oxides, temperature and flow velocity distributions from a vehicular exhaust plume. A Monte Carlo algorithm was used to solve the PDF transport equations in order to obtain the dispersion distribution of nitrogen oxides concentration. The model was then validated by a series of sensitivity experimental studies in order to assess the effects of vehicular exhaust tailpipe velocities, wind speeds and chemistry on the initial dispersion of NO and NO₂ mass concentrations from the vehicular exhaust plume. The results show that the mass concentrations of nitrogen oxides decrease along the centerline of the vehicular exhaust plume in the downstream distance. The dispersion process can be enhanced when the vehicular exhaust tailpipe velocity is much larger than the wind speed. The oxidation reaction of NO plays an important role when the wind speed is large and the vehicular exhaust exit velocity is small, which leads to chemical reduction of NO, and the formation and accumulation of NO₂ in the exhaust plume. It is also found that the effect of vehicular exhaust-induced turbulence in the vicinity of the exhaust tailpipe exit is more dominant than the effect of wind turbulence, while the wind turbulence gradually shows a significant role for the dispersion of nitrogen oxides along with the development of exhaust plume. The range of dispersion of nitrogen oxides in the radial direction is increased along with the development of vehicular exhaust plume.     

A Microcomputer-based Forecasting Model: Potential Applications for Emergency Response Plans and Air Quality Studies

Most atmospheric transport and diffusion models within emergency response systems have very limited physics and are forced to rely on the assumption that wind and turbulence conditions at the time of the release will be representative over the period for which dispersion must be predicted. For releases where the principal concern is about the first few kilometers of travel, such an assumption is appropriate. However, for large accidental releases during stable conditions, the plume may travel for several hours before it is diluted to safe levels and the assumption of persistence may be inappropriate, particularly for transport in complex terrain. Under these circumstances, a model that can forecast changes in wind and turbulence conditions is required. We have installed such a model on microcomputers and tested it in complex terrain near Salt Lake City. One-hour tracer releases produced surface concentrations that remain high for much longer times than that expected based on one hour’ travel time with the mean wind at the source height. Furthermore, relatively large concentrations were found at distances of over 40 km from the source. The model was generally able to reproduce the principal features described by the measurements, although some effects of subgrid scale terrain were missed.     

Predictive modelling of dispersion controlled reactive plumes at the laboratory-scale

A model-based interpretation of laboratory-scale experimental data is presented. Hydrolysis experiments carried out using thin glass tanks filled with glass beads to construct a hypothetical and inert, homogeneous porous medium were analysed using a 2D numerical model. A new empirical formula, based upon results for non-reactive (tracer) experiments is used to calculate transversal dispersivity values for a range of grain sizes and any flow velocities. Combined with effective diffusion coefficients calculated from Stokes-Einstein type equations, plume lengths arising from mixing between two solutes can be predicted accurately using numerical modelling techniques. Moreover, pH and ion concentration profiles lateral to the direction of flow of the mixing species can be determined at any given point downstream, without the need for result fitting. In our case, this approach does not lead to overpredictions of lateral mixing, as previously reported when using parameters derived from non-reactive tracer experiments to describe reactive solute transport. The theory is based on the assumption of medium homogeneity.     

Short-range atmospheric dispersion over a heterogeneous surface—I. Lateral dispersion

Results are presented from a series of diffusion trials in which a tracer gas, sulphur hexafluoride, was released from an elevated point source over the heterogeneous surface of the Canadian Precambrian Shield. The experimental procedures used in the sampling and analysis of the tracer gas, and in the collection of supporting meteorological information, are described briefly. Physical and meteorological data are presented for 39 successful trials.Under steady-state meteorological conditions, the crosswind concentration distributions were approximately normal in shape. Lateral Gaussian dispersion parameters were extracted from the profiles and compared statistically with the predictions of a number of standard schemes. Best agreement was found with Pasquill's (1976) method, which uses observed wind direction fluctuations to deduce the lateral spread of the plume. The success of Pasquill's method for the rough, heterogeneous surface of the Shield suggests that it may be quite generally applicable. The spread of the plume was found to scale best with meteorological measurements made near the release height, where the flow is characteristic of the heterogeneous surface as a whole. When scaled using Pasquill's procedure, lateral spread is independent of the type of vegetative cover beneath the plume. Similarly, normalized dispersion over a snow-covered surface progresses at the same rate as over a snow-free surface     

Short range dispersion experiments in an urban area

We present results from a series of nine tracer experiments studying urban dispersion at distances under 600 m from a ground level point source in Worcester, Massachusetts. Gaussian forms provide a good fit to the lateral concentration distributions. The measured parameters were compared with models based on stability classification and wind direction fluctuations and to other urban and rural experiments. The comparison showed general consistencies with urban models and data, with some evidence for short range enhancement of the plume. The growth of the cross wind dispersion coefficient (σ_y) and of the standard deviation of wind direction fluctuation (σ_θ) with sampling time were investigated and showed considerably slower growth than is commonly assumed.     

Some observations of pollutant transport associated with elevated plumes

The chemistry of long-range pollutant transport is strongly influenced by atmospheric dispersion characteristics. Recent aircraft plume sampling has suggested that the dispersion growth of elevated plumes may be significantly slower than would be predicted from the well-known behavior of ground-based plumes. The slower growth of the elevated plumes would lead not only to significant plume impact at farther downwind distances but would increase the importance of chemical reactions in the plume and the downwind impact on visibility.Plume dispersion data at large downwind distances are quite limited. Standard diffusion graphs have been extrapolated to 100 km from the wealth of data available at smaller downwind distances.A large number of aircraft flights have been made by Meteorology Research Inc. (MRI) in the last four years under the sponsorship of EPA and others. A number of these flights have sampled individual plumes to distances up to 100 km under a variety of environmental conditions. The data tend to show that elevated plumes (above the surface mixing layer) may grow at a much slower rate than those existing within the boundary layer. Differences in growth rate may be associated with differences in turbulent characteristics or with differences in wind direction (shear) within the two layers.The aircraft data provide an opportunity to extend the dispersion information available at downwind distances that are of importance in intermediate scale pollutant transport. The paper deals with an analysis of these data, an examination of the environmental characteristics associated with the sampling flights and a comparison of the results with the limited supply of observational data already available.     

The long-range dispersion of a plume from an isolated point source

The dispersion of the plume from a sulphide smelter at Mount Isa, Australia, has been determined at distances of up to 1000 km from the source. Simultaneous measurements by an airborne correlation spectrometer, flame photometer and aitken counter have allowed accurate determinations of plume width at these large distances.Radiosonde and pilot-balloon data from four positions spanning the region have been used to calculate the trajectories of each of the plumes measured in the study. In each case the measured plume position was in good agreement with the position predicted on the basis of the wind data.A simple model based on the diurnal variation of the structure of the atmosphere, as well as the turning of the wind with height, is shown to account adequately for the measurements of plume width during well-mixed atmospheric conditions at distances of between 25 and 1000 km from the source.     

Wind-tunnel study of entrainment in two-dimensional dense-gas plumes at the EPA's fluid modeling facility

This wind-tunnel study has been conducted as part of a collaborative effort to investigate the effect of large surface roughness on the entrainment of air from a neutrally stable simulated atmospheric boundary layer into a continuous dense-gas plume. The present study examined the entrainment rates of dense-gas plumes as they were transported over two surfaces with similar geometry but significantly different roughness lengths (factor of 6). Extensive measurements of the flow and plume structures over a wide range of source Richardson numbers (Ri*) are reported. Carbon dioxide was released from a two-dimensional source in order to obtain a plume with virtually constant Ri*. Over the small roughness, the plume depths were generally large compared with the element heights, whereas over the large roughness, plume depths were comparable with the element heights. Retardation of mean velocities in the lower levels of the dense plumes (with compensating increases in the upper levels) was observed, as well as strong suppression of turbulence over quite large fractions of the boundary-layer depth. These effects increased as Ri* increased. Propagation of dense gas was observed upstream of the source due to gravity spreading. The flow within the plumes was observed to become laminar at the larger Ri*. The primary measurements comprised longitudinal surface concentration profiles. Where the plumes were fully turbulent, the plots of inverse concentration versus downwind distance formed reasonably straight lines. The sought-after entrainment velocities are proportional to the slopes of these lines and were found to diminish quite rapidly with Ri*. More in-depth analyses and intercomparisons with the results of the other laboratories are contained in a companion paper in this same volume (Briggs et al., 2001, Atmospheric Environment 35, 2265–2284).     

A controlled field experiment on groundwater contamination by a multicomponent DNAPL: creation of the emplaced-source and overview of dissolved plume development

A unique field experiment has been undertaken at the CFB Borden research site to investigate the development of dissolved chlorinated solvent plumes from a residual dense non-aqueous phase liquid (DNAPL) source. The "emplaced-source" tracer test methodology involved a controlled emplacement of a block-shaped source of sand containing chlorinated solvents below the water table. The gradual dissolution of this residual DNAPL solvent source under natural aquifer conditions caused dissolved solvent plumes of trichloromethane (TCM), trichloroethene (TCE) and perchloroethene (PCE) to continuously develop down gradient. Source dissolution and 3-D plume development were successfully monitored via 173 multilevel samplers over a 475-day tracer test period prior to site remediation research being initiated. Detailed groundwater level and hydraulic conductivity data were collected. Development of plumes with concentrations spanning 1-700,000 micrograms/1 is described and key processes controlling their migration identified. Plumes were observed to be narrow due to the weakness of transverse dispersion processes and long due to advection and significant longitudinal dispersion, very limited sorptive retardation and negligible, if any, attenuation due to biodegradation or abiotic reaction. TCM was shown to be essentially conservative, TCE very nearly conservative and PCE, consistent with its greater hydrophobicity, more retarded yet having a greater mobility than observed in previous Borden field tests. The absence of biodegradation was ascribed to the prevailing aerobic conditions and lack of any additional biodegradable carbon substrates. The transient groundwater flow regime caused significant transverse lateral plume movement, plume asymmetry and was likely responsible for most of the, albeit limited, transverse horizontal plume spreading. In agreement with the widespread incidence of extensive TCE and PCE plumes throughout the industrialized world, the experiment indicates such solvent plumes are likely to be highly mobile and persistent, at least in aquifers that are aerobic and have low sorption potential (low foc content).     

A complex terrain dispersion model for regulatory applications at the Westvaco luke mill

A data set for studying transport and dispersion in complex terrain was collected at the Westvaco Corporation's Luke Mill, located in the Potomac River valley in western Maryland. Meteorological analyses indicate very strong channeling of winds and the presence of strong inversions and wind shears in a shallow layer at the height of the surrounding mountaintops (300 m above the valley floor). Wind velocities observed near the valley floor are unrepresentative of wind velocities at plume height. Observed turbulence intensities at plume height are about twice as large as those observed over flat terrain. Standard stability classification schemes generally underestimate plume dispersion at this site. When high 3-h and 24-h average SO₂ concentrations are observed, winds are usually light and an inversion is present. These instances of relatively high concentrations are often associated with periods when the wind shifts direction 180° from up-valley to down-valley or vice versa, and the nearly stagnant polluted air mass blows against the mountainsides.A dispersion model was developed that is Gaussian in form but uses observed meteorological data to the maximum extent possible. For example, observed turbulence intensities at plume height are used to estimate dispersion. Plume impaction on terrain is calculated if the plume height is below a critical height dependent on the Hill Froude number. Evaluation of the model with the full 2-y data set shows that it can estimate the second highest 3-h and 24-h average concentrations (of regulatory significance) with a mean bias of less than 7%.     

Development,Evaluation, and Application of a Primary Aerosol Model

ABSTRACT

The Segmented-Plume Primary Aerosol Model (SPPAM) has been developed over the past several years. The earlier model development goals were simply to generalize the widely used Industrial Source Complex Short-Term (ISCST) model to simulate plume transport and dispersion under light wind conditions and to handle a large number of roadway or line sources. The goals have been expanded to include development of improved algorithm for effective plume transport velocity, more accurate and efficient line and area source dispersion algorithms, and recently, a more realistic and computationally efficient algorithm for plume depletion due to particle dry deposition. A performance evaluation of the SPPAM has been carried out using the 1983 PNL dual tracer experimental data. The results show the model predictions to be in good agreement with observations in both plume advection-dispersion and particulate matter (PM) depletion by dry deposition. For PM_2.5 impact analysis, the SPPAM has been applied to the Rubidoux area of California. Emission sources included in the modeling analysis are: paved road dust, diesel vehicular exhaust, gasoline vehicular exhaust, and tire wear particles from a large number of roadways in Rubidoux and surrounding areas. For the selected modeling periods, the predicted primary PM_2.5 to primary PM10 concentration ratios for the Rubidoux sampling station are in the range of 0.39–0.46. The organic fractions of the primary PM_2.5 impacts are estimated to be at least 34–41%. Detailed modeling results indicate that the relatively high organic fractions are primarily due to the proximity of heavily traveled roadways north of the sampling station. The predictions are influenced by a number of factors; principal among them are the receptor locations relative to major roadways, the volume and composition of traffic on these roadways, and the prevailing meteorological conditions.     

Modelling of nonreactive tracer dipole tests in a shear zone at the Grimsel test site

The investigation of the migration of a high pH plume in a fractured shear zone is foreseen by a long-term experiment at the Grimsel rock laboratory. In order to characterise the initial conditions for the long-term experiment and to evaluate an optimal hydraulic in situ set-up, several dipole experiments with nonreacting tracers have been performed. The dipole experiments differ in geometry, pumping rates and orientation to the background water flow. Several single and double-porosity models have been applied to fit the results of these dipole tracer tests in order to extract values for some transport parameters and discriminate for certain transport processes. A two-dimensional porous medium approach was successfully used to fit tracer breakthrough curves measured for a dipole experiment. A model based on a one-dimensional dual porous medium approach was also successful, although the applied hydraulic dipole, with similar injection and extraction rates, suggests the existence of an extended two-dimensional flow field. For the two-dimensional porous medium approach, tracer breakthrough could only be fitted with a complex flow field geometry within the heterogeneous fractured shear zone. The heterogeneity was generated by heterogeneous porosity and hydraulic permeability distributions. Predictions for further dipole geometries and a sorbing tracer have been calculated by means of both models using the flow and transport parameters deduced from fits for a single dipole experiment. This allows for comparison with the measured breakthrough of sorbing tracers. The foreseen experiment with sorbing (radionuclide) tracers will help decide on the appropriate approach that should be used to describe such dipole experiments in this shear zone. Additionally, the migration and spreading of a solution with high pH has been calculated taking into account mineral dissolution and precipitation in a two-dimensional porous medium approach in order to estimate the amount and character of the mineral reactions induced by the interaction between the high pH solution and the rock.     

Numerical simulation of scalar dispersion downstream of a square obstacle using gradient-transport type models

We present a numerical study of scalar transport released from a line source downstream of a square obstacle to investigate the capabilities and limitations of gradient-transport modeling in predicting atmospheric dispersion. The standard k–? and k–ω models and a Reynolds Stress Transport closure are employed and compared to predict the time-averaged turbulent flow field, while a standard gradient–diffusion model is initially adopted to relate the scalar flux to mean gradients of the concentration field. The analysis of two algebraic closures for turbulent scalar fluxes based on the generalized-gradient–diffusion hypothesis and its quadratic extension is also presented. In spite of the rather simple flow setup, where both the flow and the scalar fields can be assumed homogeneous in the spanwise direction, the analysis clarifies several critical issues concerning gradient-transport type models. We established the dominant role of predicted turbulent kinetic energy on scalar dispersion when a scalar diffusivity is employed, irrespectively of the Reynolds stress closure adopted for the averaged momentum equation. Moreover, the standard gradient–diffusion hypothesis failed to predict the streamwise component of the scalar flux, which is characterized by a counter-gradient-transport mechanism. Although the resulting contribution in the averaged scalar transport equation is small in the present flow configuration, this limitation can become severe for strongly inhomogeneous flows in the presence of point sources, where the spread of the scalar plume is essentially three-dimensional. The predictive capabilities of gradient-transport type modeling are found clearly improved using algebraic closures, which appear to represent a promising tool for predicting atmospheric dispersion in complex flows when unsteady transport mechanisms are not dominant.     

A simple network approach to modelling dispersion among large groups of obstacles

A simple network approach has been developed to simulate the movement of pollutant within urban areas. The model uses estimates of pollutant exchange obtained from velocity measurements in experiments with various regular obstacle arrays. The transfer of tracer material was modelled using concepts of advection along streets, well-mixed flow properties within street segments and exchange velocities (akin to aerodynamic conductances) across side and top facets of the street segments.The results predicted both the centreline concentration and lateral dispersion of the tracer with reasonable accuracy for a range of packing densities and wind directions. The basic model's concentration predictions were accurate to better than a factor of two in all cases for the region from two obstacle rows behind a source located within the array to around eight rows behind, a range of distances that falls into the so-called “neighbourhood-scale” for dispersion problems. The results supported the use of parameterized rates of exchange between regions of flow as being useful for fast, approximate dispersion modelling. It was thought that the effects of re-entrainment of tracer back into the canopy were of significance, but modelling designed to incorporate these effects did not lead to general improvements to the modelling for these steady-state source experiments.The model's limitations were also investigated. Chief amongst these was that it worked poorly among tall buildings where the well-mixed assumption within street segments was inadequate.     

Fluorescent dye imaging of the volume sampled by single well forced-gradient tracer tests evaluated in a laboratory-scale aquifer physical model

This study presents a new method to visualise forced-gradient tracer tests in 2-D using a laboratory-scale aquifer physical model. Experiments were designed to investigate the volume of aquifer sampled in vertical dipole flow tracer tests (DFTT) and push-pull tests (PPT), using a miniature monitoring well and straddle packer arrangement equipped with solute injection and recovery chambers. These tests have previously been used to estimate bulk aquifer hydraulic and transport properties for the evaluation of natural attenuation and other remediation approaches. Experiments were performed in a silica glass bead-filled box, using a fluorescent tracer (fluorescein) to deduce conservative solute transport paths. Digital images of fluorescein transport were captured under ultraviolet light and processed to analyse tracer plume geometry and obtain point-concentration breakthrough histories. Inorganic anion mixtures were also used to obtain conventional tracer breakthrough histories. Concentration data from the conservative tracer breakthrough curves was compared with the digital images and a well characterised numerical model. The results show that the peak tracer breakthrough response in dipole flow tracer tests samples a zone of aquifer close to the well screen, while the sampling volume of push-pull tests is limited by the length of the straddle packers used. The effective sampling volume of these single well forced-gradient tests in isotropic conditions can be estimated with simple equations. The experimental approach offers the opportunity to evaluate under controlled conditions the theoretical basis, design and performance of DFTTs and PPTs in porous media in relation to measured flow and transport properties.