Factors controlling BTEX and chlorinated solvents plume length under natural attenuation conditions

Natural attenuation is presently used at numerous sites where groundwater is contaminated. In order to simulate this attenuation, reactive transport models are often used but they are quite complex and depend on both physical and chemical conditions in the aquifer. As complex numerical models cannot be used to study all possible cases, we develop here analytical solutions to draw general conclusions. Our strategy, called MIKSS (Mixed Instantaneous and Kinetics Superposition Sequence), allows the calculation of the concentrations of all reacting substances in a plume. It is an extension of the superimposition principle that is able to treat the case of joint kinetics and instantaneous reactions. The basic equations have been extended to treat different reactions that occur in the plume core and at its fringe. At first we consider one organic substance degraded under all oxidising conditions (toluene for instance). For this problem the size of the plume depends on the reduced source width and on the ratio of the organic substance concentration to the sum of the electron acceptors' concentrations. For several BTEX substances having different degradation behaviour the formulation is similar, but leads to quite different plume lengths for each substance. Contrary to the case of one substance, the plumes can be quite long and may not satisfy the target risk level. For chlorinated solvents we developed a specific approach to take under consideration all reactions and particularly the competition for hydrogen. A formula is given to assess the size of the plume core, i.e. the zone with highly reducing conditions. The factors influencing the core length are the same as for BTEX (source width, dispersivity, organic carbon content). The size of the TCE plume is calculated from the plume core length and the kinetic constant of TCE degradation. Using assumptions of degradation constants for DCE and VC it is also possible to calculate the longitudinal concentration profile of these substances. The degradation of moderately substituted solvents under oxic conditions reduces the size of their plumes but under these conditions TCE becomes the major threat. Among the conditions studied in this paper, very few chlorinated solvents sites can lead to a negligible risk at an acceptable distance from the source.     

The Odor Impact Model

Abstract

This paper presents the simulation and field evaluation results of two approaches to localize pollutant emission sources with open-path Fourier transform infrared (OPFTIR) spectroscopy. The first approach combined the plume’s peak location information reconstructed from the Smooth Basis Function Minimization (SBFM) algorithm and the wind direction data to calculate source projection lines. In the second approach, the plume’s peak location was determined with the Monte Carlo methodology by randomly sampling within the beam segment having the largest path-integrated concentration. We first conducted a series of simulation studies to investigate the sensitivity of using different basis functions in the SBFM algorithm. It was found that fitting with the beta and Weibull basis functions generally gave better estimates of the peak locations than with the normal basis function when the plumes were mainly within the OP-FTIR’s monitoring line. However, for plumes that were symmetric to the peak position or spread over the OP-FTIR, fitting with the normal basis function gave better performance. In the field experiment, two tracer gases were released simultaneously from two locations and the OP-FTIR collected data downwind from the sources with a maximum beam path length of 97 m. For the first approach, the release locations were within the 0.25- to 0.5-probability area only after the uncertainty of the peak locations was included in the calculation process. The second approach was easy to implement and still performed as satisfactorily as the first approach. The distances from the sources to the best-fit lines (i.e., the regression lines) of the estimated locations were smaller than 10 m.     

Monitoring groundwater contamination and delineating source zones at industrial sites: uncertainty analyses using integral pumping tests

Field-scale characterisations of contaminant plumes in groundwater, as well as source zone delineations, are associated with uncertainties that can be considerable. A major source of uncertainty in environmental datasets is due to variability of sampling results, as a direct consequence of the heterogeneity of environmental matrices. We develop a methodology for quantifying uncertainties in field-scale mass flow and average concentration estimations, using integral pumping tests (IPTs), where the contaminant concentration is measured as a function of time in a pumping well. This procedure increases the sampling volume and reduces the effect of small-scale variability that may bias point-scale measurements. In particular, using IPTs, the interpolation uncertainty of conventional point-scale measurements is transformed to a quantifiable uncertainty related to the (unknown) plume position relative to the pumping well. We show that this plume position uncertainty generally influenced the predicted mass flows and average concentrations (of acenapthene, benzene and CHCs) to a greater extent than a boundary condition uncertainty related to the local water balance, considering 19 control planes at a highly heterogeneous industrial site in southwest Germany. Furthermore, large (order of magnitude) uncertainties only occurred if the conditions were strongly heterogeneous in the nearest vicinity of the well. We also develop a consistent methodology for an assessment of the combined effect of uncertainty in hydraulic conditions and uncertainty in reactive transport parameters for delimiting of both contaminant source zones and zones absent of source, based on (downgradient) IPTs.     

On the translation of uncertainty from toxicokinetic to toxicodynamic models--the TCDD example

When estimating human health risks from exposure to TCDD using toxicokinetic and toxicodynamic models, it is important to understand how model choice and assumptions necessary for modeling add to the uncertainty of risk estimates. Several toxicokinetic models have been proposed for the risk assessment of dioxins, in particular the elimination kinetics in humans has been a matter of constant debate. For a long time, a simple linear elimination kinetics has been common choice. Thus, it was used for the statistical analysis of the largest occupationally exposed cohort, the German Boehringer cohort. We challenge this assumption by considering, amongst others, a nonlinear modified Michaelis-Menten-type elimination kinetics, the so-called Carrier kinetics. Using the area under the lipid TCDD concentration time curve as dose metrics, we model the time to cancer-related death using the Cox proportional hazards model as toxicodynamic model. This risk assessment set-up was simulated in order to quantify uncertainty of both the dose (TCDD body burden) and the risk estimates, depending on the use of the kinetic model, variations of carcinogenic effect of TCDD and variations of latency period (lag time). If past exposure is estimated assuming a linear elimination kinetics although a Carrier kinetics actually holds, then high exposures in reality will be underestimated through statistical analysis and low exposures will be overestimated, respectively. This bias will carry over on the estimated individual concentration-time curves and the therefrom derived TCDD dose metric values. Using biased dose values when estimating a dose-response relationship will finally lead to biased risk estimates. The extent of bias and the decrease of precision are quantified in selected scenarios through this simulation approach. Our findings are in concordance with recent results in the field of dioxin risk assessment. They also reinforce the general demand for the scheduled uncertainty assessments in risk analyses.     

Numerical experiments and field results on the size of steady state plumes

Contaminated groundwater poses a serious risk for drinking water supplies. Under certain conditions, however, groundwater contamination remains restricted to a tolerable extent because of natural attenuation processes. We present an innovative approach to evaluate the size of these so-called steady-state plumes by 2-D and 1-D modelling in homogeneous aquifers. If longitudinal mixing is negligible, scenarios can be modelled in a simplified way using a 1-D domain vertical to the direction of flow. We analysed the sensitivity of the plume length with respect to biodegradation kinetics, flow velocity, transverse vertical dispersivity alphat, the source and aquifer geometry and reaction stoichiometry. Our findings indicate that for many readily biodegradable compounds transverse-dispersive mixing rather than reaction kinetics is the limiting factor for natural attenuation. Therefore, if alphat, aquifer and source geometry and concentrations of electron acceptors and donors are known, the length of the steady state contaminant plume can be predicted. The approach is validated under field conditions for an ammonium plume at a former landfill site in SW Germany.     

Assessing the natural attenuation of organic contaminants in aquifers using plume-scale electron and carbon balances: model development with analysis of uncertainty and parameter sensitivity

A quantitative methodology is described for the field-scale performance assessment of natural attenuation using plume-scale electron and carbon balances. This provides a practical framework for the calculation of global mass balances for contaminant plumes, using mass inputs from the plume source, background groundwater and plume residuals in a simplified box model. Biodegradation processes and reactions included in the analysis are identified from electron acceptors, electron donors and degradation products present in these inputs. Parameter values used in the model are obtained from data acquired during typical site investigation and groundwater monitoring studies for natural attenuation schemes. The approach is evaluated for a UK Permo-Triassic Sandstone aquifer contaminated with a plume of phenolic compounds. Uncertainty in the model predictions and sensitivity to parameter values was assessed by probabilistic modelling using Monte Carlo methods. Sensitivity analyses were compared for different input parameter probability distributions and a base case using fixed parameter values, using an identical conceptual model and data set. Results show that consumption of oxidants by biodegradation is approximately balanced by the production of CH4 and total dissolved inorganic carbon (TDIC) which is conserved in the plume. Under this condition, either the plume electron or carbon balance can be used to determine contaminant mass loss, which is equivalent to only 4% of the estimated source term. This corresponds to a first order, plume-averaged, half-life of > 800 years. The electron balance is particularly sensitive to uncertainty in the source term and dispersive inputs. Reliable historical information on contaminant spillages and detailed site investigation are necessary to accurately characterise the source term. The dispersive influx is sensitive to variability in the plume mixing zone width. Consumption of aqueous oxidants greatly exceeds that of mineral oxidants in the plume, but electron acceptor supply is insufficient to meet the electron donor demand and the plume will grow. The aquifer potential for degradation of these contaminants is limited by high contaminant concentrations and the supply of bioavailable electron acceptors. Natural attenuation will increase only after increased transport and dilution.     

Mixing-controlled biodegradation in a toluene plume--results from two-dimensional laboratory experiments

Various abiotic and biotic processes such as sorption, dilution, and degradation are known to affect the fate of organic contaminants, such as petroleum hydrocarbons in saturated porous media. Reactive transport modeling of such plumes indicates that the biodegradation of organic pollutants is, in many cases, controlled by mixing and therefore occurs locally at the plume's fringes, where electron donors and electron-acceptors mix. Herein, we aim to test whether this hypothesis can be verified by experimental results obtained from aerobic and anaerobic degradation experiments in two-dimensional sediment microcosms. Toluene was selected as a model compound for oxidizable contaminants. The two-dimensional microcosm was filled with quartz sand and operated under controlled flow conditions simulating a contaminant plume in otherwise uncontaminated groundwater. Aerobic degradation of toluene by Pseudomonas putida mt-2 reduced a continuous 8.7 mg L(-1) toluene concentration by 35% over a transport distance of 78 cm in 15.5 h. In comparison, under similar conditions Aromatoleum aromaticum strain EbN1 degraded 98% of the toluene infiltrated using nitrate (68.5+/-6.2 mg L(-1)) as electron acceptor. A major part of the biodegradation activity was located at the plume fringes and the slope of the electron-acceptor gradient was steeper during periods of active biodegradation. The distribution of toluene and the significant overlap of nitrate at the plume's fringe indicate that biokinetic and/or microscale transport processes may constitute additional limiting factors. Experimental data is corroborated with results from a reactive transport model using double Monod kinetics. The outcome of the study shows that in order to simulate degradation in contaminant plumes, detailed data sets are required to test the applicability of models. These will have to deal with the incorporation of existing parameters coding for substrate conversion kinetics and microbial growth.     

Factors influencing ozone chemistry in subsonic aircraft plumes

This study investigates several factors that could influence ozone chemistry occurring in subsonic aircraft plumes in the upper troposphere. The study focuses on uncertainties in gas-phase rate parameters, but also examines the influence of selected heterogeneous reactions, the rate of expansion of the plume, ambient and initial plume concentrations, and the time of emissions. Monte Carlo analysis with Latin hypercube sampling was applied to an expanding box model of an aircraft plume, in order to estimate the sensitivities of O₃ perturbations (ΔO₃) to uncertainties in rate constants in the RADM2 chemical mechanism. The resulting coefficient of variation in ΔO₃ at the end of a 36 h simulation was about 50%. Influential uncertainties in gas-phase rate parameters include those for photolysis of NO₂ and HCHO, O₃+NO, HO₂+NO, and formation of PAN and HNO₃. With high background concentrations of non-methane hydrocarbons, uncertainties in rate parameters of reactions involving peroxy radicals from ethene and propene oxidation were also influential. The coefficient of variation for ΔO₃ due to uncertainties in emission indices of NO_x, CO, and organic compounds was less than 15%. The effects of the heterogeneous reaction of N₂O₅ leading to HNO₃ formation, and hypothesized reactions of HNO₃ and NO₂ on soot, were also investigated. The results suggest that the latter two reactions could be influential for ΔO₃ if published estimates of reaction probabilities and high estimates of soot concentrations in plumes are realistic.     

Prediction of cloud effects in chimney plumes

A numerical model to predict the occurrence of visible condensation and cloud length in chimney plumes is tested against observations of the plume from a 500 MW natural gas-fired power station at Melbourne, Australia. The model employs two entrainment parameters selected from the literature on plume trajectories and not fitted to the observations reported here. A criterion for a plume to be visible is developed for droplets around 5 μm radius and plume distribution of condensed water determined from Gaussian two-dimensionalization of temperature and total water. The model correctly discriminates between cloudy and non-cloudy chimney plumes, between occasions of persistent cloud that extends into the far-field and when cloud terminates in the coherent-plume-phase and reliably forecasts cloud length in this latter case. The results emphasize that good meteorological data are required for accurate predictions.     

Natural attenuation of chlorinated ethene compounds: model development and field-scale application at the Dover site

A multi-dimensional and multi-species reactive transport model was developed to aid in the analysis of natural attenuation design at chlorinated solvent sites. The model can simulate several simultaneously occurring attenuation processes including aerobic and anaerobic biological degradation processes. The developed model was applied to analyze field-scale transport and biodegradation processes occurring at the Area-6 site in Dover Air Force Base, Delaware. The model was calibrated to field data collected at this site. The calibrated model reproduced the general groundwater flow patterns, and also, it successfully recreated the observed distribution of tetrachloroethene (PCE), trichloroethene (TCE), dichloroethylene (DCE), vinyl chloride (VC) and chloride plumes. Field-scale decay rates of these contaminant plumes were also estimated. The decay rates are within the range of values that were previously estimated based on lab-scale microcosm and field-scale transect analyses. Model simulation results indicated that the anaerobic degradation rate of TCE, source loading rate, and groundwater transport rate are the important model parameters. Sensitivity analysis of the model indicated that the shape and extent of the predicted TCE plume is most sensitive to transmissivity values. The total mass of the predicted TCE plume is most sensitive to TCE anaerobic degradation rates. The numerical model developed in this study is a useful engineering tool for integrating field-scale natural attenuation data within a rational modeling framework. The model results can be used for quantifying the relative importance of various simultaneously occurring natural attenuation processes.     

DNAPL distribution in the source zone: effect of soil structure and uncertainty reduction with increased sampling density

This paper focuses on parameters describing the distribution of dense nonaqueous phase liquid (DNAPL) contaminants and investigates the variability of these parameters that results from soil heterogeneity. In addition, it quantifies the uncertainty reduction that can be achieved with increased density of soil sampling. Numerical simulations of DNAPL releases were performed using stochastic realizations of hydraulic conductivity fields generated with the same geostatistical parameters and conditioning data at two sampling densities, thus generating two simulation ensembles of low and high density (three-fold increase) of soil sampling. The results showed that DNAPL plumes in aquifers identical in a statistical sense exhibit qualitatively different patterns, ranging from compact to finger-like. The corresponding quantitative differences were expressed by defining several alternative measures that describe the DNAPL plume and computing these measures for each simulation of the two ensembles. The uncertainty in the plume features under study was affected to different degrees by the variability of the soil, with coefficients of variation ranging from about 20% to 90%, for the low-density sampling. Meanwhile, the increased soil sampling frequency resulted in reductions of uncertainty varying from 7% to 69%, for low- and high-uncertainty variables, respectively. In view of the varying uncertainty in the characteristics of a DNAPL plume, remedial designs that require estimates of the less uncertain features of the plume may be preferred over others that need a more detailed characterization of the source zone architecture.     

Inverse modeling to estimate LNAPL plume release timing

Methodologies are presented for dating releases of light nonaqueous phase liquids (LNAPLs) using an inverse modeling approach with simple analytical models. Models for LNAPL plume migration are presented to predict LNAPL plume velocity in the unsaturated and saturated zones as a function of basic soil and fluid properties. A relative mobility factor is introduced for LNAPL movement at the water table that depends primarily on the van Genuchten n parameter (related to the breadth of the soil pore size distribution) and the magnitude of water table fluctuations. Estimated LNAPL plume velocities compare reasonably with more rigorous numerical models, which may be used in cases where data availability warrant the greater effort entailed.Two methods of estimating release timing and its uncertainty are investigated. A direct estimation method is described that determines travel time for a single observed travel distance based on estimated soil and fluid properties. Release date uncertainty may be determined using the first order (FO) or Monte Carlo (MC) methods. The second method for estimating release date involves nonlinear parameter estimation utilizing distance vs. time measurements and other data.A case study is presented for a field site where independent estimates of release timing were obtained from a numerical modeling analysis. Release timing estimates based on direct inversion of the analytical timing model agree well with the numerical analysis. Results for a second field site indicate that release date confidence limits estimated by the FO method, assuming log-normally distributed travel times, are close to values determined by the MC method, which makes no assumption regarding the form of the travel time probability distribution.Results for a hypothetical problem indicate that LNAPL velocity and travel time may be accurately estimated if sufficient data on travel distance vs. time are available. Incorporating prior information on relevant soil and fluid properties into the objective function reduces the uncertainty in release date if prior estimates are accurate. However, biased prior estimates may lead to over- or underestimation of release date uncertainty. Simultaneous estimation of soil and fluid properties and release date is possible if prior information is available to condition the parameter estimates.     

Choice of dispersion coefficients in reactive transport calculations on smoothed fields

Local dispersion dominates the mixing of compounds that are introduced separately into the subsurface and do not partition into any other than the aqueous phase. Thus, reactions between these compounds are controlled by dispersive mixing if they are not limited by kinetics. I quantify longitudinal dispersive mixing by the longitudinal effective dispersion coefficient of a conservative tracer introduced by a point-like injection [Water Resour. Res. 36 (12) (2000) 3591-3604]. In the upscaling of mixing-controlled reactive transport, I apply the mean velocity and the effective dispersion coefficient to the macroscopic transport calculations, whereas the reactive parameters on the macro-scale are identical to those on the local scale. The applicability of the approach is demonstrated for the transport of compounds undergoing a second-order irreversible bimolecular reaction. Ten realizations of a two-dimensional heterogeneous log-conductivity field are considered. Using the effective dispersion parameters, the overall mass balance is met in the ensemble average, whereas solute spreading is underestimated. I assess the lack of spreading by the difference between the expected macrodispersion and effective dispersion coefficients. I extend the approach to simulations on log-conductivity fields obtained by kriging of regularly spaced conductivity measurements. These fields contain the large-scale features of the true fields but do not resolve the small-scale variability. For the calculations on the kriged fields, the corresponding conditional covariance is substituted into the analytical expressions of effective dispersion, yielding a correction effective dispersion coefficient. The comparison between simulations on the fully resolved fields and on the kriged fields indicates that the approach is valid for wide plumes meeting the ergodicity condition. The high variability of mixing on small scales unresolved by kriging, however, leads to severe uncertainty when mixing-controlled reactions are predicted for narrow plumes.     

Rates of conversion of sulfur dioxide to sulfate in a scrubbed power plant plume.

The rate of conversion of SO2 to SO4(2-) was re-estimated from measurements made in the plume of the Cumberland power plant, located on the Cumberland River in north-central Tennessee, after installation of flue gas desulfurization (FGD) scrubbers for SO2 removal in 1994. The ratio of SO2 to NOy emissions into the plume has been reduced to approximately 0.1, compared with a prescrubber value of approximately 2. To determine whether the SO2 emissions reduction has correspondingly reduced plume-generated particulate SO4(2-) production, we have compared the rates of conversion before and after scrubber installation. The prescrubber estimates were developed from measurements made during the Tennessee Plume Study conducted in the late 1970s. The postscrubber estimates are based upon two series of research flights in the summers of 1998 and 1999. During two of these flights, the Cumberland plume did not mix with adjacent power plant plumes, enabling rate constants for conversion to be estimated from samples taken in the plume at three downwind distances. Dry deposition losses and the fact the fact that SO2 is no longer in large excess compared with SO4(2-) have been taken into account, and an upper limit for the conversion rate constant was re-estimated based on plume excess aerosol volume. The estimated upper limit values are 0.069 hr(-1) and 0.034 hr(-1) for the 1998 and 1999 data, respectively. The 1999 rate is comparable with earlier values for nonscrubbed plumes, and although the 1998 upper limit value is higher than expected, these estimates do not provide strong evidence for deviation from a linear relationship between SO2 emissions and SO4(2-) formation.     

An investigation of the environmental impact of an artificial thermal plume

Experimental analysis of the mean and turbulent structures of artificial thermal plumes rising in the boundary layer up into the capping stable layers is reported. Scaling parameters are used to compare the structural aspects obtained from ten experimental cases. Vertical profiles of the mean excesses (temperature and vertical velocity) and of the dissipative parameters (dissipation rate and temperature structure parameter) within the plume are given. The estimates of dissipation rate and of the horizontal width of the column are used to predict the variation of the vertical eddy diffusivity coefficient from the heat source to the top level of the plume.     

Influence of temporally variable groundwater flow conditions on point measurements and contaminant mass flux estimations

Monitoring of contaminant concentrations, e.g., for the estimation of mass discharge or contaminant degradation rates, often is based on point measurements at observation wells. In addition to the problem, that point measurements may not be spatially representative, a further complication may arise due to the temporal dynamics of groundwater flow, which may cause a concentration measurement to be not temporally representative. This paper presents results from a numerical modeling study focusing on temporal variations of the groundwater flow direction. “Measurements” are obtained from point information representing observation wells installed along control planes using different well frequencies and configurations. Results of the scenario simulations show that temporally variable flow conditions can lead to significant temporal fluctuations of the concentration and thus are a substantial source of uncertainty for point measurements. Temporal variation of point concentration measurements may be as high as the average concentration determined, especially near the plume fringe, even when assuming a homogeneous distribution of the hydraulic conductivity. If a heterogeneous hydraulic conductivity field is present, the concentration variability due to a fluctuating groundwater flow direction varies significantly within the control plane and between the different realizations. Determination of contaminant mass fluxes is also influenced by the temporal variability of the concentration measurement, especially for large spacings of the observation wells. Passive dosimeter sampling is found to be appropriate for evaluating the stationarity of contaminant plumes as well as for estimating average concentrations over time when the plume has fully developed. Representative sampling has to be performed over several periods of groundwater flow fluctuation. For the determination of mass fluxes at heterogeneous sites, however, local fluxes, which may vary considerably along a control plane, have to be accounted for. Here, dosimeter sampling in combination with time integrated local water flux measurements can improve mass flux estimates under dynamic flow conditions.     

Developing and evaluating techniques for localizing pollutant emission sources with open-path Fourier transform infrared measurements and wind data

This paper presents the simulation and field evaluation results of two approaches to localize pollutant emission sources with open-path Fourier transform infrared (OP-FTIR) spectroscopy. The first approach combined the plume's peak location information reconstructed from the Smooth Basis Function Minimization (SBFM) algorithm and the wind direction data to calculate source projection lines. In the second approach, the plume's peak location was determined with the Monte Carlo methodology by randomly sampling within the beam segment having the largest path-integrated concentration. We first conducted a series of simulation studies to investigate the sensitivity of using different basis functions in the SBFM algorithm. It was found that fitting with the beta and Weibull basis functions generally gave better estimates of the peak locations than with the normal basis function when the plumes were mainly within the OP-FTIR's monitoring line. However, for plumes that were symmetric to the peak position or spread over the OP-FTIR, fitting with the normal basis function gave better performance. In the field experiment, two tracer gases were released simultaneously from two locations and the OP-FTIR collected data downwind from the sources with a maximum beam path length of 97 m. For the first approach, the release locations were within the 0.25- to 0.5-probability area only after the uncertainty of the peak locations was included in the calculation process. The second approach was easy to implement and still performed as satisfactorily as the first approach. The distances from the sources to the best-fit lines (i.e., the regression lines) of the estimated locations were smaller than 10 m.     

Impact of transverse and longitudinal dispersion on first-order degradation rate constant estimation

A two-dimensional analytical model is employed for estimating the first-order degradation rate constant of hydrophobic organic compounds (HOCs) in contaminated groundwater under steady-state conditions. The model may utilize all aqueous concentration data collected downgradient of a source area, but does not require that any data be collected along the plume centerline. Using a least squares fit of the model to aqueous concentrations measured in monitoring wells, degradation rate constants were estimated at a former manufactured gas plant (FMGP) site in the Midwest U.S. The estimated degradation rate constants are 0.0014, 0.0034, 0.0031, 0.0019, and 0.0053 day(-1) for acenaphthene, naphthalene, benzene, ethylbenzene, and toluene, respectively. These estimated rate constants were as low as one-half those estimated with the one-dimensional (centerline) approach of Buscheck and Alcantar [Buscheck, T.E., Alcantar, C.M., 1995. Regression techniques and analytical solutions to demonstrate intrinsic bioremediation. In: Hinchee, R.E., Wilson, J.T., Downey, D.C. (Eds.), Intrinsic Bioremediation, Battelle Press, Columbus, OH, pp. 109-116] which does not account for transverse dispersivity. Varying the transverse and longitudinal dispersivity values over one order of magnitude for toluene data obtained from the FMGP site resulted in nearly a threefold variation in the estimated degradation rate constant-highlighting the importance of reliable estimates of the dispersion coefficients for obtaining reasonable estimates of the degradation rate constants. These results have significant implications for decision making and site management where overestimation of a degradation rate may result in remediation times and bioconversion factors that exceed expectations. For a complex source area or non-steady-state plume, a superposition of analytical models that incorporate longitudinal and transverse dispersion and time may be used at sites where the centerline method would not be applicable.     

A Theory of Plume Rise Compared with Field Observations

A theory for the rise of a plume in a horizontal wind is proposed in which it is assumed that, for some distance downwind of a high stack, the effects of atmospheric turbulence may be ignored in comparison with the effects of turbulence generated by the plume. The theory, an extension of the local similarity ideas used by Morton, Taylor, and Turner,¹ has two empirical parameters which measure the rate that surrounding fluid is entrained into the plume. Laboratory measurements of buoyant plume motion in laminar unstratified cross flow are used to estimate the empirical parameters. Using this determination of the parameters in the theory, the trajectories of atmospheric plumes may be predicted. To make such a prediction, the observed wind velocity and temperature as functions of altitude, and flow conditions at the stack orifice, are used in numerically integrating the equations. The resulting trajectories are compared with photographs, made by Leavitt, et al.,² of TVA, of plumes from 500 to 600 ft high stacks. Within 10 stack heights downwind of the stack, the root mean square discrepancy between the observed height of the trajectory above ground level and the theoretical value is 14%, which is about the uncertainty in the observed height. The maximum plume rise within the field of observation is within 15% of that predicted by the present theory.     

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).