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1.
Both forward and backward transport modeling methods are being developed for characterization of sources in atmospheric releases of toxic agents. Forward modeling methods, which describe the atmospheric transport from sources to receptors, use forward-running transport and dispersion models or computational fluid dynamics models which are run many times, and the resulting dispersion field is compared to observations from multiple sensors. Forward modeling methods include Bayesian updating and inference schemes using stochastic Monte Carlo or Markov Chain Monte Carlo sampling techniques. Backward or inverse modeling methods use only one model run in the reverse direction from the receptors to estimate the upwind sources. Inverse modeling methods include adjoint and tangent linear models, Kalman filters, and variational data assimilation, among others.This survey paper discusses these source estimation methods and lists the key references. The need for assessing uncertainties in the characterization of sources using atmospheric transport and dispersion models is emphasized.  相似文献   

2.
Sorption equilibria and rates were characterized for a matrix of four aquifer sands and two slightly to moderately hydrophobic organic solutes (nitrobenzene and lindane), and the effects of sorption on the behavior of these solutes in saturated systems of the soils were determined. Experimental data were used to test and evaluate a variety of mathematical models for predicting contaminant fate and transport in groundwater systems.Observed equilibrium relationships between soil and solution phase solute concentrations were found to be described best by the nonlinear Freundlich isotherm model. It was further determined that the sorption process in the systems tested is rate controlled, requiring several days to approach equilibrium in completely mixed batch reactors. Subsequent modeling of solute transport in continuous flow soil column reactors was found to be most successful when rate-controlled models were used, the best results were obtained with a dual-resistance model incorporating the coupled mass transport steps of boundary-layer and intraparticle diffusion.  相似文献   

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Warren C  Mackay D  Whelan M  Fox K 《Chemosphere》2005,61(10):1458-1467
A novel and flexible approach is described for simulating the behaviour of chemicals in river basins. A number (n) of river reaches are defined and their connectivity is described by entries in an n x n matrix. Changes in segmentation can be readily accommodated by altering the matrix entries, without the need for model revision. Two models are described. The simpler QMX-R model only considers advection and an overall loss due to the combined processes of volatilization, net transfer to sediment and degradation. The rate constant for the overall loss is derived from fugacity calculations for a single segment system. The more rigorous QMX-F model performs fugacity calculations for each segment and explicitly includes the processes of advection, evaporation, water-sediment exchange and degradation in both water and sediment. In this way chemical exposure in all compartments (including equilibrium concentrations in biota) can be estimated. Both models are designed to serve as intermediate-complexity exposure assessment tools for river basins with relatively low data requirements. By considering the spatially explicit nature of emission sources and the changes in concentration which occur with transport in the channel system, the approach offers significant advantages over simple one-segment simulations while being more readily applicable than more sophisticated, highly segmented, GIS-based models.  相似文献   

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In this paper the meteorological processes responsible for transporting tracer during the second ETEX (European Tracer EXperiment) release are determined using the UK Met Office Unified Model (UM). The UM predicted distribution of tracer is also compared with observations from the ETEX campaign. The dominant meteorological process is a warm conveyor belt which transports large amounts of tracer away from the surface up to a height of 4 km over a 36 h period. Convection is also an important process, transporting tracer to heights of up to 8 km. Potential sources of error when using an operational numerical weather prediction model to forecast air quality are also investigated. These potential sources of error include model dynamics, model resolution and model physics. In the UM a semi-Lagrangian monotonic advection scheme is used with cubic polynomial interpolation. This can predict unrealistic negative values of tracer which are subsequently set to zero, and hence results in an overprediction of tracer concentrations. In order to conserve mass in the UM tracer simulations it was necessary to include a flux corrected transport method. Model resolution can also affect the accuracy of predicted tracer distributions. Low resolution simulations (50 km grid length) were unable to resolve a change in wind direction observed during ETEX 2, this led to an error in the transport direction and hence an error in tracer distribution. High resolution simulations (12 km grid length) captured the change in wind direction and hence produced a tracer distribution that compared better with the observations. The representation of convective mixing was found to have a large effect on the vertical transport of tracer. Turning off the convective mixing parameterisation in the UM significantly reduced the vertical transport of tracer. Finally, air quality forecasts were found to be sensitive to the timing of synoptic scale features. Errors in the position of the cold front relative to the tracer release location of only 1 h resulted in changes in the predicted tracer concentrations that were of the same order of magnitude as the absolute tracer concentrations.  相似文献   

7.
Quantification of the relationship between dense nonaqueous phase liquid (DNAPL) source strength, source longevity and spatial distribution is increasingly recognized as important for effective remedial design. Partitioning tracers are one tool that may permit interrogation of DNAPL architecture. Tracer data are commonly analyzed under the assumption of linear, equilibrium partitioning, although the appropriateness of these assumptions has not been fully explored. Here we focus on elucidating the nonlinear and nonequilibrium partitioning behavior of three selected alcohol tracers - 1-pentanol, 1-hexanol and 2-octanol in a series of batch and column experiments. Liquid-liquid equilibria for systems comprising water, TCE and the selected alcohol illustrate the nonlinear distribution of alcohol between the aqueous and organic phases. Complete quantification of these equilibria facilitates delineation of the limits of applicability of the linear partitioning assumption, and assessment of potential inaccuracies associated with measurement of partition coefficients at a single concentration. Column experiments were conducted under conditions of non-equilibrium to evaluate the kinetics of the reversible absorption of the selected tracers in a sandy medium containing a uniform entrapped saturation of TCE-DNAPL. Experimental tracer breakthrough data were used, in conjunction with mathematical models and batch measurements, to evaluate alternative hypotheses for observed deviations from linear equilibrium partitioning behavior. Analyses suggest that, although all tracers accumulate at the TCE-DNAPL/aqueous interface, surface accumulation does not influence transport at concentrations typically employed for tracer tests. Moreover, results reveal that the kinetics of the reversible absorption process are well described using existing mass transfer correlations originally developed to model aqueous boundary layer resistance for pure-component NAPL dissolution.  相似文献   

8.
Air quality models are typically used to predict the fate and transport of air emissions from industrial sources to comply with federal and state regulatory requirements and environmental standards, as well as to determine pollution control requirements. For many years, the U.S. Environmental Protection Agency (EPA) widely used the Industrial Source Complex (ISC) model because of its broad applicability to multiple source types. Recently, EPA adopted a new rule that replaces ISC with AERMOD, a state-of-the-practice air dispersion model, in many air quality impact assessments. This study compared the two models as well as their enhanced versions that incorporate the Plume Rise Model Enhancements (PRIME) algorithm. PRIME takes into account the effects of building downwash on plume dispersion. The comparison used actual point, area, and volume sources located on two separate facilities in conjunction with site-specific terrain and meteorological data. The modeled maximum total period average ground-level air concentrations were used to calculate potential health effects for human receptors. The results show that the switch from ISC to AERMOD and the incorporation of the PRIME algorithm tend to generate lower concentration estimates at the point of maximum ground-level concentration. However, the magnitude of difference varies from insignificant to significant depending on the types of the sources and the site-specific conditions. The differences in human health effects, predicted using results from the two models, mirror the concentrations predicted by the models.  相似文献   

9.
Aquifer heterogeneity (structure) and NAPL distribution (architecture) are described based on tracer data. An inverse modelling approach that estimates the hydraulic structure and NAPL architecture based on a Lagrangian stochastic model where the hydraulic structure is described by one or more populations of lognormally distributed travel times and the NAPL architecture is selected from eight possible assumed distributions. Optimization of the model parameters for each tested realization is based on the minimization of the sum of the square residuals between the log of measured tracer data and model predictions for the same temporal observation. For a given NAPL architecture the error is reduced with each added population. Model selection was based on a fitness which penalized models for increasing complexity. The technique is demonstrated under a range of hydrologic and contaminant settings using data from three small field-scale tracer tests: the first implementation at an LNAPL site using a line-drive flow pattern, the second at a DNAPL site with an inverted five-spot flow pattern, and the third at the same DNAPL site using a vertical circulation flow pattern. The Lagrangian model was capable of accurately duplicating experimentally derived tracer breakthrough curves, with a correlation coefficient of 0.97 or better. Furthermore, the model estimate of the NAPL volume is similar to the estimates based on moment analysis of field data.  相似文献   

10.
A large database including temporal trends of physical, ecological and socio-economic data was developed within the EUROCAT project. The aim was to estimate the nutrient fluxes for different socio-economic scenarios at catchment and coastal zone level of the Po catchment (Northern Italy) with reference to the Water Quality Objectives reported in the Water Framework Directive (WFD 2000/60/CE) and also in Italian legislation. Emission data derived from different sources at national, regional and local levels are referred to point and non-point sources. While non-point (diffuse) sources are simply integrated into the nutrient flux model, point sources are irregularly distributed. Intensive farming activity in the Po valley is one of the main Pressure factors Driving groundwater pollution in the catchment, therefore understanding the spatial variability of groundwater nitrate concentrations is a critical issue to be considered in developing a Water Quality Management Plan. In order to use the scattered point source data as input in our biogeochemical and transport models, it was necessary to predict their values and associated uncertainty at unsampled locations. This study reports the spatial distribution and uncertainty of groundwater nitrate concentration at a test site of the Po watershed using a probabilistic approach. Our approach was based on geostatistical sequential Gaussian simulation used to yield a series of stochastic images characterized by equally probable spatial distributions of the nitrate concentration across the area. Post-processing of many simulations allowed the mapping of contaminated and uncontaminated areas and provided a model for the uncertainty in the spatial distribution of nitrate concentrations.  相似文献   

11.
Aquifer heterogeneity (structure) and NAPL distribution (architecture) are described based on tracer data. An inverse modelling approach that estimates the hydraulic structure and NAPL architecture based on a Lagrangian stochastic model where the hydraulic structure is described by one or more populations of lognormally distributed travel times and the NAPL architecture is selected from eight possible assumed distributions. Optimization of the model parameters for each tested realization is based on the minimization of the sum of the square residuals between the log of measured tracer data and model predictions for the same temporal observation. For a given NAPL architecture the error is reduced with each added population. Model selection was based on a fitness which penalized models for increasing complexity. The technique is demonstrated under a range of hydrologic and contaminant settings using data from three small field-scale tracer tests: the first implementation at an LNAPL site using a line-drive flow pattern, the second at a DNAPL site with an inverted five-spot flow pattern, and the third at the same DNAPL site using a vertical circulation flow pattern. The Lagrangian model was capable of accurately duplicating experimentally derived tracer breakthrough curves, with a correlation coefficient of 0.97 or better. Furthermore, the model estimate of the NAPL volume is similar to the estimates based on moment analysis of field data.  相似文献   

12.
When soil structure varies in different soil types and the horizons of these soil types, it has a significant impact on water flow and contaminant transport in soils. This paper focuses on the effect of soil structure variations on the transport of pesticides in the soil above the water table. Transport of a pesticide (chlorotoluron) initially applied on soil columns taken from various horizons of three different soil types (Haplic Luvisol, Greyic Phaeozem and Haplic Cambisol) was studied using two scenarios of ponding infiltration. The highest infiltration rate and pesticide mobility were observed for the Bt1 horizon of Haplic Luvisol that exhibited a well-developed prismatic structure. The lowest infiltration rate was measured for the Bw horizon of Haplic Cambisol, which had a poorly developed soil structure and a low fraction of large capillary pores and gravitational pores. Water infiltration rates were reduced during the experiments by a soil structure breakdown, swelling of clay and/or air entrapped in soil samples. The largest soil structure breakdown and infiltration decrease was observed for the Ap horizon of Haplic Luvisol due to the low aggregate stability of the initially well-aggregated soil. Single-porosity and dual-permeability (with matrix and macropore domains) flow models in HYDRUS-1D were used to estimate soil hydraulic parameters via numerical inversion using data from the first infiltration experiment. A fraction of the macropore domain in the dual-permeability model was estimated using the micro-morphological images. Final soil hydraulic parameters determined using the single-porosity and dual-permeability models were subsequently used to optimize solute transport parameters. To improve numerical inversion results, the two-site sorption model was also applied. Although structural changes observed during the experiment affected water flow and solute transport, the dual-permeability model together with the two-site sorption model proved to be able to approximate experimental data.  相似文献   

13.
A modeling system that includes a global chemical transport model (CTM) and a nested continental CTM (TEAM) was used to simulate the atmospheric transport, transformations and deposition of mercury (Hg). Three scenarios were used: (1) a nominal scenario, (2) a scenario conducive to local deposition and (3) a scenario conducive to long-range transport. Deposition fluxes of Hg were analyzed at three receptor locations in New York State. For the nominal scenario, the anthropogenic emission sources (including re-emission of deposited Hg) in New York State, the rest of the contiguous United States, Asia, Europe, and Canada contributed 11-1, 25-9, 13-19, 5-7, and 2-5%, respectively to total Hg deposition at these three receptors. Natural sources contributed 16-4%. The results from the local deposition and long-range transport scenarios varied only slightly from these results. However, there are still uncertainties in our understanding of the atmospheric chemistry of Hg that are likely to affect these estimates of local, regional and global contributions. Comparison of model simulation results with data from the Mercury Deposition Network suggests that local and regional contributions may currently be overestimated.  相似文献   

14.
Predictions of forest ecosystem response to changes in climate and atmospheric CO(2) concentration require hierarchically structured process models. Present forest simulation models have conceptual limitations that restrict their application to climate-change studies. A major drawback of forest succession models is that they often lack physiological details in the simulation of annual tree growth. On the other hand, aggregated ecosystem models assume spatially homogeneous forests, and do not account for successional changes in forest composition and canopy structure. The concept of a new coupled carbon-water-energy-forest vegetation model is presented which attempts to overcome the main limitations of existing models by implementing a modern view of ecological hierarchy and a robust approach for scaling ecological processes in space and time.  相似文献   

15.
Colloid-facilitated transport has been recognized as a potentially important and overlooked contaminant transport process. In particular, it has been observed that conventional two phase sorption models are often unable to explain transport of highly sorbing compounds in the subsurface appropriately in the presence of colloids. In this study a one-dimensional model for colloid-facilitated transport of chemicals in unsaturated porous media is developed. The model has parts for simulating coupled flow, and colloid transport and dissolved and colloidal contaminant transport. Richards' equation is solved to model unsaturated flow, and the effect of colloid entrapment and release on porosity and hydraulic conductivity of the porous media is incorporated into the model. Both random sequential adsorption and Langmuir approaches have been implemented in the model in order to incorporate the effect of surface jamming. The concept of entrapment of colloids into the air-water interface is used for taking into account the effect of retardation caused due to existence of the air phase. A non-equilibrium sorption approach with options of linear and Langmuir sorption assumptions are implemented that can represent the competition and site saturation effects on sorption of multiple compounds both to the solid matrix and to the colloidal particles. Several demonstration calculations are performed and the conditions in which the non-equilibrium model can be approximated by an equilibrium model are also studied.  相似文献   

16.
The Idaho National Engineering and Environmental Laboratory (INEEL) has implemented a phased approach to ecological risk assessment (ERA). The first step in this process is a screening-level ERA at each facility. Basic to this approach was the development of ecologically based screening levels (EBSLs), defined as concentrations of chemicals in soil (or other media) that are not expected to produce any adverse effects on selected ecological receptors under chronic exposure conditions (analogous to preliminary remediation goals or soil screening levels). EBSLs are calculated by rearrangement of standard exposure equations to solve for soil concentration when chemical intake rate is set at a developed toxicity reference value (TRV). A TRV is defined as a chronic dose that is likely to be without appreciable risk of deleterious effects. This definition was extended to define TRVs and ultimately EBSLs for the functional groups used in the INEEL screening-level ERAS.  相似文献   

17.
A source-resolved model has been developed to predict the contribution of different sources to primary organic aerosol concentrations. The model was applied to the eastern US during a 17 day pollution episode beginning on 12 July 2001. Primary organic matter (OM) and elemental carbon (EC) concentrations are tracked for eight different sources: gasoline vehicles, non-road diesel vehicles, on-road diesel vehicles, biomass burning, wood burning, natural gas combustion, road dust, and all other sources. Individual emission inventories are developed for each source and a three-dimensional chemical transport model (PMCAMx) is used to predict the primary OM and EC concentrations from each source. The source-resolved model is simple to implement and is faster than existing source-oriented models. The results of the source-resolved model are compared to the results of chemical mass balance models (CMB) for Pittsburgh and multiple urban/rural sites from the Southeastern Aerosol Research and Characterization (SEARCH) network. Significant discrepancies exist between the source-resolved model and the CMB model predictions for some of the sources. There is strong evidence that the organic PM emissions from natural gas combustion are overestimated. It also appears that the OM and EC emissions from wood burning and off-road diesel are too high in the Northeastern US. Other similarities and discrepancies between the source-resolved model and the CMB model for primary OM and EC are discussed along with problems in the current emission inventory for certain sources.  相似文献   

18.
Recent monitoring data indicate that portions of Italy's Venice Lagoon ecosystem have been degraded due to biological and chemical pollution from a variety of potential sources. Using polychlorinated dibenzo-p-dioxin (PCDD) and dibenzofuran (PCDF) data collected from sediment, fish and shellfish in the Lagoon, a screening-level ecological risk assessment (ERA) was performed to evaluate the risks to representative aquatic biota and wildlife receptors. Risks to aquatic invertebrates posed by PCDD/Fs in sediment were evaluated by comparing measured tissue concentrations in fish and shellfish to appropriate ecotoxicological reference values. For mammalian and avian receptors, risks posed by theoretical exposures to PCDD/Fs through the food chain were calculated using conservative wildlife exposure models. Results of the screening-level approach indicate that the potential for adverse effects to fish and aquatic invertebrate receptors from PCDD/Fs in surficial sediments are unlikely. Adverse effects to wildlife are possible but highly uncertain, and warrants further investigation in a more comprehensive ERA.  相似文献   

19.
The Spokane, Washington area is classified as a non-attainment area for the 24-h PM10 standard due to a history of high particulate matter concentrations. A Eulerian regional air quality model (CALMET/CALGRID) has been used to characterize the emission, transport and dispersion of PM10 and PM2.5 in Spokane. Observations from a residential site (Rockwood, RW) and an industrial site (Crown Zellerbach, CZ), spanning July 1994–August 1996 were used to evaluate the current emission inventory. Two major tasks were devised to conduct the objectives of this investigation. First, a simple and efficient urban dispersion model (WYNDValley) was used to simulate important episodes characterized by the highest PM10 and PM2.5 concentrations. The selected episodes included four days with wet conditions for which no roads would have been emitting and seven days with dry conditions for which roads would emit. In the second step, a single road-emitting event was selected from the previous predicted results for further analysis using the Eulerian regional air quality model to examine the emission inventory. The urban and regional models predicted the observed concentration distributions reasonably well for the source emissions inventoried in Spokane. The mass concentrations of PM10 were well predicted for the roads emitting case examined by both models indicating that the emission inventory based primarily upon area sources including roads is reasonably well characterized, at least at the RW site. The area sources around CZ are less well characterized, so that the PM10 concentrations are underpredicted at CZ. The models appear unable to reach an equilibrium mass balance status at the beginning of the simulation, and the urban model seems unable to properly resolve the nocturnal boundary layer.  相似文献   

20.
Sources of mercury contamination in aquatic systems were studied in a comprehensive literature review. The results show that the most important anthropogenic sources of mercury pollution in aquatic systems are: (1) atmospheric deposition, (2) erosion, (3) urban discharges, (4) agricultural materials, (5) mining, and (6) combustion and industrial discharges. Capping and dredging are two possible remedial approaches to mercury contamination in aquatic systems, and natural attenuation is a passive decontamination alternative. Capping seems to be an economical and effective remedial approach to mercury-contaminated aquatic systems. Dredging is an expensive remedial approach. However, for heavily polluted systems, dredging may be more effective. Natural attenuation, involving little or no cost, is a possible and very economical choice for less contaminated sites. Proper risk assessment is necessary to evaluate the effectiveness of remedial and passive decontamination methods as well as their potential adverse environmental effects. Modeling tools have a bright future in the remediation and passive decontamination of mercury contamination in aquatic systems. Existing mercury transport and transformation models were reviewed and compared.  相似文献   

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