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.     

Targeting of observations for accidental atmospheric release monitoring

In the event of an accidental atmospheric release of radionuclides from a nuclear power plant, accurate real-time forecasting of the activity concentrations of radionuclides is acutely required by the decision makers for the preparation of adequate countermeasures. Yet, the accuracy of the forecasted plume is highly dependent on the source term estimation. Inverse modelling and data assimilation techniques should help in that respect. However the plume can locally be thin and could avoid a significant part of the radiological monitoring network surrounding the plant. Deploying mobile measuring stations following the accident could help to improve the source term estimation. In this paper, a method is proposed for the sequential reconstruction of the plume, by coupling a sequential data assimilation algorithm based on inverse modelling with an observation targeting strategy. The targeting design strategy consists in seeking the optimal locations of the mobile monitors at time t + 1 based on all available observations up to time t.The performance of the sequential assimilation with and without targeting of observations has been assessed in a realistic framework. It focuses on the Bugey nuclear power plant (France) and its surroundings within 50 km from the plant. The existing surveillance network is used and realistic observational errors are assumed. The targeting scheme leads to a better estimation of the source term as well as the activity concentrations in the domain. The mobile stations tend to be deployed along plume contours, where activity concentration gradients are important. It is shown that the information carried by the targeted observations is very significant, as compared to the information content of fixed observations. A simple test on the impact of model error from meteorology shows that the targeting strategy is still very useful in a more uncertain context.     

Persistence of polycyclic aromatic hydrocarbons in sediments in the deeper area of the Northern Adriatic Sea (Mediterranean Sea)

The Po Valley is the most important agricultural and industrial area of Adriatic basin. In this area there are several rivers which transport polycyclic aromatic hydrocarbons (PAHs) into the sea via suspended particulate matter. This study describes the persistence of PAHs in the deep and coastal sediments of the Northern Adriatic. Different environmental conditions were studied: salinity, temperature, sunlight, sediment particle size and organic matter in sediment. The average conditions in the deep areas of the Northern Adriatic are: salinity higher than 37, temperature lower than 11 °C, darkness and clayey sediments with a high organic matter content. These conditions increase the persistence of the PAHs in the deep area of the Northern Adriatic.     

A fluctuating plume model for concentration fluctuations in a plant canopy

A one-particle Lagrangian model for continuous releases in the non-Gaussian inhomogeneous turbulence of a canopy layer is derived based on the fluctuating plume model of Franzese [2003. Lagrangian stochastic modeling of a fluctuating plume in the convective boundary layer. Atmos. Environ. 37, 1691–1701.]. The model equations are filtered by a time-dependent low-pass filter applied to the turbulent kinetic energy in order to obtain a fluctuating plume model able to simulate the vertical meandering of the cloud centroid through non-stationary Lagrangian equations. The model satisfies the well-mixed condition. The relative dispersion of particles and the concentration fluctuation statistics of a passive tracer inside a modeled vegetal canopy are studied. The probability density function of the concentration relative to the plume centroid is parameterized and the mean and variance fields of concentration are simulated and compared with wind-tunnel data and numerical simulations. A skewed, reflected probability density function for the vertical position of the plume centroid is considered.     

Simulation of the evolution of particle size distributions containing coarse particulate in the atmospheric surface layer with a simple convection-diffusion-sedimentation model

The Fugitive Dust Model (FDM) and Industrial Source Complex (ISC), widely used coarse particulate dispersion models, have been shown inaccurate due to the neglect of vertical variations in atmospheric wind speed and turbulent diffusivity (Vesovic et al., 2001), omission of the gravitational advection velocity, and an underestimation of the ground deposition velocity (Kim and Larson, 2001). A simple, transient two-dimensional convection-diffusion-sedimentation model is proposed to simulate the evolution in particle size distribution of an aerosol ‘puff’ containing coarse particulate in the atmospheric surface layer. Monin-Okhubov similarity theory, accompanied by empirical observations made by Businger et al. (1971), is adopted to characterize the surface layer wind speed and turbulent diffusivity profiles over a wide range of atmospheric conditions. A first order analysis of the crossing trajectories effect suggests simulation data presented here are not significantly affected by particle inertia. The model is validated against Suffield experimental data in which coarse particulate deposition was measured out to a distance of 800 m from the source (Walker, 1965). Good agreement is found for the decay in ground deposits with distance from the source for stable atmospheres. Deposition data was also simulated for unstable atmospheric stratification and the current model was determined to modestly underestimate the peak concentration with increasing accuracy further downwind of the release. The current model's effective deposition velocity was compared to that suggested by Kim et al. (2000) and shows improvement with respect to FDM. Lastly, the model was used to simulate the dispersion of nine lognormal aerosol puffs in the lowest 50 m of the atmospheric surface layer for four classes of atmospheric stability. The simulated mass median aerodynamic diameters (MMAD) at multiple downwind sampling locations were calculated and plotted with distance from the source. The first 50 m from the source was found to have a substantial impact on the evolution of MMAD for stable atmospheric conditions. Away from the source, it was observed that particle size distributions were truncated by removal of all particles larger than about 60 μm. A particle Peclet number was also defined to quantify the relative importance of turbulent dispersion and sedimentation on particle motion in the vertical direction.     

Irradiation of sorbents by ions of polymorphic metals for modeling <Superscript>90</Superscript>strontium sedimentation

Background, Aims and Scope Advances in radioecology can support improvements in environmental remediation technologies, especially by illuminating interaction processes between polymorphic metal radionuclides and various materials and their ions in aqueous solutions. This study modeled interaction processes of ⁹⁰Sr with transitive metals to delineate the behavior of polymorphic metal radionuclides. Experimental and modeling results confirmed Sr sedimentation was sensitive to the physical impact of radionuclides on various sorbents and possible chemical reactions occurring between the radionuclides and sorbents. Methods Models were developed to simulate ⁹⁰Sr sedimentation process, and the potential physical and chemical reactions accompanying the process. Models were verified, inorganic salts were used as sorbents to absorb metal cations, activity levels were recorded before and after mixing the inorganic salts while the efficiency of sedimentation using the heavy metals composites was quantified. Results and Discussion This research demonstrates that the process of the sedimentation is complex and occurs in several stages. Micro-structural analysis shows that zones of interaction between the sorbent and source metal are formed during the irradiation of the target’s metal surface. Electrical-microscopic analysis indicates that the composition of the formed zones of interaction of Ti (Sr) with target metals has various structures. Roentgenophase analysis indicates that the interaction of the ions of a precipitable source and a target occurs according to constitution diagrams of equilibrium systems. The results indicate that application of inorganic salts composites based on modeling increases the efficiency of the deactivation of aqueous solutions when compared to standard aluminum sulfate composite. Conclusions Experimental and modeling results confirm ⁹⁰Sr sedimentation is sensitive to the physical impact of radionuclides on various sorbents and possible chemical reactions occurring between the radionuclides and sorbents. The models support estimation of the physical impact of polymorphic metal radionuclides on various components of sorbents and possible chemical reactions occurring between the radionuclides and sorbents during the interaction. Inorganic salt composites deactivate and clear ⁹⁰Sr and Sr⁺² from water. This paper is openly accessible!     

A study of the movement of radioactive material released during the Windscale fire in October 1957 using ERA40 data

In October 1957 a fire in Pile Number 1, a nuclear reactor at the Windscale Works, Sellafield, resulted in the accidental release of radionuclides to the atmosphere. Previous studies have described the atmospheric transport of the resultant radioactive plume from its release on the Cumbrian coast of Northwest England to its passage across mainland Europe. Those past studies have suffered from uncertainties concerning the quantity and timing of emissions and meteorological conditions. Crabtree [1959. The travel and diffusion of the radioactive material emitted during the Windscale accident. Quarterly Journal of the Royal Meteorological Society 85, 362] initially produced estimates of plume transport based on weather observations and radiosonde profiles. Later, ApSimon et al. [1985. Long-range atmospheric dispersion of radioisotopes—I. The MESOS model. Atmospheric Environment 19(1), 99–111] based estimates of plume transport on trajectories calculated from weather charts. More recently, Nelson et al. [2006. A study of the movement of radioactive material discharged during the Windscale fire in October 1957. Atmospheric Environment, 40, 58–75] used a full three-dimensional dispersion model using digitised weather data from similar charts.This study aims to further reduce uncertainty in the plume's behaviour by using the latest available Numerical Weather Prediction Model reanalysis of meteorological data from the European Centre for Medium Range Weather Forecasts (ERA-40) coupled with current best estimates of the radioactive emissions profile. The results presented here generally support the findings of previous studies though an improvement in model comparisons against observational measurements has been found. The opportunity was also taken to extend the time horizon, and hence geographical coverage, of the modelled plume. It is considered that this paper presents the best estimate to date of the plume's behaviour.     

Simulation of the evolution of particle size distributions in a vehicle exhaust plume with unconfined dilution by ambient air

Over the past several years, numerous studies have linked ambient concentrations of particulate matter (PM) to adverse health effects, and more recent studies have identified PM size and surface area as important factors in determining the health effects of PM. This study contributes to a better understanding of the evolution of particle size distributions in exhaust plumes with unconfined dilution by ambient air. It combines computational fluid dynamics (CFD) with an aerosol dynamics model to examine the effects of different streamlines in an exhaust plume, ambient particle size distributions, and vehicle and wind speed on the particle size distribution in an exhaust plume. CFD was used to calculate the flow field and gas mixing for unconfined dilution of a vehicle exhaust plume, and the calculated dilution ratios were then used as input to the aerosol dynamics simulation. The results of the study show that vehicle speed affected the particle size distribution of an exhaust plume because increasing vehicle speed caused more rapid dilution and inhibited coagulation. Ambient particle size distributions had an effect on the smaller sized particles (approximately 10 nm range under some conditions) and larger sized particles (>2 microm) of the particle size distribution. The ambient air particle size distribution affects the larger sizes of the exhaust plume because vehicle exhaust typically contains few particles larger than 2 microm. Finally, the location of a streamline in the exhaust plume had little effect on the particle size distribution; the particle size distribution along any streamline at a distance x differed by less than 5% from the particle size distributions along any other streamline at distance x.     

Simulation of Sulfate and Nitrate Chemistry in Power Plant Plumes

ABSTRACT

The rate of formation of secondary particulate matter (PM) in power plant plumes varies as the plume material mixes with the background air. Consequently, the rate of oxidation of sulfur dioxide (SO₂) and nitrogen dioxide (NO₂) to sulfate and nitric acid, respectively, can be very different in plumes and in the background air (i.e., air outside the plume). In addition, the formation of sulfate and nitric acid in a power plant plume is a strong function of the chemical composition of the background air and the prevailing meteorological conditions.

We describe the use of a reactive plume model, the Reactive and Optics Model of Emissions, to simulate sulfate and nitrate formation in a power plant plume for a variety of background conditions. We show that SO₂ and NO₂ oxidation rates are maximum in the background air for volatile organic compound (VOC)-limited airsheds but are maximum at some downwind distance in the plume when the background air is nitrogen oxide (NO_x)-limited. Our analysis also shows that it is essential to obtain measurements of background concentrations of ozone, aldehydes, peroxyacetyl nitrate, and other VOCs to properly describe plume chemistry.     

The chernobyl accident: Modelling of dispersion over europe of the radioactive plume and comparison with air activity measurements

Following the release of radionuclides from the Chernobyl power plant accident, a long-range transport and deposition model is used to describe the plume dispersion over Europe. The aim of this study is the validation of a fast Lagrangjan model and a better understanding of the relative impact of some mechanisms, such as the initial plume rise. Comparisons between results and ¹³⁷Cs measurement activity are discussed according to spatial and temporal variations. It is shown that many measurements can be explained only if the initial plume rise taken at 925, 850 and 700mb is considered.     

Radiative transfer budgets for scattering and absorbing plumes: Measurements and model predictions

The 1981 VISTTA field study characterized the composition and appearance of particle-rich plumes from three different sources. This paper compares the VISTTA observations with the predictions of two plume visibility models. Observations and predictions are analyzed from the perspective of exact solutions to the equations of radiative transfer for a somewhat idealized atmosphere. These solutions, which explicity relate plume/sky contrast to the composition of plume and background and the geometry of sun, plume and observer, are shown to be consistent with the VISTA observations. The simplified relationships are used as the basis for budgeting radiative transfer by the plume and background, and for analyses of the sensitivity of plume appearance to individual variables.The optics predictions of the two models are less accurate for plumes dominated by particle scattering than they are for plumes dominated by NO₂ absorption. Inaccurate prediction of plume particle size distributions can be identified as an important source of error. Inaccurate prediction of background sky radiance is suspected as another.     

Comparison of E. coli, enterococci, and fecal coliform as indicators for brackish water quality assessment.

Escherichia coli (E. coli), enterococci, and fecal coliform data were collected and compared as potential indicators for swimmablility assessment of a brackish waterbody (Lake Pontchartrain, Louisiana). These indicators were measured during lake background conditions, in stormwater runoff (before dilution with lake water), and in the outfall plume within the lake following storm events. Microbial indicator titers associated with suspended particles and lake-bottom sediments were also investigated. Overall reduction rate constants for fecal coliform, E. coli, and enterococci in lake water and sediment were measured and reported. Attachment of microbial indicators to suspended matter and subsequent sedimentation appeared to be a significant fate mechanism. A slower reduction rate of indicator organisms in sediment further suggested that bottom sediment may act as a reservoir for prolonging indicator organism survival and added concern of recontamination of overlaying waters due to potential solids resuspension. Results indicated that enterococci might be a more stable indicator than E. coli and fecal coliform and, consequently, a more conservative indicator under brackish water conditions.     

Evaluation of Downwash Modifications to the Industrial Source Complex Model

The Industrial Source Complex (ISC) model has been modified to account for Improved understanding of plume rise and downwash around buildings. Two sets of observations are used to compare the modified and the original ISC models, showing that the new model better simulates the observed concentrations during high-wind conditions when downwash usually occurs.     

Biodegradation modelling of a dissolved gasoline plume applying independent laboratory and field parameters

Biodegradation of organic contaminants in groundwater is a microscale process which is often observed on scales of 100s of metres or larger. Unfortunately, there are no known equivalent parameters for characterizing the biodegradation process at the macroscale as there are, for example, in the case of hydrodynamic dispersion. Zero- and first-order degradation rates estimated at the laboratory scale by model fitting generally overpredict the rate of biodegradation when applied to the field scale because limited electron acceptor availability and microbial growth are not considered. On the other hand, field-estimated zero- and first-order rates are often not suitable for predicting plume development because they may oversimplify or neglect several key field scale processes, phenomena and characteristics. This study uses the numerical model BIO3D to link the laboratory and field scales by applying laboratory-derived Monod kinetic degradation parameters to simulate a dissolved gasoline field experiment at the Canadian Forces Base (CFB) Borden. All input parameters were derived from independent laboratory and field measurements or taken from the literature a priori to the simulations. The simulated results match the experimental results reasonably well without model calibration. A sensitivity analysis on the most uncertain input parameters showed only a minor influence on the simulation results. Furthermore, it is shown that the flow field, the amount of electron acceptor (oxygen) available, and the Monod kinetic parameters have a significant influence on the simulated results. It is concluded that laboratory-derived Monod kinetic parameters can adequately describe field scale degradation, provided all controlling factors are incorporated in the field scale model. These factors include advective–dispersive transport of multiple contaminants and electron acceptors and large-scale spatial heterogeneities.     

Performance of a Gaussian model for centerline concentrations in the wake of buildings

This paper examines the performance and inherent limitations of a Gaussian plume model for predicting ground-level plume centerline concentrations in the wake of buildings. The Gaussian plume equation has been modified to incorporate building wake enhanced dispersion parameters. Model-predicted concentrations were compared to three sets of field observations. Predicted and observed concentrations were partitioned into groups by source-receptor distance, atmospheric stability class, and source-release height. The group analyses provided a way to identify sources of model error. The variability of errors was found to have values between 50 and 100 % of the mean observed concentration for groups where the mean error was small.     

Development of a microscale emission factor model for particulate matter for predicting real-time motor vehicle emissions

The U.S. Environmental Protection Agency's National Exposure Research Laboratory is pursuing a project to improve the methodology for modeling human exposure to motor vehicle emissions. The overall project goal is to develop improved methods for modeling the source through the air pathway to human exposure in significant exposure microenvironments. Current particulate matter (PM) emission models, particle emission factor model (used in the United States, except California) and motor vehicle emission factor model (used in California only), are suitable only for county-scale modeling and emission inventories. There is a need to develop a site-specific real-time emission factor model for PM emissions to support human exposure studies near roadways. A microscale emission factor model for predicting site-specific real-time motor vehicle PM (MicroFacPM) emissions for total suspended PM, PM less than 10 microm aerodynamic diameter, and PM less than 2.5 microm aerodynamic diameter has been developed. The algorithm used to calculate emission factors in MicroFacPM is disaggregated, and emission factors are calculated from a real-time fleet, rather than from a fleet-wide average estimated by a vehicle-miles-traveled weighting of the emission factors for different vehicle classes. MicroFacPM requires input information necessary to characterize the site-specific real-time fleet being modeled. Other variables required include average vehicle speed, time and day of the year, ambient temperature, and relative humidity.     

Fractionation and composition of colloidal and suspended particulate materials in rivers

The association of pollutants (nutrients, heavy metals and organic compounds) with colloidal and suspended particle matter (SPM) plays a dominant role in determining their transport, fate, biogeochemistry, bioavailability and toxicity in natural waters. A scheme for the fractionation and composition of colloidal and SPM from river waters has been tested. All four separation methods, i.e. sieving, continuous flow centrifugation, tangential flow filtration, sedimentation field-flow fractionation, were for the first time used to separate five size particulate fractions from river. Significant (gram) amounts of colloidal material (<1 microm) in three size ranges, nominally 1-0.2, 0.2-0.006 and 0.006-0.003 microm were obtained. The separation scheme was able to process large samples (100 l), within reasonable times (1 day) and the apparatus was portable. The aquatic colloid size was also characterized with high resolution by using sedimentation field-flow fractionation technique. The mass-based particle size distribution for the water sample showed a broad size distribution between 0.05 and 0.4 microm with the maximum around 0.14 microm. There was a systematic increase in the content of organic carbon (estimated by loss on ignition), Mg, Ca, Na, Cu and Zn with decreasing particle size, highlighting the importance of the colloidal (<1 microm) fraction. It was concluded that the colloidal Cu and Zn concentrations in rivers might be much higher than those reported before.     

Theoretical study of the impact of particulate matter gravitational settling on ambient coarse particulate matter monitoring for agricultural emissions

The particle size distributions (PSDs) of particulate matter (PM) in the downwind plume from simulated sources of a cotton gin were analyzed to determine the impact of PM settling on PM monitoring. The PSD of PM in a plume varies as a function of gravitational settling. Gravitational settling has a greater impact on the downwind PSD from sources with PSDs having larger mass median diameters (MMDs). The change in PSD is a function of the source PSD of emitted PM, wind speed, and downwind distance. Both MMD and geometric standard deviation (GSD) in the downwind plume decrease with an increase in downwind distance and source MMD. The larger the source MMD, the greater the change in the downwind MMD and GSD. Also, the greater the distance from the source to the sampler, the greater the change in the downwind MMD and GSD. Variations of the PSD in the downwind plume significantly impact PM10 sampling errors associated with the U.S. Environmental Protection Agency (EPA) PM10 samplers. For the emission sources with MMD > 10 microm, the PM10 oversampling rate increases with an increase in downwind distance caused by the decrease of GSD of the PSD in the downwind plume. Gravitational settling of particles does not help reduce the oversampling problems associated with the EPA PM10 sampler. Furthermore, oversampling rates decrease with an increase of the wind speed.     

Validation of the operational emergency response model at the Swedish Meteorological and Hydrological Institute using data from etex and the chernobyl accident

The Eulerian atmospheric tracer transport model MATCH (Multiscale Atmospheric Transport and Chemistry model) has been extended with a Lagrangian particle model treating the initial dispersion of pollutants from point sources. The model has been implemented at the Swedish Meteorological and Hydrological Institute in an emergency response system for nuclear accidents and can be activated on short notice to provide forecast concentration and deposition fields.The model has been used to simulate the transport of the inert tracer released during the ETEX experiment and the transport and deposition of ¹³⁷Cs from the Chernobyl accident. Visual inspection of the results as well as statistical analysis shows that the extent, time of arrival and duration of the tracer cloud, is in good agreement with the observations for both cases, with a tendency towards over-prediction for the first ETEX release. For the Chernobyl case the simulated deposition pattern over Scandinavia and over Europe as a whole agrees with observations when observed precipitation is used in the simulation. When model calculated precipitation is used, the quality of the simulation is reduced significantly and the model fails to predict major features of the observed deposition field.