Atmospheric fate and transport of dioxins: local impacts

We conducted model simulations of the atmospheric fate and transport of PCDD/F to assess the fraction of emitted PCDD/F that would deposit within 100 km from the source. We considered eight major categories of PCDD/F emission sources and six different locations, to cover a wide range of source characteristics, PCDD/F congener profiles and particle size distributions, meteorological conditions and terrain configurations. These results suggest that for sources that have tall stacks and/or high plume rise (e.g., copper smelters, cement kilns, sinter plants), only a small fraction of PCDD/F emissions is deposited locally (typically, less than 10% within 100 km). Other source categories such as municipal solid waste incinerators, medical waste incinerators and diesel trucks lead to a greater fraction of PCDD/F being deposited locally; nevertheless, the majority of their PCDD/F emissions tends to be transported beyond 100 km. Although local impacts may need to be addressed for these latter source categories, it appears that the long-range potential impacts of PCDD/F need to be addressed for all source categories. Sensitivity studies were conducted to investigate the effect of various key model inputs on simulation results. These studies suggest that an advanced atmospheric dispersion model should be used for cases where PCDD/F emissions may present some local concerns because the results are very sensitive to the treatment of dispersion. Also, it is essential to obtain accurate characterizations of the particle size distribution of particulate PCDD/F because the dry deposition flux is very sensitive to the particle size distribution.     

Use of CALPUFF for exposure assessment in a near-field,complex terrain setting

CALPUFF is an atmospheric source-receptor model recommended by the U.S. Environmental Protection Agency for use on a case-by-case basis in complex terrain and wind conditions. The ability of the model to provide useful information for exposure assessments in areas with those topographical and meteorological conditions has received little attention. This is an important knowledge gap for use of CALPUFF outside of regulatory applications, such as exposure analyses conducted in support of risk assessments and health studies. We compared deposition of cadmium (Cd), lead (Pb), and zinc (Zn) calculated with CALPUFF as a result of emissions from a zinc smelter with corresponding concentrations of the metals measured in attic dust and soil samples obtained from the surrounding area. On a point-by-point analysis, predictions from CALPUFF explained 11% (lead) to 53% (zinc) of the variability in concentrations measured in attic dust. Levels of heavy metals in soil interpolated to 100 residential addresses from the distribution of concentrations measured in soil samples also agreed well with deposition predicted with CALPUFF: R² of 0.46, 0.76, and 079 for Pb, Cd, and Zn, respectively. Community-average concentrations of Cd, Pb, and Zn measured in soil were significantly (p < 0.0001) and strongly correlated (R² ranged from 0.77 to 0.98) with predicted deposition rates. These findings demonstrate that CALPUFF can provide reasonably accurate predictions of the patterns of long-term air pollutant deposition in the near-field associated with emissions from a discrete source in complex terrain. Because deposition estimates are calculated as a linear function of air concentrations, CALPUFF is expected to be reliable model for prediction of long-term average, near-field ambient air concentrations in complex terrain as well.     

Road traffic impact on urban water quality: a step towards integrated traffic,air and stormwater modelling

Methods for simulating air pollution due to road traffic and the associated effects on stormwater runoff quality in an urban environment are examined with particular emphasis on the integration of the various simulation models into a consistent modelling chain. To that end, the models for traffic, pollutant emissions, atmospheric dispersion and deposition, and stormwater contamination are reviewed. The present study focuses on the implementation of a modelling chain for an actual urban case study, which is the contamination of water runoff by cadmium (Cd), lead (Pb), and zinc (Zn) in the Grigny urban catchment near Paris, France. First, traffic emissions are calculated with traffic inputs using the COPERT4 methodology. Next, the atmospheric dispersion of pollutants is simulated with the Polyphemus line source model and pollutant deposition fluxes in different subcatchment areas are calculated. Finally, the SWMM water quantity and quality model is used to estimate the concentrations of pollutants in stormwater runoff. The simulation results are compared to mass flow rates and concentrations of Cd, Pb and Zn measured at the catchment outlet. The contribution of local traffic to stormwater contamination is estimated to be significant for Pb and, to a lesser extent, for Zn and Cd; however, Pb is most likely overestimated due to outdated emissions factors. The results demonstrate the importance of treating distributed traffic emissions from major roadways explicitly since the impact of these sources on concentrations in the catchment outlet is underestimated when those traffic emissions are spatially averaged over the catchment area.     

The MICS-Asia study: model intercomparison of long-range transport and sulfur deposition in East Asia

An intercomparison study involving eight long-range transport models for sulfur deposition in East Asia has been initiated. The participating models included Eulerian and Lagrangian frameworks, with a wide variety of vertical resolutions and numerical approaches. Results from this study, in which models used common data sets for emissions, meteorology, and dry, wet and chemical conversion rates, are reported and discussed. Model results for sulfur dioxide and sulfate concentrations, wet deposition amounts, for the period January and May 1993, are compared with observed quantities at 18 surface sites in East Asia. At many sites the ensemble of models is found to have high skill in predicting observed quantities. At other sites all models show poor predictive capabilities. Source–receptor relationships estimated by the models are also compared. The models show a high degree of consistency in identifying the main source–receptor relationships, as well as in the relative contributions of wet/dry pathways for removal. But at some locations estimated deposition amounts can vary by a factor or 5. The influence of model structure and parameters on model performance is discussed. The main factors determining the deposition fields are the emissions and underlying meteorological fields. Model structure in terms of vertical resolution is found to be more important than the parameterizations used for chemical conversion and removal, as these processes are highly coupled and often work in compensating directions.     

Modelling local and synoptic scale influences on ozone concentrations in a topographically complex region of Southern Italy

A modelling study with the on-line coupled Eulerian chemical-weather model WRF/Chem for the Southern Italian region around Cosenza (Calabria) was conducted to identify the influences of synoptic scale meteorology, local scale wind systems and local emissions on ozone concentrations in this orographically complex region. Four periods of 5–7 days were chosen, one from each season, which had wind pattern characteristics representative of typical local climatological conditions, in order to study the local versus non-local impacts on ozone transport and formation. To account for the complex terrain, the horizontal resolution of the smallest modelling domain was 3 km. Model results were compared with measurements to demonstrate the capability of the model to reproduce ozone concentrations in the region. The comparison was favourable with a mean bias of ?1.1 ppb. The importance of local emissions on ozone formation and destruction was identified with the use of three different emission scenarios. Generally the influence of regional emissions on the average ozone concentration was small. However during periods when mountain-sea wind systems were well developed and synoptic scale winds were weak, the influence of local emissions from the urban area was at its greatest. The maximum influence of local emissions on ozone concentrations was 18 ppb.     

The effects of roadside structures on the transport and dispersion of ultrafine particles from highways

Understanding local-scale transport and dispersion of pollutants emitted from traffic sources is important for urban planning and air quality assessments. Predicting pollutant concentration patterns in complex environments depends on accurate representations of local features (e.g., noise barriers, trees, buildings) affecting near-field air flows. This study examined the effects of roadside barriers on the flow patterns and dispersion of pollutants from a high-traffic highway in Raleigh, North Carolina, USA. The effects of the structures were analyzed using the Quick Urban & Industrial Complex (QUIC) model, an empirically based diagnostic tool which simulates fine-scale wind field and dispersion patterns around obstacles. Model simulations were compared with the spatial distributions of ultrafine particles (UFP) from vehicular emissions measured using a passenger van equipped with a Differential Mobility Analyzer/Condensation Particle Counter. The field site allowed for an evaluation of pollutant concentrations in open terrain, with a noise barrier present near the road, and with a noise barrier and vegetation present near the road.Results indicated that air pollutant concentrations near the road were generally higher in open terrain situations with no barriers present; however, concentrations for this case decreased faster with distance than when roadside barriers were present. The presence of a noise barrier and vegetation resulted in the lowest downwind pollutant concentrations, indicating that the plume under this condition was relatively uniform and vertically well-mixed. Comparison of the QUIC model with the mobile UFP measurements indicated that QUIC reasonably represented pollutant transport and dispersion for each of the study configurations.     

Source apportion of atmospheric particulate matter: a joint Eulerian/Lagrangian approach

PM_2.5 samples were collected during an annual monitoring campaign (January 2012–January 2013) in the urban area of Naples, one of the major cities in Southern Italy. Samples were collected by means of a standard gravimetric sampler (Tecora Echo model) and characterized from a chemical point of view by ion chromatography. As a result, 143 samples together with their ionic composition have been collected. We extend traditional source apportionment techniques, usually based on multivariate factor analysis, interpreting the chemical analysis results within a Lagrangian framework. The Hybrid Single-Particle Lagrangian Integrated Trajectory Model (HYSPLIT) model was used, providing linkages to the source regions in the upwind areas. Results were analyzed in order to quantify the relative weight of different source types/areas. Model results suggested that PM concentrations are strongly affected not only by local emissions but also by transboundary emissions, especially from the Eastern and Northern European countries and African Saharan dust episodes.     

A complex terrain dispersion model for regulatory applications

This paper demonstrates the development of a model designed to estimate concentrations associated with a source situated in complex terrain. The model is designed to provide estimates of concentration distributions and is thus primarily suitable for regulatory applications. The model assumes that the concentration at a receptor is a combination of concentrations caused by two asymptotic states: the plume remains horizontal, and the plume climbs over the hill. The factor that weights the two states is a function of the fractional mass of the plume above the dividing streamline height. The model has been evaluated against data from four complex terrain sites. The evaluation shows that the model performs at least as well as CTDMPLUS (Perry, S.G., 1992. CTDMPLUS, a dispersion model for sources near complex topography. Part I: technical formations. Journal of Applied Meteorology 31, 633–645), a more comprehensive model designed for complex terrain applications.     

A statistical approach for estimating uncertainty in dispersion modeling: An example of application in southwestern USA

A method based on a statistical approach of estimating uncertainty in simulating the transport and dispersion of atmospheric pollutants is developed using observations and modeling results from a tracer experiment in the complex terrain of the southwestern USA. The method takes into account the compensating nature of the error components by representing all terms, except dispersion error and variance of stochastic processes. Dispersion error and the variance of the stochastic error are estimated using the maximum likelihood estimation technique applied to the equation for the fractional error. Mesoscale Model 5 (MM5) and a Lagrangian random particle dispersion model with three optional turbulence parameterizations were used as a test bed for method application. Modeled concentrations compared well with the measurements (correlation coefficients on the order of 0.8). The effects of changing two structural components (the turbulence parameterization and the model grid vertical resolution) on the magnitude of the dispersion error also were examined. The expected normalized dispersion error appears to be quite large (up to a factor of three) among model runs with various turbulence schemes. Tests with increased vertical resolution of the atmospheric model (MM5) improved most of the dispersion model statistical performance measures, but to a lesser extent compared to selection of a turbulence parameterization. Method results confirm that structural components of the dispersion model, namely turbulence parameterizations, have the most influence on the expected dispersion error.     

Urban scale modeling of particle number concentration in Stockholm

A three-dimensional dispersion model has been implemented over the urban area of Stockholm (35×35 km) to assess the spatial distribution of number concentrations of particles in the diameter range 3–400 nm. Typical number concentrations in the urban background of Stockholm is 10 000 cm⁻³, while they are three times higher close to a major highway outside the city and seven times higher within a densely trafficked street canyon site in the city center. The model, which includes an aerosol module for calculating the particle number losses due to coagulation and dry deposition, has been run for a 10-day period. Model results compare well with measured data, both in levels and in temporal variability. Coagulation was found to be of little importance in terms of time averaged concentrations, contributing to losses of only a few percent as compared to inert particles, while dry deposition yield particle number losses of up to 25% in certain locations. Episodic losses of up to 10% due to coagulation and 50% due to deposition, are found some kilometers downwind of major roads, rising in connection with low wind speed and suppressed turbulent mixing. Removal due to coagulation and deposition will thus be more significant for the simulation of extreme particle number concentrations during peak episodes.The study shows that dispersion models with proper aerosol dynamics included may be used to assess particle number concentrations in Stockholm, where ultrafine particles principally originate from traffic emissions. Emission factors may be determined from roadside measurements, but ambient temperature must be considered, as it has a strong influence on particle number emissions from vehicles.     

A Comparison of Model Performance between AERMOD and AUSTAL2000

ABSTRACT

In this study the performance of the American Meteorological Society and U.S. Environmental Protection Agency Regulatory Model (AERMOD), a Gaussian plume model, is compared in five test cases with the German Dispersion Model according to the Technical Instructions on Air Quality Control (Ausbreitungsmodell gemäβ der Technischen Anleitung zur Reinhaltung der Luft) (AUSTAL2000), a Lagrangian model. The test cases include different source types, rural and urban conditions, flat and complex terrain. The predicted concentrations are analyzed and compared with field data. For evaluation, quantile-quantile plots were used. Further, a performance measure is applied that refers to the upper end of concentration levels because this is the concentration range of utmost importance and interest for regulatory purposes. AERMOD generally predicted concentrations closer to the field observations. AERMOD and AUSTAL2000 performed considerably better when they included the emitting power plant building, indicating that the downwash effect near a source is an important factor. Although AERMOD handled mountainous terrain well, AUSTAL2000 significantly underestimated the concentrations under these conditions. In the urban test case AUSTAL2000 did not perform satisfactorily. This may be because AUSTAL2000, in contrast to AERMOD, does not use any algorithm for nightly turbulence as caused by the urban heat island effect. Both models performed acceptable for a nonbuoyant volume source. AUSTAL2000 had difficulties in stable conditions, resulting in severe underpredictions. This analysis indicates that AERMOD is the stronger model compared with AUSTAL2000 in cases with complex and urban terrain. The reasons for that seem to be AUSTAL2000's simplification of the meteorological input parameters and imprecision because of rounding errors.

IMPLICATIONS This study contributes to the understanding of dispersion modeling and demonstrates the advantage of detailed meteorological data. It also helps air quality regulators and planners to identify the most appropriate model to use. It is indicated that AERMOD is more suitable for air quality planning and regulation, when all required meteorological information is available, because its predictions are mostly closer to field observations. Furthermore AUSTAL2000 predicted concentrations that showed a narrow range and triggered far less impacts from the source.     

Modeling studies of ammonia dispersion and dry deposition at some hog farms in North Carolina

A modeling study was conducted on dispersion and dry deposition of ammonia taking one hog farm as a unit. The ammonia emissions used in this study were measured under our OPEN (Odor, Pathogens, and Emissions of Nitrogen) project over a waste lagoon and from hog barns. Meteorological data were also collected at the farm site. The actual layout of barns and lagoons on the farms was used to simulate dry deposition downwind of the farm. Dry deposition velocity, dispersion, and dry deposition of ammonia were studied over different seasons and under different stability conditions using the short-range dispersion/air quality model, AERMOD. Dry deposition velocities were highest under near-neutral conditions and lowest under stable conditions. The highest deposition at short range occurred under nighttime stable conditions and the lowest occurred during daytime unstable conditions. Significant differences in deposition over crop and grass surfaces were observed under stable conditions.     

Lagrangian sampling of 3-D air quality model results for regional transport contributions to sulfate aerosol concentrations at Baltimore,MD, in summer 2004

We use ensemble-mean Lagrangian sampling of a 3-D Eulerian air quality model, CMAQ, together with ground-based ambient monitors data from several air monitoring networks and satellite (MODIS) observations to provide source apportionment and regional transport vs. local contributions to sulfate aerosol and PM_2.5 concentrations at Baltimore, MD, for summer 2004. The Lagrangian method provides estimates of the chemical and physical evolution of air arriving in the daytime boundary layer at Baltimore. Study results indicate a dominant role for regional transport contributions on those days when sulfate air pollution is highest in Baltimore, with a principal transport pathway from the Ohio River Valley (ORV) through southern Pennsylvania and Maryland, consistent with earlier studies. Thus, reductions in sulfur emissions from the ORV under the EPA's Clean Air Interstate Rule may be expected to improve particulate air quality in Baltimore during summer. The Lagrangian sampling of CMAQ offers an inexpensive and complimentary approach to traditional methods of source apportionment based on multivariate observational data analysis, and air quality model emissions separation. This study serves as a prototype for the method applied to Baltimore. EPA is establishing a system to allow air quality planners to readily produce and access equivalent results for locations of their choice.     

The effect of the limited availability of H2O2 in the competitive deposition of sulfur and oxidized nitrogen

To understand the influence of the reduction of SO2 emissions from a single source in the S and N deposition around its local environment, the application of the Sulphur Transport Eulerian Model 2 (STEM-II) was introduced in this paper. Observed local deposition patterns were analysed and explained in terms of the main processes involved in the pollutants deposition. It was necessary to take into account the limited availability of H2O2 because of its influence on both S(IV) and oxidized nitrogen deposition. In order to estimate the quantitative relationship between the SO2 emissions reduction and the observed S and N deposition patterns, these processes were simulated for different meteorological conditions. Simulation results were in agreement with both observed deposition patterns and limited availability of H2O2, specially if significant changes in the S deposition patterns were considered. Both observed and estimated S deposition patterns changed their top value location from the Southwest (1990) to the Northwest (1997) of the domain, because of the reduction of dry deposition. The global reduction of total S depositions, estimated and observed, were in good agreement too. Model simulations could explain the higher S dry deposition reduction, considering the emissions reduction strategy applied.     

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

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

A comparison of model performance between AERMOD and AUSTAL2000

In this study the performance of the American Meteorological Society and U.S. Environmental Protection Agency Regulatory Model (AERMOD), a Gaussian plume model, is compared in five test cases with the German Dispersion Model according to the Technical Instructions on Air Quality Control (Ausbreitungsmodell gem?beta der Technischen Anleitung zur Reinhaltung der Luft) (AUSTAL2000), a Lagrangian model. The test cases include different source types, rural and urban conditions, flat and complex terrain. The predicted concentrations are analyzed and compared with field data. For evaluation, quantile-quantile plots were used. Further, a performance measure is applied that refers to the upper end of concentration levels because this is the concentration range of utmost importance and interest for regulatory purposes. AERMOD generally predicted concentrations closer to the field observations. AERMOD and AUSTAL2000 performed considerably better when they included the emitting power plant building, indicating that the downwash effect near a source is an important factor. Although AERMOD handled mountainous terrain well, AUSTAL2000 significantly underestimated the concentrations under these conditions. In the urban test case AUSTAL2000 did not perform satisfactorily. This may be because AUSTAL2000, in contrast to AERMOD, does not use any algorithm for nightly turbulence as caused by the urban heat island effect. Both models performed acceptable for a nonbuoyant volume source. AUSTAL2000 had difficulties in stable conditions, resulting in severe underpredictions. This analysis indicates that AERMOD is the stronger model compared with AUSTAL2000 in cases with complex and urban terrain. The reasons for that seem to be AUSTAL2000's simplification of the meteorological input parameters and imprecision because of rounding errors.     

Long-range transport of acidifying substances in East Asia—Part II: Source–receptor relationships

Region-to-grid source–receptor (S/R) relationships are established for sulfur and reactive nitrogen deposition in East Asia, using the Eulerian-type Community Multiscale Air Quality (CMAQ) model with emission and meteorology data for 2001. We proposed a source region attribution methodology by analyzing the non-linear responses of the CMAQ model to emission changes. Sensitivity simulations were conducted where emissions of SO₂, NO_x, and primary particles from a source region were reduced by 25%. The difference between the base and sensitivity simulations was multiplied by a factor of four, and then defined as the contribution from that source region. The transboundary influence exhibits strong seasonal variation and generally peaks during the dry seasons. Long-range transport from eastern China contributes a significant percentage (>20%) of anthropogenic reactive nitrogen as well as sulfur deposition in East Asia. At the same time, northwestern China receives approximately 35% of its sulfur load and 45% of its nitrogen load from foreign emissions. Sulfur emissions from Miyakejima and other volcanoes contribute approximately 50% of the sulfur load in Japan in 2001. Sulfur inflows from regions outside the study domain, which is attributed by using boundary conditions derived from the MOZART global atmospheric chemistry model, are pronounced (10–40%) over most parts of Asia. Compared with previous studies using simple Lagrangian models, our results indicate higher influence from long-range transport. The estimated S/R relationships are believed to be more realistic since they include global influence as well as internal interactions among different parts of China.     

Modelling atmospheric mercury transport and deposition across Europe and the UK

There are inadequate measurements of surface ambient concentrations of mercury species and their deposition rates for the UK deposition budget to be characterized. In order to estimate the overall mercury flux budget for the UK, a simple long-term 1D Lagrangian trajectory model was constructed that treats emissions (1998), atmospheric transformation and deposition across Europe. The model was used to simulate surface concentrations of mercury and deposition across Europe at a resolution of 50 km×50 km and across the UK at 20 km×20 km. The model appeared to perform adequately when compared with the few available measurements, reproducing mean concentrations of elemental gaseous mercury at particular locations and the magnitude of regional gradients. The model showed that 68% of the UK's mercury emissions are exported and 32% deposited within the UK. Of deposition to the UK, 25% originates from the Northern Hemisphere/global background, 41% from UK sources and 33% from other European countries. The total mercury deposition to the UK is in good agreement with other modelling, 9.9 tonne yr⁻¹ cf. 9.0 tonne yr⁻¹, for 1998. However, the attribution differs greatly from the results of other coarser-scale modelling, which allocates 55% of the deposition to the UK from UK sources, 4% from other European countries and 60% from the global background atmosphere. The model was found to be sensitive to the speciation of emissions and the dry deposition velocity of elemental gaseous mercury. The uncertainties and deficiencies are discussed in terms of model parameterization and input data, and measurement data with which models can be validated. There is an urgent requirement for measurements of removal terms, concentrations, and deposition with which models can be parameterized and validated.     

Source apportionment of particulate matter (PM2.5) in an urban area using dispersion,receptor and inverse modelling

Air pollution emission inventories are the basis for air quality assessment and management strategies. The quality of the inventories is of great importance since these data are essential for air pollution impact assessments using dispersion models. In this study, the quality of the emission inventory for fine particulates (PM_2.5) is assessed: first, using the calculated source contributions from a receptor model; second, using source apportionment from a dispersion model; and third, by applying a simple inverse modelling technique which utilises multiple linear regression of the dispersion model source contributions together with the observed PM_2.5 concentrations. For the receptor modelling the chemical composition of PM_2.5 filter samples from a measurement campaign performed between January 2004 and April 2005 are analysed. Positive matrix factorisation is applied as the receptor model to detect and quantify the various source contributions. For the same observational period and site, dispersion model calculations using the Air Quality Management system, AirQUIS, are performed. The results identify significant differences between the dispersion and receptor model source apportionment, particularly for wood burning and traffic induced suspension. For wood burning the receptor model calculations are lower, by a factor of 0.54, but for the traffic induced suspension they are higher, by a factor of 7.1. Inverse modelling, based on regression of the dispersion model source contributions and the PM_2.5 concentrations, indicates similar discrepancies in the emissions inventory. In order to assess if the differences found at the one site are generally applicable throughout Oslo, the individual source category emissions are rescaled according to the receptor modelling results. These adjusted PM_2.5 concentrations are compared with measurements at four independent stations to evaluate the updated inventory. Statistical analysis shows improvement in the estimated concentrations for PM_2.5 at all sites. Similarly, inverse modelling is applied at these independent sites and this confirms the validity of the receptor model results.