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.     

BTEX exposures in an area impacted by industrial and mobile sources: Source attribution and impact of averaging time

The impacts of emissions plumes from major industrial sources on black carbon (BC) and BTEX (benzene, toluene, ethyl benzene, xylene isomers) exposures in communities located >10 km from the industrial source areas were identified with a combination of stationary measurements, source identification using positive matrix factorization (PMF), and dispersion modeling. The industrial emissions create multihour plume events of BC and BTEX at the measurement sites. PMF source apportionment, along with wind patterns, indicates that the observed pollutant plumes are the result of transport of industrial emissions under conditions of low boundary layer height. PMF indicates that industrial emissions contribute >50% of outdoor exposures of BC and BTEX species at the receptor sites. Dispersion modeling of BTEX emissions from known industrial sources predicts numerous overnight plumes and overall qualitative agreement with PMF analysis, but predicts industrial impacts at the measurement sites a factor of 10 lower than PMF. Nonetheless, exposures associated with pollutant plumes occur mostly at night, when residents are expected to be home but are perhaps unaware of the elevated exposure. Averaging data samples over long times typical of public health interventions (e.g., weekly or biweekly passive sampling) misapportions the exposure, reducing the impact of industrial plumes at the expense of traffic emissions, because the longer samples cannot resolve subdaily plumes. Suggestions are made for ways for future distributed pollutant mapping or intervention studies to incorporate high time resolution tools to better understand the potential impacts of industrial plumes.

Implications: Emissions from industrial or other stationary sources can dominate air toxics exposures in communities both near the source and in downwind areas in the form of multihour plume events. Common measurement strategies that use highly aggregated samples, such as weekly or biweekly averages, are insensitive to such plume events and can lead to significant under apportionment of exposures from these sources.     

Lidar-assisted measurement of PM10 emissions from agricultural tilling in California's San Joaquin Valley – Part I: lidar

Vertical profiling with point samplers is an accepted method for quantifying the fluxes of PM₁₀ from non-point fugitive dust sources, but is limited by uncertainty in estimates of the actual height of the dust plume, especially for plumes that exceed the highest sampling height. Agricultural land preparation operations in the San Joaquin Valley were monitored using upwind–downwind vertical PM₁₀ profiles and data collected during the first successful experiment to include light detection and ranging (lidar), in 1998, were analyzed to provide modeling criteria for the 1996 and 1997 data. A series of six comprehensive PM₁₀ tests with concurrent lidar data was examined to: (a) develop a framework for analyzing upwind–downwind point PM₁₀ concentration profiles of land preparation operations (disking, listing, root cutting, and ripping) and (b) identify conditions under which the field sampling strategies affect the reproducibility of PM₁₀ concentration measurements. Lidar data were used to verify that the plume heights and shapes extrapolated from the point sampler vertical profiles adequately described the plumes. The shortcomings of the vertical profiling technique and lidar methods are discussed in the light of developing efficient robust methods for accurate PM₁₀ emissions quantification from complex non-point sources.     

Emissions of sulfur trioxide from coal-fired power plants

Emissions of sulfur trioxide (SO3) are a key component of plume opacity and acid deposition. Consequently, these emissions need to be low enough to not cause opacity violations and acid deposition. Generally, a small fraction of sulfur (S) in coal is converted to SO3 in coal-fired combustion devices such as electric utility boilers. The emissions of SO3 from such a boiler depend on coal S content, combustion conditions, flue gas characteristics, and air pollution devices being used. It is well known that the catalyst used in the selective catalytic reduction (SCR) technology for nitrogen oxides control oxidizes a small fraction of sulfur dioxide in the flue gas to SO3. The extent of this oxidation depends on the catalyst formulation and SCR operating conditions. Gas-phase SO3 and sulfuric acid, on being quenched in plant equipment (e.g., air preheater and wet scrubber), result in fine acidic mist, which can cause increased plume opacity and undesirable emissions. Recently, such effects have been observed at plants firing high-S coal and equipped with SCR systems and wet scrubbers. This paper investigates the factors that affect acidic mist production in coal-fired electric utility boilers and discusses approaches for mitigating emission of this mist.     

A model for the maximum credible hourly impact on any ground receptor from point sources with thermal plume rise

A pollutant dispersion model is developed, allowing fast evaluation of the maximum credible 1-h average concentration on any given ground-level receptor, along with the corresponding critical meteorological conditions (wind speed and stability class) for stacks with buoyant plumes in urban or rural areas. Site-specific meteorological data are not required, as the computed concentrations are maximized against all credible combinations of wind speed, stability class, and mixing height. The analysis is based on the dispersion relations of Pasquill-Gifford and Briggs for rural and urban settings, respectively, the buoyancy induced dispersion correlation of Pasquill, the wind profile exponent values suggested by Irwin, the buoyant plume rise relations of Briggs, as well as the Benkley and Schulman's model for the minimum mixing heights. The model is particularly suited for air pollution management studies, as it allows fast screening of the maximum impact on any selected receptor and evaluation of the ways to have this impact reduced. It is also suited for regulatory purposes, as it can be used to define the minimum stack size requirements for a given source as a function of the exit gas volume and temperature, the pollutant emission rates and their hourly concentration standards, as well as the source location relative to sensitive receptors.     

Simulation of stack plume opacity

The visual impact of primary particles emitted from stacks is regulated according to stack opacity criteria. In-stack monitoring of the flue gas opacity allows plant operators to ensure that the plant meets U.S. Environmental Protection Agency opacity regulations. However, the emission of condensable gases such as SO3 (that hydrolyzes to H2SO4), HCl, and NH3, which may lead to particle formation after their release from the stack, makes the prediction of stack plume opacity more difficult. We present here a computer simulation model that calculates the opacity due to both primary particles emitted from the stack and secondary particles formed in the atmosphere after the release of condensable gases from the stack. A comprehensive treatment of the plume rise due to buoyancy and momentum is used to calculate the location at which the condensed water plume has evaporated (i.e., where opacity regulations apply). Conversion of H2SO4 to particulate sulfate occurs through nucleation and condensation on primary particles. A thermodynamic aerosol equilibrium model is used to calculate the amount of ammonium, chloride, and water present in the particulate phase with the condensed sulfate. The model calculates the stack plume opacity due to both primary and secondary particles. Examples of model simulations are presented for three scenarios that differ by the emission control equipment installed at the power plant: (1) electrostatic precipitators (ESP), (2) ESP and flue gas desulfurization, and (3) ESP and selective catalytic reduction. The calculated opacity is most sensitive to the primary particulate emissions. For the conditions considered here, SO3 emissions showed only a small effect, except if one assumes that most H2SO4 condenses on primary particles. Condensation of NH4Cl occurs only at high NH3 emission rates (about 25 ppm stack concentration).     

Rates of Conversion of Sulfur Dioxide to Sulfate in a Scrubbed Power Plant Plume

ABSTRACT

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 NO_y emissions into the plume has been reduced to ~0.1, compared with a prescrubber value of ~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 post-scrubber 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.     

Lidar Observations of the Diurnal Behavior of the Cumberland Power Plant Plume

Mobile lidar observations were made downwind of TVA’s Cumberland (Tennessee) power plant as part of the STATE (Sulfur Transport and Transformation in the Environment) program. Vertical profiles of aerosol backscatter have been processed and displayed to show plume structure as an intensity-modulated TV presentation. Available meteorological data, especially the pilot balloon and radiosonde measurements collected during the STATE experiment, have been used to aid in the interpretation of the lidar display. The data show: ? Well defined nighttime plumes, which often tilt or display a layered structure in the shape of a “>”.

? Late morning convective breakup of the plume.

? Well mixed convective plumes during the day.

? Reformation of the layered nighttime plume during the late afternoon.

It appears that the nighttime plume behavior can be related qualitatively to the strong directional shear of the wind with height that often accompanies the stable nighttime atmosphere. The nighttime plume shapes frequently differ markedly from the oval shape one expects of a gaussian plume. Daytime plumes are in better conformance to the expected shape except when constricted by the surface or the top of the mixing layer     

Volatile nanoparticle formation and growth within a diluting diesel car exhaust

A major source of particle number emissions is road traffic. However, scientific knowledge concerning secondary particle formation and growth of ultrafine particles within vehicle exhaust plumes is still very limited. Volatile nanoparticle formation and subsequent growth conditions were analyzed here to gain a better understanding of "real-world" dilution conditions. Coupled computational fluid dynamics and aerosol microphysics models together with measured size distributions within the exhaust plume of a diesel car were used. The impact of soot particles on nucleation, acting as a condensational sink, and the possible role of low-volatile organic components in growth were assessed. A prescribed reduction of soot particle emissions by 2 orders of magnitude (to capture the effect of a diesel particle filter) resulted in concentrations of nucleation-mode particles within the exhaust plume that were approximately 1 order of magnitude larger. Simulations for simplified sulfuric acid-water vapor gas-oil containing nucleation-mode particles show that the largest particle growth is located in a recirculation zone in the wake of the car. Growth of particles within the vehicle exhaust plume up to detectable size depends crucially on the relationship between the mass rate of gaseous precursor emissions and rapid dilution. Chassis dynamometer measurements indicate that emissions of possible hydrocarbon precursors are significantly enhanced under high engine load conditions and high engine speed. On the basis of results obtained for a diesel passenger car, the contributions from light diesel vehicles to the observed abundance of measured nucleation-mode particles near busy roads might be attributable to the impact of two different time scales: (1) a short one within the plume, marked by sufficient precursor emissions and rapid dilution; and (2) a second and comparatively long time scale resulting from the mix of different precursor sources and the impact of atmospheric chemistry.     

Application of Airborne Lidar in Particulate Air Quality Problem Delineation,Monitoring Network Design and Control Strategy Development

Airborne lidar (light detection and ranging) data were collected during two field programs in 1989 in the border metropolitan area comprising El Paso (U.S.) and Ciudad Juarez (Mexico). These data were utilized to provide estimates of suspended particulate distributions in the presence of historical data with limited spatial and temporal density in the U.S. and almost no historical data in Mexico. The resulting information was used to help ascertain the magnitude and spatial extent of the particulate air quality problem and to help determine the number and disposition of recommended permanent particulate monitors in the area. The results support the hypothesis that, given a few representative measurements for calibration, airborne lidar might be used in specific situations to develop detailed concentration patterns and to provide useful estimates of pollutant flux, when combined with appropriate measurements of wind velocity profiles. Such information, in turn, should be useful for the development of control strategies for potential alleviation of particulate air quality problems.     

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.     

Modeling of potential power plant plume impacts on Dallas-Fort Worth visibility

During wintertime, haze episodes occur in the Dallas-Ft. Worth (DFW) urban area. Such episodes are characterized by substantial light scattering by particles and relatively low absorption, leading to so-called "white haze." The objective of this work was to assess whether reductions in the emissions of SO2 from specific coal-fired power plants located over 100 km from DFW could lead to a discernible change in the DFW white haze. To that end, the transport, dispersion, deposition, and chemistry of the plume of a major power plant were simulated using a reactive plume model (ROME). The realism of the plume model simulations was tested by comparing model calculations of plume concentrations with aircraft data of SF6 tracer concentrations and ozone concentrations. A second-order closure dispersion algorithm was shown to perform better than a first-order closure algorithm and the empirical Pasquill-Gifford-Turner algorithm. For plume impact assessment, three actual scenarios were simulated, two with clear-sky conditions and one with the presence of fog prior to the haze. The largest amount of sulfate formation was obtained for the fog episode. Therefore, a hypothetical scenario was constructed using the meteorological conditions of the fog episode with input data values adjusted to be more conducive to sulfate formation. The results of the simulations suggest that reductions in the power plant emissions lead to less than proportional reductions in sulfate concentrations in DFW for the fog scenario. Calculations of the associated effects on light scattering using Mie theory suggest that reduction in total (plume + ambient) light extinction of less than 13% would be obtained with a 44% reduction in emissions of SO2 from the modeled power plant.     

Analysis of air quality observations with the aid of the source-receptor relationship approach

In this study, an attempt was made to analyze time series of air quality measurements (O3, SO2, SO4(2-), NOx) conducted at a remote place in the eastern Mediterranean (Finokalia at Crete Island in 1999) to obtain concrete information on potential contributions from emission sources. For the definition of a source-receptor relationship, advanced meteorological and dispersion models appropriate to identify "areas of influence" have been used. The model tools used are the Regional Atmospheric Modeling System and the Lagrangian-type particle dispersion model (forward and backward in time), with capabilities to derive influence functions and definition of "areas of influence." When high levels of pollutants have been measured at the remote location of Finokalia, particles are released from this location (receptor) and traced backward in time. The influence function derived from particle distributions characterizes dispersion conditions in the atmosphere and also provides information on potential contributions from emission sources within the modeling domain to this high concentration. As was shown in the simulation results, the experimental site of Finokalia in Crete is influenced during the selected case studies, primarily by pollutants emitted from the urban conglomerate of Athens. Secondarily, it is influenced by polluted air masses arriving from Italy and/or the Black Sea Region. For some specific cases, air pollutants monitored at Finokalia were possibly related to war activities in the West Balkan Region (Kosovo).     

The evolution of particles in the plume from a large coal-fired boiler with flue gas desulfurization

Airborne measurements were made of gaseous and particulate species in the plume of a large coal-fired power plant after flue gas desulfurization (FGD) controls were installed. These measurements were compared with measurements made before the controls were installed. The light scattering and number and volume distributions of plume excess particles were determined by nephelometry and optical particle counting techniques. The plume impact based on optical techniques was much lower than that observed in earlier measurements. Indeed, plume excess volumes as a function of particle size were of the same magnitude as the variability of the background volume distribution. In situ excess plume scattering actually decreased with distance from the source, in contrast to pre-FGD conditions. The upper limit for the dry rate of SO2-to-SO4(2-) conversion was estimated from plume excess volume measurements to be about 4% hr-1. This is slightly greater than the upper limit, 3.5% hr-1, estimated by earlier researchers, but the same as that estimated using the present technique with the earlier data. The cross-plume profile of volume suggests SO2-to-SO4(2-) conversion is highest at the plume edges. The greatest benefit of SO2 reduction on plume excess volume and visibility appears to occur far down-wind of the source.     

Screening and Scenarios of Traffic Emissions at Trier,Germany

SCOPE AND BACKGROUND: In the course of the European Council Directive on permissible air pollutant limit values, valid starting from 2005 there is an urgent call for action, particularly for fine dust (PM10). Current investigations (Junk & Helbig 2003, Reuter & Baumüller 2003) show that the limit values in certain places in congested areas are exceeded. Only if it is possible to locate these Hot Spots purposeful measures to reduce the ambient air pollution can be conducted. For an efficient identification of these Hot Spots numerical computer models or establishing special measurements networks are too expensive. Using the statistical model STREET 5.0 (KTT 2003) a cost-effective screening of the air pollution situation caused by the traffic can be done. METHODS: STREET is based on the 3-dimensional micro-scale non-hydrostatic flow- and dispersion model MISCAM (Eichhorn 1989). The results of over 100.000 different calculations with MISCAM are stored in a Database and used to calculate the emissions with STREET. In collaboration with the city council of Trier more than 150 streets were investigated, mapped, and calculated. A special urban climate measuring network supplies the necessary meteorological input data about the wind field and precipitation events in the valley of the Moselle. Information about road width and road orientation as well as building density was derived from aerial photographs. Traffic censuses and mobile air pollutants measurements supplied the remaining input data. We calculated the mean annual air pollutant concentrations for NO2, CO, SO2, O3, benzene as well as PM10. RESULTS: A comparison of the model results with the values obtained from the stations of the central emission measuring network of Rhineland-Palatinate (ZIMEN, annual report 2002) shows very good agreements. The model was not only used to calculate the annual air pollutant but also for urban planning and management. The absolute level of the air pollutant is mainly dependent on the amount of traffic in the street canyons. Therefore four different case-scenarios with varying quantity of traffic were calculated and interpreted for each street. The results of the calculation show that on the basis of the mean values for both NO2 and benzene, it is not to be expected that the limits PERSPECTIVES: Furthermore the model can be used to find the maximum tolerable numbers of cars for a street without exceeding the air pollutant thresholds.     

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.     

Correlating emissions with time and temperature to predict worst-case emissions from open liquid area sources

The two primary factors influencing ambient air pollutant concentrations are emission rate and dispersion rate. Gaussian dispersion modeling studies for odors, and often other air pollutants, vary dispersion rates using hourly meteorological data. However, emission rates are typically held constant, based on one measured value. Using constant emission rates can be especially inaccurate for open liquid area sources, like wastewater treatment plant units, which have greater emissions during warmer weather, when volatilization and biological activity increase. If emission rates for a wastewater odor study are measured on a cooler day and input directly into a dispersion model as constant values, odor impact will likely be underestimated. Unfortunately, because of project schedules, not all emissions sampling from open liquid area sources can be conducted under worst-case summertime conditions. To address this problem, this paper presents a method of varying emission rates based on temperature and time of the day to predict worst-case emissions. Emissions are varied as a linear function of temperature, according to Henry's law, and a tenth order polynomial function of time. Equation coefficients are developed for a specific area source using concentration and temperature measurements, captured over a multiday period using a data-logging monitor. As a test case, time/temperature concentration correlation coefficients were estimated from field measurements of hydrogen sulfide (H2S) at the Rowlett Creek Wastewater Treatment Plant in Garland, TX. The correlations were then used to scale a flux chamber emission rate measurement according to hourly readings of time and temperature, to create an hourly emission rate file for input to the dispersion model ISCST3. ISCST3 was then used to predict hourly atmospheric concentrations of H2S. With emission rates varying hourly, ISCST3 predicted 384 acres of odor impact, compared with 103 acres for constant emissions. Because field sampling had been conducted on relatively cool days (85-90 degrees F), the constant emission rate underestimated odor impact significantly (by 73%).     

Split-level Plumes

Two recent power plant plume studies by mobile, ground-based and airborne lidar have recorded cross-section images of plumes with sharply-defined layered and connected bands of aerosol in the vertical. Of the external parameters considered, wind direction and speed changes in the vertical were found to be associated most with these plume types. Statistical analyses indicate that both direction and speed shear are highly correlated with the layered plumes.