Water tank measurements of buoyant plume rise and structure in neutral crossflows

In this paper, an experimental study of the rise and development of a single buoyant plume and a pair of in-line buoyant plumes is presented. The investigations were carried out at small scale in a water filled towing tank using both quantitative flow visualisation and local concentration measurements. The measured plume trajectories for a single plume were compared with the Briggs plume rise equation and predictions from a numerical integral model. Plume trajectories were studied for twin in-line plumes, with particular attention to changes in the plume trajectory, especially any additional rise that resulted from the interaction between the two plumes. Concentration field distributions in cross-sections through both single and interacting twin plumes were obtained from the local concentration measurement system. These showed how the interaction affected the plume structure, notably the double vortex system that occurs in a fully developed plume.     

Comparison of the industrial source complex and AERMOD dispersion models: case study for human health risk assessment

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.     

Ground-based remote sensing measurements of aerosol and ozone in an urban area: A case study of mixing height evolution and its effect on ground-level ozone concentrations

We have estimated the mixing height (MH) and investigated the relationship between vertical mixing and ground-level ozone concentrations in Seoul, Korea, by using three ground-based active remote sensing instruments operating side by side: micro-pulse lidar (MPL), differential absorption lidar (DIAL), and differential optical absorption spectroscopy (DOAS). The MH is estimated from MPL measurements of aerosol extinction profiles by the gradient method under convective conditions. Comparisons of the MHs estimated from MPL and radiosonde measurements show a good agreement (r²=0.99). Continuous MPL measurements with high temporal and vertical resolution reveal the diurnal variations of the MH under convective conditions and the presence of a residual layer during the nighttime. Comprehensive measurements of ozone and aerosol by MPL, DIAL and DOAS during an high ozone episode (24–26 May 2000) in Seoul, Korea, reveal that (1) photochemical ozone production and advection from upwind regions (the western part of Seoul) contribute two peaks of ozone concentrations at the ground around 14:00 and 18:00 local time on 25 May 2000, respectively, and (2) the entrainment and the fumigation processes of ozone aloft in the nighttime residual layer into the ground is a major contributor of high concentrations of ground-level ozone observed on the following day (26 May 2000).     

An Inversion Algorithm for Determining Area-Source Emissions from Downwind Concentration Measurements

Measuring emissions from nonuniform area sources, such as waste repository sites, has been a difficult problem. A simple but reliable method is not available. An objective method of inverting downwind concentration measurements, utilizing an assumed form of atmospheric dispersion to reconstruct total emission rate and distribution, is described in this study. The Gaussian dispersion model is compared to a more realistic model based on K-theory and similarity expressions. A sensitivity analysis is presented indicating the atmospheric conditions under which a successful application of the method could be anticipated. Field releases of sulfur hexaf luoride (SF₆) from a simulated area source in flat terrain were conducted to check the method,ability to reconstruct source distribution, and total emission rate. The sensitivity analysis and the field study confirm that a few ground-level concentration measurements and a simple determination of the atmospheric dispersion characteristics are sufficient, under neutral to stable conditions, to obtain the total emission rate accurately. Reconstruction of the spatial pattern of the source is possible by utilizing concentration information from samplers located on two separate ground-level receptor lines, if a shift in the wind direction occurs and if it can be assumed that the total emission rate is time invariant. A method of cross-checking the accuracy of the reconstruction, using a simultaneous tracer release, is presented.     

Fumigation of pollutants in and above the entrainment zone into a growing convective boundary layer: a large-eddy simulation

Fumigation of a passive plume located in or above the entrainment zone (EZ) into a growing convective boundary layer (CBL) has been simulated by large-eddy simulation (LES). Three non-dimensional parameters, α(=w_e0/w_*0), z₀/z_i0, and σ_z0/z_i0, are used to classify different cases, where w_*0 is the convective velocity scale, w_e0 the initial entrainment velocity, z_i0 the initial CBL height, z₀ the initial plume height, and σ_z0 is the initial plume half-depth. Forty cases have been run and analysed. The crosswind-integrated concentrations have been compared with existing laboratory data from a saline convection tank. The results show that LES is a promising tool to reproduce fumigation processes. With a relatively coarse grid mesh near the EZ, LES derives reliable results that are in a good agreement with the laboratory data. The first parameter, α, containing the effects due to inversion strength, plays an important role in determining C₀(T), the ground-level concentration (GLC) as a function of dimensionless time, T. For large α (say >0.03, corresponding to fast entrainment), variation of α gives significant change in C₀(T); whereas for a wide range of α between 0.01 and 0.02 (corresponding to slow entrainment), C₀(T) is almost independent of α. The starting time of fumigation does not vary significantly with the second parameter, z₀/z_i0 (relative height of plume), although C₀(T) is, in general, smaller for a higher plume. This confirms laboratory findings that the traditional notion of zero fumigation for a high plume (say above 1.10z_i) is not correct. The effect of the third parameter, σ_z0/z_i0, is on the magnitude of C₀(T); thinner initial plumes have higher GLCs.     

COMPLEX I and II Model Performance Evaluation in Nevada and New Mexico

The COMPLEX I and COMPLEX II Gaussian dispersion models for complex terrain applications have been made available by EPA. Various terrain treatment options under IOPT(25) can be selected for a particular application, one of which [IOPT(25) = 1] is an algorithm similar to that of the VALLEY model. A model performance evaluation exercise involving three of the available options with both COMPLEX models was carried out using SF⁶ tracer measurements taken during worst-case stable impaction conditions in complex terrain at the Harry Allen Plant site in southern Nevada. The models did not reproduce observed concentrations on an event by event basis, as correlation coefficients for 1-h concentrations of 0-0.3 were exhibited. When observed and calculated cumulative frequency distributions for 1-h and 3-h concentrations were compared, a close correspondence between observations and concentrations calculated with COMPLEX I, IOPT(25) = 2 or 3 was noted; both options consistently overestimated observed concentrations. With IOPT(25) = 1, upper percentile (maximum) values in the calculated frequency distribution exceeded the corresponding IOPT(25) = 2 or 3 value by roughly a factor of 2, and observed values by 2.5-5. COMPLEX II typically produced maximum values 2-4 times as great as COMPLEX I for the same terrain treatment option. From these results it is concluded that: 1) the physically unrealistic sector-spread approach used in VALLEY and COMPLEX I under stable impaction conditions is a surrogate for wind direction variation, and 2) the doubling of the plume centerline concentration due to ground reflection under terrain impingement conditions that is included in IOPT(25) = 1 is inappropriate.

These findings were found to be consistent with an analysis of noncurrent observed and calculated SO₂ χ/Q frequency distributions for 1, 3, and 24 hours near the Four Corners Plant in New Mexico. The comparison involved a four-year calculated χ/Q data set and a two-year observed χ/Q data set at the worst-case high terrain impact location near the plant.     

Effect of Refractory on the Thermal Stability of SF6

The thermal decomposition of SF₆ is known to be oxygen-independent. Nevertheless, because of its high stability, the use of SF6 as a "conservative" surrogate in incinerator performance evaluation has been advocated and researched. This paper shows that refractory decreases markedly the stability of SF₆. The resulting increase in SF₆ decomposition was from 0 percent to 95 percent at 900°C, and the temperatures at which 90-99 percent decomposition occurred were lowered by 300-150°C. Refractory also decreased the stability of CCl₄ and C₂Cl₄, but to a lesser extent. The difference between the decompositions of C₂Cl₄ and SF₆ was reduced from several orders of magnitude to a factor of 2-4. Such a drastic and adverse change in relative stability could render SF₆ unsuitable as a "conservative" surrogate. The requirements for a "conservative" surrogate and the need for caution in its use are discussed, and further research areas are indicated.     

Principal Plume Dispersion Models: TVA Power Plants

The body of information presented in this paper is directed to those individuals who may be concerned with principal plume dispersion models at coal-burning power plants. About 20 years of comprehensive field surveillance and documentation of dispersion of power plant emissions for a varied range of unit sizes, stack heights, and meteorological conditions have determined the Tennessee Valley Authority’s interpretation of principal plume dispersion models. TVA’s experience indicates that as unit sizes are increased and taller stacks are constructed, the plume dispersion model associated with maximum surface concentrations changes. Maximum surface concentrations for principal plume dispersion models were approximately equal for the early small plants. However, the coning model was considered the critical plume dispersion model because the frequency of recurrence of surface concentrations from this model was appreciably greater than other models.

There were progressive changes because of an increase in unit sizes and stack heights; the magnitude of maximum surface concentrations from the coning model decreased, and the magnitude (relative to the coning model) of concentrations from the inversion breakup model increased. However, with plumes from newer and larger units with higher stacks, the trapping dispersion model became prominent. Finally, by the time unit size had increased to 900 mw and stack height to about 245 meters, as at Bull Run Power Plant, the magnitude of surface concentrations associated with trapping had increased to such a degree that it became the critical dispersion model identified with power plants of this size.     

The evolution of photochemical smog in a power plant plume

The evolution of photochemical smog in a plant plume was investigated with the aid of an instrumented helicopter. Air samples were taken in the plume of the Cumberland Power Plant, located in central Tennessee, during the afternoon of 16 July 1995 as part of the Southern Oxidants Study – Nashville Middle Tennessee Ozone Study. Twelve cross-wind air sampling traverses were made at six distance groups from 35 to 116 km from the source. During the sampling period the winds were from the west–northwest and the plume drifted towards the city of Nashville TN. Ten of the traverses were made upwind of the city, where the power plant plume was isolated, and two traverses downwind of the city when the plumes were possibly mixed. The results revealed that even six hours after the release, excess ozone production was limited to the edges of the plume. Only when the plume was sufficiently dispersed, but still upwind of Nashville, was excess ozone (up to 109 ppbv, 50–60 ppbv above background levels) produced in the center of the plume. The concentrations image of the plume and a Lagrangian particle model suggests that portions of the power plant plume mixed with the urban plume. The mixed urban power plant plume began to regenerate O₃ that peaked at 120 ppbv at a short distance (15–25 km) downwind of Nashville. Ozone productivity (the ratio of excess O₃ to NO_y and NO_z) in the isolated plume was significantly lower compared with that found in the city plume. The production of nitrate, a chain termination product, was significantly higher in the power plant plume compared to the mixed plume, indicating shorter chain length of the photochemical smog chain reaction mechanism.     

Integrating lidar and satellite optical depth with ambient monitoring for 3-dimensional particulate characterization

A combination of in-situ PM_2.5, sunphotometers, upward pointing lidar and satellite aerosol optical depth (AOD) instruments have been employed to better understand variability in the correlation between AOD and PM_2.5 at the surface. Previous studies have shown good correlation between these measures, especially in the US east, and encouraged the use of satellite data for spatially interpolating between ground sensors. This work shows that cases of weak correlation can be better understood with knowledge of whether the aerosol is confined to the surface planetary boundary layer (PBL) or aloft. Lidar apportionment of the fraction of aerosol optical depth that is within the PBL can be scaled to give better agreement with surface PM_2.5 than does the total column amount. The study has shown that lidar combined with surface and remotely sensed data might be strategically used to improve our understanding of long-range or regionally transported pollutants in multiple dimensions.     

Abatement of Sulfur Hexafluoride Emissions from the Semiconductor Manufacturing Process by Atmospheric-Pressure Plasmas

Abstract

Sulfur hexafluoride (SF₆) is an important gas for plasma etching processes in the semiconductor industry. SF₆ intensely absorbs infrared radiation and, consequently, aggravates global warming. This study investigates SF₆ abatement by nonthermal plasma technologies under atmospheric pressure. Two kinds of nonthermal plasma processes—dielectric barrier discharge (DBD) and combined plasma catalysis (CPC)—were employed and evaluated. Experimental results indicated that as much as 91% of SF₆ was removed with DBDs at 20 kV of applied voltage and 150 Hz of discharge frequency for the gas stream containing 300 ppm SF₆, 12% oxygen (O₂), and 40% argon (Ar), with nitrogen (N₂) as the carrier gas. Four additives, including Ar, O₂, ethylene (C₂H₄), and H₂O_(g), are effective in enhancing SF₆ abatement in the range of conditions studied. DBD achieves a higher SF₆ removal efficiency than does CPC at the same operation condition. But CPC achieves a higher electrical energy utilization compared with DBD. However, poisoning of catalysts by sulfur (S)-containing species needs further investigation. SF₆ is mainly converted to SOF₂,SO₂F₄, sulfur dioxide (SO₂), oxygen difluoride (OF₂), and fluoride (F₂). They do not cause global warming and can be captured by either wet scrubbing or adsorption. This study indicates that DBD and CPC are feasible control technologies for reducing SF₆ emissions.     

Impact of the mixing boundary layer on the relationship between PM2.5 and aerosol optical thickness

The purpose of this paper is to study the relationship between columnar aerosol optical thickness and ground-level aerosol mass. A set of Sun photometer, elastic backscattering lidar and TEOM measurements were acquired during April 2007 in Lille, France. The PM2.5 in the mixed boundary layer is estimated using the lidar signal, aerosol optical thickness, or columnar integrated Sun photometer size distribution and compared to the ground-level station measurements. The lidar signal recorded in the lowest level (240 m) is well correlated to the PM2.5 (R² = 0.84). We also show that the correlation between AOT-derived and measured PM2.5 is significantly improved when considering the mixed boundary layer height derived from the lidar. The use of the Sun photometer aerosol fine fraction volume does not improve the correlation.     

A multi-layer model for pollutant dispersion with dry deposition to the ground

This paper presents a semi-analytical solution for the steady advection–diffusion equation that allows simulating the vertical turbulent dispersion of air pollution with deposition to the ground. The performances of the solution, with a proper parameterization of the vertical profiles of wind and eddy diffusivity, were evaluated against Hanford diffusion experiment dataset using two tracers (Doran and Horst, 1985): a non-depositing gas (SF₆) and depositing particles (ZnS). Results show that the dispersion model with the K-parameterization included produces a good fitting of the measured ground-level concentration data and there are no big differences between the parameterizations taken from literature. A comparison with other models was shown and discussed.     

Modeling of Potential Power Plant Plume Impacts on Dallas-Fort Worth Visibility

ABSTRACT

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.     

Dissociation of Sulfur Hexafluoride Tracer Gas in the Presence of an Indoor Combustion Source

ABSTRACT

As an odorless, nontoxic, and inert compound, sulfur hexafluoride (SF₆) is one of the most widely used tracer gases in indoor air quality studies in both controlled and uncontrolled environments. This compound may be subject to reactions with water vapor under elevated temperature to form acidic inorganic compounds such as HF and H₂SO₄. Thus, in the presence of unvented combustion sources such as kerosene heaters, natural gas heaters, gas log fireplaces, candles, and lamps, the SF₆ dissociation may interfere with measurements of the emissions from these sources. Tests were conducted in a research house with a vent-free natural gas heater to investigate these potential interferences. It was observed that the heater operation caused about a 5% reduction of SF₆ concentration, which can be an error source for the ventilation rate measurement and consequently the estimated pollutant emission rates. Further analysis indicates that this error can be much greater than the observed 5% under certain test conditions because it is a function of the ventilation flow rate. Reducing the tracer gas concentration has no effect on this error. A simple theoretical model is proposed to estimate the magnitude of this error.

The second type of interference comes from the primary and secondary products of the SF₆ dissociation, mainly H₂SO₄, SO₂, HF, and fine particulate matter (PM). In the presence of ~5 ppm SF₆, the total airborne concentrations of these species increased by a factor of 4-10. The tests were performed at relatively high SF₆ concentrations, which is necessary to determine the interferences quantitatively. The second type of interference can be significantly reduced if the SF₆ concentration is kept at a low ppb level.     

Modelling pollutants dispersion and plume rise from large hydrocarbon tank fires in neutrally stratified atmosphere

Petrochemical industries normally use storage tanks containing large amounts of flammable and hazardous substances. Therefore, the occurrence of a tank fire, such as the large industrial accident on 11th December 2005 at Buncefield Oil Storage Depots, is possible and usually leads to fire and explosions. Experience has shown that the continuous production of black smoke from these fires due to the toxic gases from the combustion process, presents a potential environmental and health problem that is difficult to assess. The goals of the present effort are to estimate the height of the smoke plume, the ground-level concentrations of the toxic pollutants (smoke, SO₂, CO, PAHs, VOCs) and to characterize risk zones by comparing the ground-level concentrations with existing safety limits. For the application of the numerical procedure developed, an external floating-roof tank has been selected with dimensions of 85 m diameter and 20 m height. Results are presented and discussed. It is concluded that for all scenarios considered, the ground-level concentrations of smoke, SO₂, CO, PAHs and VOCs do not exceed the safety limit of IDLH and there are no “death zones” due to the pollutant concentrations.     

Decomposition of SF6 in an RF Plasma Environment

Abstract

Sulfur hexafluoride (SF₆)-contained gas is a common pollutant emitted during the etching process used in the semiconductor industry. This study demonstrated the application of radio-frequency (RF) plasma in the decomposition of SF₆. The decomposition fraction of SF₆ [η_SF6 (C_in–C_out)/C_in x 100%] and the mole fraction profile of the products were investigated as functions of input power and feed O₂/SF₆ ratio in an SiO₂ reactor. The species detected in both SF₆/Ar and SF₆/O₂/Ar RF plasmas were SiF₄, SO₂, F₂, SO₂F₂, SOF₂, SOF₄, S₂F₁₀, S₂OF₁₀, S₂O₂F₁₀, and SF₄. The results revealed that at 40 W, η_SF6 exceeded 99%, and the reaction products were almost all converted into stable compounds such as SiF₄, SO₂, and F₂ with or without the addition of oxygen. Sulfur oxyfluorides such as SO₂F₂, SOF₂, SOF₄, S₂OF₁₀, and S₂O₂F₁₀ were produced only below 40 W. The results of this work can be used to design a plasma/chemical system for online use in a series of a manufacturing process to treat SF₆-containing exhaust gases.     

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.     

Modeling and monitoring of CO,NO and NO2 in a modern townhouse

Mass-balance models for indoor concentrations of CO, NO and NO₂ were applied to an energy-efficient townhouse. Model parameters included source emission rates, infiltrating airflows, and, for NO₂, loss rate coefficients. Emission factors for CO, NO and NO₂ were estimated for each of the gas-fired appliances in the house. Airflows were estimated using sulfur hexafluoride (SF₆) decay techniques. Loss rates for NO₂ were calculated as the difference between NO₂ removal rates and estimated air exchange rates; CO and NO concentrations decayed at a rate not significantly different than that for SF₆. Comparing model predictions with measured concentrations yielded differences averaging 17% for CO and NO, and 28% for NO₂.     

Predictions of Maximum Ground-Level H2S Concentrations Resulting from Two Sour Gas Well Blowouts

Alberta has recently experienced two sour gas well blowouts: Lodgepole and Claresholm. Sulphur emissions associated with the blowouts were about 1400 and 2 tonnes per day, respectively. The Lodgepole blowout was not only of much greater magnitude but also lasted significantly longer than the Claresholm blowout (67 vs. 4 days). Special air quality monitoring with respect to H₂S was conducted to assess impacts of the blowouts. Monitoring was especially extensive for the Lodgepole incident. Maximum observed ground-level H₂S concentrations were compared to predictions obtained using a Gaussian model which makes allowance for the effects of sonic exit velocity on plume spread and the effects of wind shear on plume transport. There was appreciable agreement between predicted and observed values.