Aerosol entrainment from a sparged non-Newtonian slurry

Previous bench-scale experiments have provided data necessary for the development of empirical models that describe aerosol entrainment from bubble bursting. However, previous work has not been extended to non-Newtonian liquid slurries. Design of a waste treatment plant on the Hanford Site in Washington required an evaluation of the applicability of these models outside of their intended range. For this evaluation, aerosol measurements were conducted above an air-sparged mixing tank filled with simulated waste slurry possessing Bingham plastic rheological properties. Three aerosol-size fractions were measured at three sampling heights and for three different sparging rates. The measured entrainment was compared with entrainment models. One model developed based on bench-scale air-water experiments agreed well with measured entrainment. Another model did not agree well with the measured entrainment. It appeared that the source of discrepancy between measured and modeled entrainment stemmed from application beyond the range of data used to develop the model. A possible separation in entrainment coefficients between air-water and steam-water systems was identified. A third entrainment model was adapted to match experimental conditions and fit a posteri to the experimental data, resulting in a modified version that resulted in estimated entrainment rates similar to the first model.     

Analysis and Simulation of Wintertime Light Scattering by the Urban Aerosol in Dallas-Fort Worth

ABSTRACT

Wintertime atmospheric light scattering in Dallas, TX, was estimated through the use of aerosol models. Input data for the aerosol models were provided by measurements of aerosol chemistry, physical particle size distributions, and distributions of particulate sulfur by particle size, and by predictions by an atmospheric simulation model. Light scattering measurements provided a basis for testing the aerosol models. The SCAPE thermodynamic equilibrium model was used to estimate the amount of liquid water associated with particles and the ELSIE Mie scattering model was applied to estimate the resulting light scattering. The calculations were based on aerosol properties measured in Dallas during December 1994 and February 1995, and changes in scattering due to hypothetical changes in the aerosol were predicted. The predicted light scattering was compared to scattering measured by an Optec nephelom-eter; agreement was within 20% in every case.     

Optical Measurements of Aerosol Size Distributions in Great Smoky Mountains National Park: Dry Aerosol Characterization

ABSTRACT

Aerosol size distributions were measured during the summertime 1995 Southeastern Aerosol and Visibility Study (SEAVS) in Great Smoky Mountains National Park using an Active Scattering Aerosol Spectrometer (ASASP-X) optical particle counter. We present an overview of the experimental method, our data inversion technique, timelines of the size distribution parameters, and calculations of dry accumulation mode aerosol density and refractive index. Aerosol size distributions were recorded during daylight hours for aerosol in the size range 0.1 < Dp < 2.5 u,m. The particle refractive index used for the data inversion was calculated with the partial molar refractive index approach using 12-hr measured aerosol chemical composition. Aerosol accumulation mode volume concentrations ranging from 1 to 26 u,m³ cm^-3 were observed, with an average of 7 ± 5 u,m³ cm^-3. The study average dry accumulation mode geometric volume median diameter was 0.27 ± 0.03 u,m, and the mean geometric standard deviation was 1.45 ± 0.06. Using an internally mixed aerosol model, and assuming chemical homogeneity across the measured particle distribution, an average accumulation mode dry sulfate ion mass scattering efficiency of 3.8 ± 0.6 m² g^-1 was calculated.     

Processes Influencing Secondary Aerosol Formation in the San Joaquin Valley during Winter

Abstract

Air quality data collected in the California Regional PM₁₀/PM_2.5 Air Quality Study (CRPAQS) are analyzed to qualitatively assess the processes affecting secondary aerosol formation in the San Joaquin Valley (SJV). This region experiences some of the highest fine particulate matter (PM_2.5) mass concentrations in California (≤188 μg/m³ 24-hr average), and secondary aerosol components (as a group) frequently constitute over half of the fine aerosol mass in winter. The analyses are based on 15 days of high-frequency filter and canister measurements and several months of wintertime continuous gas and aerosol measurements. The phase-partitioning of nitrogen oxide (NO_x)-related nitrogen species and carbonaceous species shows that concentrations of gaseous precursor species are far more abundant than measured secondary aerosol nitrate or estimated secondary organic aerosols. Comparisons of ammonia and nitric acid concentrations indicate that ammonium nitrate formation is limited by the availability of nitric acid rather than ammonia. Time-resolved aerosol nitrate data collected at the surface and on a 90-m tower suggest that both the daytime and nighttime nitric acid formation pathways are active, and entrainment of aerosol nitrate formed aloft at night may explain the spatial homogeneity of nitrate in the SJV. NO_x and volatile organic compound (VOC) emissions plus background O₃ levels are expected to determine NO_x oxidation and nitric acid production rates, which currently control the ammonium nitrate levels in the SJV. Secondary organic aerosol formation is significant in winter, especially in the Fresno urban area. Formation of secondary organic aerosol is more likely limited by the rate of VOC oxidation than the availability of VOC precursors in winter.     

Analysis and simulation of wintertime light scattering by the urban aerosol in Dallas-Fort Worth

Wintertime atmospheric light scattering in Dallas, TX, was estimated through the use of aerosol models. Input data for the aerosol models were provided by measurements of aerosol chemistry, physical particle size distributions, and distributions of particulate sulfur by particle size, and by predictions by an atmospheric simulation model. Light scattering measurements provided a basis for testing the aerosol models. The SCAPE thermodynamic equilibrium model was used to estimate the amount of liquid water associated with particles and the ELSIE Mie scattering model was applied to estimate the resulting light scattering. The calculations were based on aerosol properties measured in Dallas during December 1994 and February 1995, and changes in scattering due to hypothetical changes in the aerosol were predicted. The predicted light scattering was compared to scattering measured by an Optec nephelometer; agreement was within 20% in every case.     

Transport of Escherichia coli through variably saturated sand columns and modeling approaches

A sand column leaching system with well-controlled suction and flow rate was built to investigate the effects on bacterial transport of air-water interface effects (AWI) correlated to water content, particle size, and column length. Adsorption of Escherichia coli strain D to silica sands was measured in batch tests. The average % adsorption for coarse and fine sands was 45.9+/-7.8% and 96.9+/-3.2%, respectively. However, results from static batch adsorption experiments have limited applicability to dynamic bacterial transport in columns. The early breakthrough of E. coli relative to bromide was clear for all columns, namely c. 0.15 to 0.3 pore volume earlier. Column length had no significant effects on the E. coli peak concentration or on total recovery in leachate, indicating retention in the top layer of sands. Tailing of breakthrough curves was more prominent for all fine sand columns than their coarse sand counterparts. Bacterial recovery in leachate from coarse and saturated sand columns was significantly higher than from fine and unsaturated columns. Observed data were fitted by the convection-dispersion model, amended for one-site and two-site adsorption to particles, and for air-water interface (AWI) adsorption. Among all models, the two-site+AWI model achieved consistently high model efficiency for all experiments. Thus it is evident from experimental and modeling results that AWI adsorption plays an important role in E. coli transport in sand columns.     

Entrainment models and their application to jets in a turbulent cross flow

In this study, simple flows, such as buoyant jet and line thermal discharged into a still, uniform environment, are modelled mathematically by using integral equations of mass, momentum and thermal energy conservation. The governing equations are solved for entrainment rate by using an assumed growth rate model, the coefficients of which are fixed empirically. Entrainment models obtained by this method predict just as well as do models developed by other researchers who used different approaches.Our entrainment models are then applied to the problem of a turbulent jet discharged into a turbulent cross flow including both the near, intermediate, and far fields in a single model. It is assumed that the entrainment rate for this case can be obtained as a sum of terms representing near field entrainment of a buoyant jet and a line thermal, and far field mixing due to ambient turbulence. The predicted trajectories, velocities, and dilution rates agree satisfactorily with experimental results.     

Biofiltration Kinetics of a Gaseous Aldehyde Mixture Using a Synthetic Matrix

Abstract

Although aldehydes contribute to ozone and particulate matter formation, there has been little research on the biofiltration of these volatile organic compounds (VOCs), especially as mixtures. Biofiltration degradation kinetics of an aldehyde mixture containing hexanal, 2-methylbutanal (2-MB), and 3-methylbutanal (3-MB) was investigated using a bench-scale, synthetic, media-based biofilter. The adsorption capacity of the synthetic media for a model VOC, 3-methylbutanal, was 10 times that of compost. Periodic residence time distribution analysis (over the course of 1 yr) via a tracer study (84–99% recovery), indicated plug flow without channeling in the synthetic media and lack of compaction in the reactor. Simple first-order and zero-order kinetic models both equally fit the experimental data, yet analysis of the measured rate constants versus fractional conversion suggested an overall first-order model was more appropriate. Kinetic analysis indicated that hexanal had a significantly higher reaction rate (k = 0.09 ± 0.005 1/sec; 23 ± 1.3 ppmv) compared with the branched aldehydes (k = 0.04 ± 0.0036 1/sec; 31 ± 1.6 ppmv for 2-MB and 0.03 ± 0.0051 1/sec; 22 ± 1.3 ppmv for 3-MB). After 3 months of operation, all three compounds reached 100% removal (50 sec residence time, 18–46 ppmv inlet). Media samples withdrawn from the biofilter and observed under scanning electron microscopy analysis indicated microbial growth, suggesting removal of the aldehydes could be attributed to biodegradation.     

Critical velocity and range of a fire-gas plume in a ventilated tunnel

To protect passengers, personnel and equipment in a tunnel fire, it is important to understand and predict the movements of the hot-gas plume. To estimate the range of a fire plume propagating under the ceiling, a model is presented, that depends on two important parameters, i.e. the energy release rate of the fire and the velocity of the ventilation flow. The theoretical results, concerning the upwind range of the plume, agree favourably with experimental data obtained from eight tunnel fire tests. The theoretical value of the critical ventilation velocity, required to arrest the upwind movement of the fire-gas, agrees well with the corresponding experimental results for a wide range of energy release rates. The influences of air entrainment, friction at the ceiling and the associated heat loss are analysed and the results discussed.     

Evaluation of the UNC toluene-SOA mechanism with respect to other chamber studies and key model parameters

In a companion paper by Hu et al. [2007. A kinetic mechanism for predicting secondary organic aerosol formation from toluene oxidation in the presence of NO_x and natural sunlight. Atmospheric Environment, doi:10.1016/j.atmosenv.2007.04.025], a kinetic mechanism was developed from data generated in the University of North Carolina's (UNC) 270 m³ dual outdoor aerosol smog chamber, to predict secondary organic aerosol (SOA) formation from toluene oxidation in the atmosphere. In this paper, experimental data sets from European Photoreactor (EUPHORE), smog chambers at the California Institute of Technology (Caltech), and the UNC 300 m³ dual-outdoor gas phase chamber were used to evaluate the toluene mechanism. The model simulates SOA formation for the ‘low-NO_x’ and ‘mid-NO_x’ experiments from EUPHORE chambers reasonably well, but over-predicts SOA mass concentrations for the ‘high-NO_x’ run. The model well simulates the SOA mass concentrations observed from the Caltech chambers. Experiments with the three key toluene products, 1,4-butenedial, 4-oxo-2-pentenal and o-cresol in the presence of oxides of nitrogen (NO_x) are also simulated by the developed mechanism. The model well predicts the NO_x time–concentration profiles and the decay of these two carbonyls, but underestimates ozone (O₃) formation for 4-oxo-2-pentenal. It well simulates SOA formation from 1,4-butenedial but overestimates (possibly due to experimental problems) the measured aerosol mass concentrations from 4-oxo-2-pentenal. The model underestimates SOA production from o-cresol, mostly due to its under-prediction of o-cresol decay. The effects of varying temperature, relative humidity, glyoxal uptake, organic nitrate yields, and background seed aerosol concentrations, were also investigated.     

Optical measurements of aerosol size distributions in Great Smoky Mountains National Park: dry aerosol characterization

Aerosol size distributions were measured during the summertime 1995 Southeastern Aerosol and Visibility Study (SEAVS) in Great Smoky Mountains National Park using an Active Scattering Aerosol Spectrometer (ASASP-X) optical particle counter. We present an overview of the experimental method, our data inversion technique, timelines of the size distribution parameters, and calculations of dry accumulation mode aerosol density and refractive index. Aerosol size distributions were recorded during daylight hours for aerosol in the size range 0.1 < Dp < 2.5 microns. The particle refractive index used for the data inversion was calculated with the partial molar refractive index approach using 12-hr measured aerosol chemical composition. Aerosol accumulation mode volume concentrations ranging from 1 to 26 micron 3 cm-3 were observed, with an average of 7 +/- 5 micron 3 cm-3. The study average dry accumulation mode geometric volume median diameter was 0.27 +/- 0.03 micron, and the mean geometric standard deviation was 1.45 +/- 0.06. Using an internally mixed aerosol model, and assuming chemical homogeneity across the measured particle distribution, an average accumulation mode dry sulfate ion mass scattering efficiency of 3.8 +/- 0.6 m2 g-1 was calculated.     

Simultaneous measurement of light-scattering properties and particle size distribution for aerosols: Application to ammonium sulfate and quartz aerosol particles

An apparatus for measuring the scattering phase function and linear polarization of aerosol particles has been developed. The apparatus uses an elliptical mirror and CCD camera to image the full angular scattering range simultaneously. An in-line aerodynamic particle sizer (APS) in the particle flow stream provides for the simultaneous measurement of the aerosol particle size distribution. This apparatus allows for a comparison of measured optical properties with theoretical model calculations based on the measured aerosol size distribution. The system was calibrated and tested using monodisperse polystyrene latex (PSL) spheres and with ammonium sulfate (AS) aerosol. We have also used the apparatus for measuring the scattering phase function and linear polarization for light scattering from irregular quartz aerosol particles. Our results show that Mie theory substantially overestimates the backscattering cross-section for quartz particles in the size parameter range X∼2–4, in agreement with previous experimental work and theoretical modeling studies. We also present a normalized synthetic phase function for quartz dust aerosol in the accumulation mode size range (0.1–2.0 μm).     

Overview of Petroleum Environmental Research Forum (PERF) dense gas dispersion modeling project

This paper provides a background for and an overview of the results of a comprehensive study of transport and dispersion of dense gas plumes over rough surfaces typical of industrial sites. The Petroleum Environmental Research Forum (PERF) 93-16 project involved model development and evaluations using observations from three wind tunnels and from the Kit Fox field experiment. Detailed discussions of the results of the research are given in the other papers in this special issue. The wind tunnel experiments produced data showing that the resulting best-fit vertical entrainment formula was close to (i.e., within about 30%) the vertical entrainment formulas already in use by current models, which were derived primarily from observations over smooth surfaces. Observations from the Kit Fox field experiment demonstrated the validity of the entrainment curves derived from the wind tunnel data. The Kit Fox data were also used to evaluate algorithms for along-wind dispersion and cloud advection speeds for short-duration releases typical of an industrial site, and to evaluate the HEGADAS dense gas dispersion model.     

Aerosol speciation and mass prediction from toluene oxidation under high NOx conditions

A kinetically based gas-particle partitioning box model is used to highlight the importance of parameter representation in the prediction of secondary organic aerosol (SOA) formation following the photo-oxidation of toluene. The model is initialized using experimental data from York University's indoor smog chamber and provides a prediction of the total aerosol yield and speciation. A series of model sensitivity experiments were performed to study the aerosol speciation and mass prediction under high NO_x conditions (VOC/NO_x = 0.2). Sensitivity experiments indicate vapour pressure estimation to be a large area of weakness in predicting aerosol mass, creating an average total error range of 70 μg m^?3 (range of 5–145 μg m^?3), using two different estimation methods. Aerosol speciation proved relatively insensitive to changes in vapour pressure. One species, 3-methyl-6-nitro-catechol, dominated the aerosol phase regardless of the vapour pressure parameterization used and comprised 73–88% of the aerosol by mass. The dominance is associated with the large concentration of 3-methyl-6-nitro-catechol in the gas-phase. The high NO_x initial conditions of this study suggests that the predominance of 3-methyl-6-nitro-catechol likely results from the cresol-forming branch in the Master Chemical Mechanism taking a significant role in secondary organic aerosol formation under high NO_x conditions. Further research into the yields and speciation leading to this reaction product is recommended.     

Environmental tobacco smoke particles in multizone indoor environments

Environmental tobacco smoke (ETS) is a major source of human exposure to airborne particles. To better understand the factors that affect exposure, and to investigate the potential effectiveness of technical control measures, a series of experiments was conducted in a two-room test facility. Particle concentrations, size distributions, and airflow rates were measured during and after combustion of a cigarette. Experiments were varied to obtain information about the effects on exposure of smoker segregation, ventilation modification, and air filtration. The experimental data were used to test the performance of an analytical model of the two-zone environment and a numerical multizone aerosol dynamics model. A respiratory tract particle deposition model was also applied to the results to estimate the mass of ETS particles that would be deposited in the lungs of a nonsmoker exposed in either the smoking or nonsmoking room. Comparisons between the experimental data and model predictions showed good agreement. For time-averaged particle mass concentration, the average bias between model and experiments was less than 10%. The average absolute error was typically 35%, probably because of variability in particle emission rates from cigarettes. For the conditions tested, the use of a portable air filtration unit yielded 65–90% reductions in predicted lung deposition relative to the baseline scenario. The use of exhaust ventilation in the smoking room reduced predicted lung deposition in the nonsmoking room by more than 80%, as did segregating the smoker from nonsmokers with a closed door.     

Evaluation of Quicklime Incorporation in Bench-Scale and Full-Scale Lime Stabilized Biosolids Using a Flat Surface pH Electrode

Abstract

Uniform lime incorporation into sewage sludge is critical for biosolid lime stabilization processes. There is no class B biosolids regulation for lime incorporation. The slurry method is currently used to evaluate the pH of limed biosolids, but this method homogenizes the biosolids and potentially masks poor lime mixing. In this study, a flat-surface pH electrode was used in bench-scale and full-scale experiments to measure the pH of lime-stabilized biosolids without creating slurries. The standard deviation of 15 pH measurements at different locations in a biosolid sample was used to assess mixing quality. The bench-scale experimental study showed that well-mixed limed biosolids had consistently high pHs (~12) with low standard deviations (<0.5 pH units), whereas poorly mixed biosolids had areas with low pH (<10) and high standard deviations (>2 pH units). Poorly mixed biosolids exhibited rapid and marked pH reduction, as well as offensive odor generation, whereas well-mixed biosolids resisted pH reduction and offensive odor generation. The full-scale study aimed at improving lime incorporation and biosolids quality confirmed the use of a flat surface pH electrode to capture low pH regions in biosolids that were masked by the current slurry method.     

A sensibility analysis of model selection in modeling the reactive transport of cesium in crushed granite

We performed a sensibility analysis of model selection in modeling the reactive transport of cesium in crushed granite through model calibration and validation. Based on some solid phase analysis data and kinetic batch experimental results, we hypothesized three two-site sorption models in the LEHGC reactive transport model to fit the breakthrough curves (BTCs) from the corresponding column experiments. The analysis of breakthrough curves shows that both the empirical two-site kinetic linear sorption model and the semi-mechanistic/semi-empirical two-site kinetic surface complexation model, regardless of their complexity, can match our experimental data fairly well under given test conditions. A numerical experiment to further compare the two models shows that they behave differently when the pore velocity is not of the same order of magnitude as our test velocities. This result indicates that further investigations to help determine a better model are needed. We suggest that a multistage column experiment, which tests over the whole range of practical flow velocities, should be conducted to help alleviate inadequate hypothesized models.     

Chemistry and aerosols in the marine boundary layer: 1-D modelling of the three ACE-2 Lagrangian experiments

Three Lagrangian experiments were conducted during IGAC's second aerosol characterization experiment (ACE-2) in the area between Portugal, Tenerife and Madeira in June/July 1997. During each Lagrangian experiment, a boundary layer air mass was followed for about 30 h, and the temporal evolution of its chemical and aerosol composition was documented by a series of vertical profiles and horizontal box pattern flown by the Meteorological Research Flight research aircraft Hercules C130. The wealth of observational data that has been collected during these three Lagrangian experiments is the basis for the development and testing of a one-dimensional Lagrangian boundary layer model with coupled gas, aqueous, and aerosol phase chemistry. The focus of this paper is on current model limitations and strengths. We show that the model is able to represent the dynamical and chemical evolution of the marine boundary layer, in some cases requiring adjustments of the subsidence velocity and of the surface heat fluxes. Entrainment of a layer rich in ozone and carbon monoxide from a residual continental boundary layer into the marine boundary layer as well as in-cloud oxidation of sulphur dioxide by hydrogen peroxide are simulated, and coherent results are obtained, concerning the evolution of the small, presumably sulphate–ammonia aerosol mode.     

Contribution of Primary and Secondary Sources to Organic Aerosol and PM2.5 at SEARCH Network Sites

Abstract

Chemical tracer methods for determining contributions to primary organic aerosol (POA) are fairly well established, whereas similar techniques for secondary organic aerosol (SOA), inherently complicated by time-dependent atmospheric processes, are only beginning to be studied. Laboratory chamber experiments provide insights into the precursors of SOA, but field data must be used to test the approaches. This study investigates primary and secondary sources of organic carbon (OC) and determines their mass contribution to particulate matter 2.5 µm or less in aerodynamic diameter (PM_2.5) in Southeastern Aerosol Research and Characterization (SEARCH) network samples. Filter samples were taken during 20 24-hr periods between May and August 2005 at SEARCH sites in Atlanta, GA (JST); Birmingham, AL (BHM); Centerville, AL (CTR); and Pensacola, FL (PNS) and analyzed for organic tracers by gas chromatography-mass spectrometry. Contribution to primary OC was made using a chemical mass balance method and to secondary OC using a mass fraction method. Aerosol masses were reconstructed from the contributions of POA, SOA, elemental carbon, inorganic ions (sulfate [SO₄ ^2?], nitrate [NO₃ ^?], ammonium [NH₄ ⁺]), metals, and metal oxides and compared with the measured PM_2.5. From the analysis, OC contributions from seven primary sources and four secondary sources were determined. The major primary sources of carbon were from wood combustion, diesel and gasoline exhaust, and meat cooking; major secondary sources were from isoprene and monoterpenes with minor contributions from toluene and β-caryophyllene SOA. Mass concentrations at the four sites were determined using source-specific organic mass (OM)-to-OC ratios and gave values in the range of 12–42 µg m^?3. Reconstructed masses at three of the sites (JST, CTR, PNS) ranged from 87 to 91% of the measured PM_2.5 mass. The reconstructed mass at the BHM site exceeded the measured mass by approximately 25%. The difference between the reconstructed and measured PM_2.5 mass for nonindustrial areas is consistent with not including aerosol liquid water or other sources of organic aerosol.     

Fusion of SeaWiFS and TOMS Satellite Data with Surface Observations and Topographic Data during Extreme Aerosol Events

ABSTRACT

Spaceborne sensors allow near-continuous aerosol monitoring throughout the world. This paper illustrates the fusion of Sea-Viewing Wide Field-of-View Sensor (SeaWiFS) and TOMS satellite data with surface observations and topographic data during four extreme aerosol events: (1) the April 1998 Asian dust storm that impacted the west coast of North America, (2) the May 1998 Central American forest fire smoke that impacted eastern North America, (3) the intense fall 1999 northern California fires, and (4) the massive February 2000 Sahara dust storm. During these dust and smoke events, the aerosol was visualized on true color SeaWiFS images as a distinct yellowish dye, the result of the aerosol increasing the reflectance of darker surfaces (ocean and land) and decreasing the reflectance of clouds. TOMS imagery also indicated increased aerosol absorption in the affected areas, while surface monitors measured major reductions in visual range. Fusing these data aids in the determination of the aerosol's spatial, temporal, and optical properties and provides supporting evidence for characterizing what is being visualized as dust or smoke. A 3-dimensional perspective of the events is obtained when incorporating topographic data and provides insight into the vertical properties of the aerosol plumes.