The Evolution of Visibility Deterioration and Aerosol Spectra in the St. Louis Urban Plume

Under the auspices of Project METROMEX, studies of visibility de-teoration downwind of St. Louis were conducted during July-August 1974-1975. Estimates of horizontal visual range, standard meteorological data, and aerosol characteristics within the mixing layer were acquired upwind, over, and downwind of the metropolitan area by means of airborne transects. Aerosol number, surface, and volume distributions for particles between 0.025-2.5 µm were generated from the airborne measurement of Aitken nucleus concentrations, cloud condensation nuclei, and aerosols detected in situ with optical probes. Visibility reduction amounting to 50% of prevailing regional upwind visibilities consistently occurs at a distance corresponding to 2-3 hours travel time downwind for an air parcel moving with the mean transport wind. The regions of visibility minimum do not coincide with locations of maximum Aitken nucleus concentrations, but rather correspond in space and time to increased values of cloud condensation nuclei and increased numbers of particles in the 0.1-2.5 µm diameter range. Comparisons of observed aerosol evolution with similar laboratory studies suggest that most of the light scattering aerosols are of secondary origin.     

The Analysis of Airborne Sulfate

This report reviews the current state of analytical methodology for sulfate in airborne particles. Methods for determination of total aerosol sulfate and total soluble sulfate are assessed. A more detailed review of the relatively new techniques for quantitative speciation of airborne sulfate then follows. Size distribution methodology and filter sampling difficulties relating to the collection of airborne sulfate-containing particles are enumerated. Experiments are suggested which use new, improved, and potentially applicable sulfate speciation techniques to obtain a better understanding of the generation, transport, transformation and removal processes that, in turn, determine the identity and concentrations of sulfate species in ambient air.     

Aircraft emissions and local air quality impacts from takeoff activities at a large International Airport

Real time number concentrations and size distributions of ultrafine particles (UFPs, diameter <100 nm) and time integrated black carbon, PM_2.5 mass, and chemical species were studied at the Los Angeles International Airport (LAX) and a background reference site. At LAX, data were collected at the blast fence (∼140 m from the takeoff position) and five downwind sites up to 600 m from the takeoff runway and upwind of the 405 freeway. Size distributions of UFPs collected at the blast fence site showed very high number concentrations, with the highest numbers found at a particle size of approximately 14 nm. The highest spikes in the time series profile of UFP number concentrations were correlated with individual aircraft takeoff. Measurements indicate a more than 100-fold difference in particle number concentrations between the highest spikes during takeoffs and the lowest concentrations when no takeoff is occurring. Total UFP counts exceeded 10⁷ particles cm⁻³ during some monitored takeoffs. Time averaged concentrations of PM_2.5 mass and two carbonyl compounds, formaldehyde and acrolein, were statistically elevated at the airport site relative to a background reference site. Peaks of 15 nm particles, associated with aircraft takeoffs, that occurred at the blast fence were matched with peaks observed 600 m downwind, with time lags of less than 1 min. The results of this study demonstrate that commercial aircraft at LAX emit large quantities of UFP at the lower end of currently measurable particle size ranges. The observed highly elevated UFP concentrations downwind of LAX associated with aircraft takeoff activities have significant exposure and possible health implications.     

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

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

The Mass Distribution of Large Atmospheric Particles

This paper describes the results of a study to determine the total mass and the mass distribution of atmospheric aerosols, especially that mass associated with particles greater than 10 μm diameter. This study also determined what fraction of the total aerosol mass a standard high-volume air sampler collects and what fraction and size interval settle out on a dust fall plate. A special aerosol sampling system was designed for this study to obtain representative samples of large airborne particles. A suburban sampling site was selected because no local point sources of aerosols existed nearby. Samples were collected under various conditions of wind velocity and direction to obtain measurements on different types of aerosols.

Study measurements show that atmospheric particulate matter has a bimodal mass distribution. Mass associated with large particles mainly ranged from 5 to 100 μm in size, while mass associated with small particles ranged from an estimated 0.03 to 5 μm in size. Combined, these two distributions produced a bimodal mass distribution with a minimum around 5 μm diameter. The high-volume air sampler was found to collect most of the total aerosol mass, not just that fraction normally considered suspended particulate. Dust fall plates did not provide a good or very useful measure of total aerosol mass. The two fundamental processes of aerosol formation, condensation and dispersion appear to account for the formation of a bimodal mass distribution in both natural and anthropogenic aerosols. Particle size distribution measurements frequently are in error because representative samples of large airborne particles are not obtained. Considering this descrepancy, air pollution regulations should specify or be based upon an upper particle size limit.     

Concentrations of particulate matter emitted from large cattle feedlots in Kansas

Particulate matter (PM) emitted from cattle feedlots are thought to affect air quality in rural communities, yet little is known about factors controlling their emissions. The concentrations of PM (i.e., PM2.5, PM10, and total suspended particulates or TSP) upwind and downwind at two large cattle feedlots (KS1, KS2) in Kansas were measured with gravimetric samplers from May 2006 to October 2009 (at KS1) and from September 2007 to April 2008 (at KS2). The mean downwind and net (i.e., downwind - upwind) mass concentrations of PM2.5, PM10, and TSP varied seasonally, indicating the need for multiple-day, seasonal sampling. The downwind and net concentrations were closely related to the moisture content of the pen surface. The PM2.5/PM10 and PM2.5/TSP ratios at the downwind sampling location were also related to the moisture content of the pen surface, humidity, and temperature. Measurement of the particle size distribution downwind of the feedlot with a cascade impactor showed geometric mean diameter ranging from 7 to 18 microm, indicating that particles that were emitted from the feedlots were generally large in size.     

Indoor/outdoor connections exemplified by processes that depend on an organic compound's saturation vapor pressure

Outdoor and indoor environments are profitably viewed as parts of a whole connected through various physical and chemical interactions. This paper examines four phenomena that share a dependence on vapor pressure—the extent to which an organic compound in the gas phase sorbs on airborne particles, sorbs on surfaces, sorbs on particles collected on a filter or activates trigeminal nerve receptors. It also defines a new equilibrium coefficient for the partitioning of organic compounds between an airstream and particles collected by a filter in that airstream. Gas/particle partitioning has been studied extensively outdoors, but sparingly indoors. Gas/surface partitioning occurs primarily indoors while gas/filter partitioning occurs at the interface between outdoors and indoors. Activation of trigeminal nerve receptors occurs at the human interface. The logarithm of an organic compound's saturation vapor pressure correlates in a linear fashion with the logarithms of equilibrium coefficients characteristic of each of these four phenomena. Since, to a rough approximation, the log of an organic compound's vapor pressure scales with its molecular weight, molecular weight can be used to make first estimates of the above processes. For typical indoor conditions, only larger compounds with lower-saturation vapor pressures (e.g., tetracosane, pentacosane, or di-2-ethylhexyl phthalate) have airborne particle concentrations comparable to or larger than gas phase concentrations. Regardless of a compound's vapor pressure, the total mass sorbed on indoor airborne particles is quite small compared to the total sorbed on indoor surfaces, reflecting the large difference in surface areas between particles within a room and surfaces within a room. If the actual surface areas are considered, accounting for roughness and porosity, the surface concentration of organics sorbed on typical airborne particles appears to be comparable to the surface concentration of organics sorbed on indoor carpets, walls and other materials (based on data from several studies in the literature). Mirroring the importance of phase distributions outdoors, an organic compound's indoor lifetime, fate and even health impacts depend on its distribution between phases and among surfaces.     

Roadside particle number distributions and relationships between number concentrations, meteorology, and traffic along a northern California freeway

Particle number distributions were measured simultaneously upwind and downwind of a suburban-agricultural freeway to determine relationships with traffic and meteorological parameters. Average traffic volumes were 6330 vehicles/hr with 10% heavy-duty vehicles, and volumes were higher in July than November. Most downwind particle number distributions were bimodal, with a primary mode at approximately 10-25 nm, indicating that newly formed particles were sampled. Total downwind 6-237 nm particle number concentrations (Ntot) ranged from 9.3 x 10(3) to 2.5 x 10(5) cm(-3), with higher daily average concentrations in November compared with July. Ntot correlated with wind speed, temperature, and relative humidity. Upwind photochemically initiated nucleation likely led to elevated background nanoparticle concentrations in July, as evidenced by increasing upwind distribution modal diameter with increasing temperature and a strong correlation between upwind Ntot and solar radiation. Also in summer, Ntot showed stronger correlation with heavy-duty vehicle volumes than wind speed, temperature, and relative humidity. These results indicate the importance of measuring background particle size distributions simultaneously with roadside distributions. There may be a minimum vehicle volume from which useful real-world vehicle particle number distributions can be measured at roadside, even when collecting samples within 10 m of the traveled lanes.     

Impact of roadside noise barriers on particle size distributions and pollutants concentrations near freeways

Increasing epidemiological evidence has established an association between a host of adverse health effects and exposure to ambient particulate matter (PM) and co-pollutants, especially those emitted from motor vehicles. Although PM and their co-pollutants dispersion profiles near the open freeway have been extensively characterized by means of both experimental measurements and numerical simulations in recent years, such investigations near freeways with roadside barriers have not been well documented in the literature. A few previous studies suggested that the presence of roadside structures, such as noise barriers and vegetation, may impact the decay of pollutant concentrations downwind of the freeway by limiting the initial dispersion of traffic emissions and increasing their vertical mixing due to the upward deflection of airflow. Since the noise barriers are now common roadside features of the freeways, particularly those running through populated urban areas, it is pertinent to investigate the impact of their presence on the particles and co-pollutants concentrations in areas adjacent to busy roadways. This study investigated two highly trafficked freeways (I-710 and I-5) in Southern California, with two sampling sites for each freeway, one with and the other without the roadside noise barriers. Particle size distributions and co-pollutants concentrations were measured in the immediate proximity of freeways and at different distances downwind of the freeways. The results showed the formation of a “concentration deficit” zone in the immediate vicinity of the freeway with the presence of roadside noise barrier, followed by a surge of pollutant concentrations further downwind at 80–100 m away from freeway. The particle and co-pollutants concentrations reach background levels at farther distances of 250–400 m compared to 150–200 m at the sites without roadside noise barriers.     

Particulate size distributions and mass measured at a motorway during the BAB II campaign

From 1 May to 25 May 2001, the BAB II campaign was carried out at the motorway BAB (656) near Heidelberg. Atmospheric concentrations of particulate matter and gases were measured together with the meteorological conditions. This paper is focused on the particulate matter measured upwind and downwind from the motorway at ground level. In order to determine the source contribution from the motorway traffic, it was necessary to measure upwind and downwind simultaneously due to variations in background concentrations. The particle number contribution from the motorway was found to be 35,000 particles cm⁻³ for particles with diameters close to 20 nm and 5000 particles cm⁻³ for particles with diameters close to 70 nm. Bimodal size distributions were observed on the downwind side, whereas the upwind side showed unimodal size distributions. For particulate mass, it can be estimated that the contribution from the motorway to the PM₁ concentrations is in a range 0.6–1.3 μg m⁻³ for the chosen measurement sites approximately 60 m from the road at a height of 6 m. The soot measurements showed diurnal variation; however, the upwind downwind difference was not measured. Correlation factors showed good correlation between total particle number and number of particles with diameters below 80 nm, CO and NO. There was no correlation between particle number and PM₁₀, which is due to the observation that particle number was dominated by the 20 nm particles.     

Particle Size Distribution of Urban Lead Aerosols

Size distributions of lead aerosols were obtained for 61 test periods in five urban and two remote areas of the United States. The tests were carried out under a variety of weather conditions in downtown, industrial, and residential locations of Los Angeles, the San Francisco Bay area, Chicago, Cincinnati, Philadelphia, and remote sites in Oklahoma and Arizona. Samples were obtained with a modified Goetz Aerosol spectrometer. Various fractions of the collected samples were analyzed by the dithizone method for lead and the size distributions were calculated on the basis of the chemical determinations. Size distributions were generally similar at the several sampling sites covered in the study.     

Compounds in Airborne Participates: Salts and Hydrocarbons

Concentrations of 10 polycyclic aromatic hydrocarbons (PAH), the aliphatlcs as a group, sulfate, nitrate, fluoride, acidity, and carbon In the airborne partlculate matter were measured at 16 sites In Cleveland, OH over a 1 year period during 1971 and 1972. Analytical methods used included gas chromatography, colorimetry, and combustion techniques. Uncertainties in the concentrations associated with the sampling procedures, and the analytical methods are evaluated. The data are discussed relative to other studies and source origins. Benzo(a)pyrene and its high concentrations downwind of coke ovens are discussed. Hydrocarbon correlation studies indicated no significant relations among compounds studied.     

Factor analysis of submicron particle size distributions near a major United States-Canada trade bridge

A factor analytic model has been applied to resolve and apportion particles based on submicron particle size distributions downwind of a United States-Canada bridge in Buffalo, NY. The sites chosen for this study were located at gradually increasing distances downwind of the bridge complex. Seven independent factors were resolved, including four factors that were common to all of the five sites considered. The common factors were generally characterized by the existence of two or more number and surface area modes. The seven factors resolved were identified as follows: fresh tail-pipe diesel exhaust, local/street diesel traffic, aged/evolved diesel particles, spark-ignition gasoline emissions, background urban emissions, heavy-duty diesel agglomerates, and secondary/transported material. Submicron (<0.5 microm) and ultrafine (<0.1 microm) particle emissions downwind of the bridge were dominated by commercial diesel truck emissions. Thus, this study obtained size distinction between fresh versus aged vehicle exhaust and spark-ignition versus diesel emissions based on the measured high time-resolution particle number concentrations. Because this study mainly used particles <300 nm in diameter, some sources that would usually exhibit number modes >100 nm were not resolved. Also, the resolved profiles suggested that the major number mode for fresh tailpipe diesel exhaust might exist below the detection limit of the spectrometer used. The average particle number contributions from the resolved factors were highest closest to the bridge.     

Potentially Allergenic Airborne Particles in the Vicinity of a Yeast and Penicillin Production Plant

Potential health risks of exposure to emissions of a yeast and penicillin production plant were investigated by measuring viable particles and protein contents of particles in ambient air. The results showed a clear decrease of the downwind number of yeast colonyforming units with increasing distance from the source. Upwind the number of yeast colony-forming units was zero. Identification showed that nearly all yeast were of the species Saccharomlces cerevisiae. Such a trend could not be found for the total number of colony-forming units (yeasts, molds, and bacteria) although the upwind concentration was slightly lower than the downwind concentration. The downwind protein concentration was significantly elevated compared to the upwind concentration.     

Fluorescent Tracer Studies of Pollutant Transport in the San Francisco Bay Area

To simulate the transport and diffusion of airborne contaminants across a metropolitan region, point-source releases of fluorescent tracer material were made near various urban centers and some 50 samplers were arrayed in expected downwind directions. The effects of land-water, hill-valley, and urban-rural differences on airflow and diffusion were observed in their existing interrelationships during these experiments. Since the tracer could be assessed with high sensitivity over great distances, tracer results provided a quantitative indicator of pollutant dispersion across an extensive metropolitan complex.

From July 1967 through June 1968, the test series included typical seasonal weather patterns, with emphasis on those conducive to the travel and accumulation of pollutants. In each test about 15 kilograms of tracer material were released during two-hour periods, and significant dosages were found at downwind distances up to 80 kilometers. All tests were conducted during daylight hours, to coincide better with the oxidant-type pollution important in this region.

Dispersion characteristics showed much greater complexity than predictable from classical models, thus limiting the applicability of such models in this region. Built-up urban areas increased the initial dispersion rates of tracer clouds, and travel over water tended to decrease them. Hilly terrain resulted in increased dispersion, but channeling associated with such terrain caused locally higher concentrations. The complex horizontal dosage patterns obtained did confirm previously observed airflow patterns as aids in predicting pollutant distributions.     

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

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

The assessment of particulate matter emitted from stone-crushing industry by correlating rock textures with particles generated after comminution and dispersed in air environment

The generation and emission of particulate matter from abrasion industry are subjects of the pollution monitoring by multidisciplinary study involving earth sciences and engineering disciplines. This work investigates the correlation between textural properties of in situ rock with class size distribution and morphology of particles generated after rock comminution and particles emitted in the air. A special comminution-dust sampling architecture was realised. The combined use of scanning electron microscopy and particle size analyser was considered in performing digital image analysis on both crushed products and airborne particles collected onto membrane filters. The results show that the size and morphology of crushed particles are linked to the petrographic rock properties. In particular, particles with fibrous morphology are prominent in rocks showing foliated textures where elongated minerals occurred, with implication for asbestos-bearing rocks. For what concerns the airborne particles, the results show that their aerodynamic diameters are independent of the crusher operating conditions. External parameters probably intervene in the distribution of the airborne particles emission, including the dynamic air fluxes, or environmental conditions. By applying mathematical models, the morphology and size range of airborne particles following the comminution processes can be predicted, and results has implication for pollutants contamination due to particulate matters emitted by crush stone industry.     

Evaluating the capabilities of Aerosol-to-Liquid Particle Extraction System (ALPXS)/ICP-MS for monitoring trace metals in indoor air

This study investigates the application of the Aerosol-to-Liquid Particle Extraction System (ALPXS), which uses wet electrostatic precipitation to collect airborne particles, for multi-element indoor stationary monitoring. Optimum conditions are determined for capturing airborne particles for metal determination by inductively coupled plasma–mass spectrometry (ICP-MS), for measuring field blanks, and for calculating limits of detection (LOD) and quantification (LOQ). Due to the relatively high flow rate (300 L min^?1), a sampling duration of 1 hr to 2 hr was adequate to capture airborne particle-bound metals under the investigated experimental conditions. The performance of the ALPXS during a building renovation demonstrated signal-to-noise ratios appropriate for sampling airborne particles in environments with elevated metal concentrations, such as workplace settings. The ALPXS shows promise as a research tool for providing useful information on short-term variations (transient signals) and for trapping particles into aqueous solutions where needed for subsequent characterization. As the ALPXS does not provide size-specific samples, and its efficiency at different flow rates has yet to be quantified, the ALPXS would not replace standard filter-based protocols accepted for regulatory applications (e.g., exposure measurements), but rather would provide additional information if used in conjunction with filter based methods.

ImplicationsThis study investigates the capability of the Aerosol-to-Liquid Particle Extraction System (ALPXS) for stationary sampling of airborne metals in indoor workplace environments, with subsequent analysis by ICP-MS. The high flow rate (300 L/min) permits a short sampling duration (< 2 hr). Results indicated that the ALPXS was capable of monitoring short-term changes in metal emissions during a renovation activity. This portable instrument may prove to be advantageous in occupational settings as a qualitative indicator of elevated concentrations of airborne metals at short time scales.     

Concentration and Size Distribution of Ultrafine Particles Near a Major Highway

Abstract

Motor vehicle emissions usually constitute the most significant source of ultrafine particles (diameter <0.1 μm) in an urban environment, yet little is known about the concentration and size distribution of ultrafine particles in the vicinity of major highways. In the present study, particle number concentration and size distribution in the size range from 6 to 220 nm were measured by a condensation particle counter (CPC) and a scanning mobility particle sizer (SMPS), respectively. Measurements were taken 30, 60, 90, 150, and 300 m downwind, and 300 m upwind, from Interstate 405 at the Los Angeles National Cemetery. At each sampling location, concentrations of CO, black carbon (BC), and particle mass were also measured by a Dasibi CO monitor, an aethalometer, and a DataRam, respectively. The range of average concentration of CO, BC, total particle number, and mass concentration at 30 m was 1.7?2.2 ppm, 3.4?10.0 μg/m³, 1.3?2.0 × 10⁵/cm³, and 30.2?64.6 μ/m³, respectively.

For the conditions of these measurements, relative concentrations of CO, BC, and particle number tracked each other well as distance from the freeway increased. Particle number concentration (6–220 nm) decreased exponentially with downwind distance from the freeway. Data showed that both atmospheric dispersion and coagulation contributed to the rapid decrease in particle number concentration and change in particle size distribution with increasing distance from the freeway. Average traffic flow during the sampling periods was 13,900 vehicles/hr. Ninety-three percent of vehicles were gasoline-powered cars or light trucks. The measured number concentration tracked traffic flow well. Thirty meters downwind from the freeway, three distinct ultrafine modes were observed with geometric mean diameters of 13, 27, and 65 nm. The smallest mode, with a peak concentration of 1.6 × 10⁵/cm³, disappeared at distances greater than 90 m from the freeway. Ultrafine particle number concentration measured 300 m downwind from the freeway was indistinguishable from upwind background concentration. These data may be used to estimate exposure to ultrafine particles in the vicinity of major highways.