Size Distribution of Participates Emitted from a Horizontal Spike Soderberg Aluminum Reduction Cell

Aerosol size distributions were measured in the air exhausted from a horizontal spike Soderberg aluminum reduction cell at the Kaiser Aluminum and Chemical Corporation plant in Tacoma, Wash. The particle size distributions were measured with the University of Washington cascade impactor, developed specifically for source testing. The particle mass concentrations and size distributions were found to vary significantly with changes in the cell process operations. For a typical aerosol size distribution at the exit of the cell hood the mass mean particle diameter was 5.5 microns and the particle size standard geometric deviation was 25.     

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.     

The modality of particle size distributions of environmental aerosols

Knowledge of the distribution of airborne particulate matter into size fractions has become an increasing area of focus when examining the effects of air pollution. While total number and mass concentrations may play an important role in exposure and risk assessment analyses, often an understanding of the particle size distributions provides more information on the type of atmospheric processes resulting in the distributions. The modality of the particle size distribution is one such aspect that has been associated with the aerosol formation mechanisms. The aim of this work is to provide a detailed analysis of the modal characteristics of a large number of particle size spectra collected over a period of three years for a range of ambient aerosol types. Measurements of over 6000 size distributions in the size range 0.016–30 μm were made using a scanning mobility particle sizer and an aerodynamic particle sizer for various ambient aerosols including: traffic influenced, urban, vegetation burning influenced, marine, modified background and suburban. Advanced data analytical procedures were adopted to combine the distributions from the two instruments for the calculation of the volume size distributions to allow clear interpretation of the modal characteristics. It was determined that, while in most cases there is a distinct nuclei mode in the number size distribution, this does not translate to a nuclei mode in the volume size distribution. Furthermore, while many of the number size distributions were different for each aerosol studied, the volume distributions were similar. This finding has serious implications for the setting of mass-based air quality standards.     

Number size distribution of atmospheric aerosols during ACE-Asia dust and precipitation events

Measurements of size-resolved particle number concentrations during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) field campaign were made at the Gosan super-site, South Korea. In East Asia, dust and precipitation phenomena play a crucial role in atmospheric environment and climate studies because they are major sources and sinks of atmospheric aerosols, especially in the springtime. Total Ozone Mapping Spectrometer (TOMS) Aerosol Index and backward trajectories are analyzed to investigate the spatial and temporal evolution of dust storms. The size distributions between dust and non-dust periods and times with and without precipitation are compared. In order to understand the temporal evolution of the aerosol size distribution during dust and precipitation events, a simple aerosol dynamics model is employed. The model predicted and observed size distributions are compared with the measured data. The results show that the coarse mode particle number concentrations increase by a factor of 10–16 during dust events. During precipitation, however, particles in the coarse mode are scavenged by impaction mechanism. It is found that the larger particles are more efficiently scavenged. The degree of scavenged particle varies depending on the rainfall rate, raindrop size distribution and aerosol size distribution.     

Particle size relationships at the Fresno Supersite

Aerosol size distributions are presented for a winter intensive study at the Fresno Supersite. The size distributions were consistent with and predictive for continuous PM2.5 measured by beta attenuation. They varied temporally with respect to source type and intensity, with the smallest mean diameters associated with high NOx concentrations during weekday morning rush hours. Conversely, small and large particle and black carbon (BC) concentrations were higher during Sunday and weekday evenings in response to traffic and residential wood combustion emissions. Ambient PM2.5 light scattering (Bsp) was precisely but systematically underestimated during winter, probably because of heating in the sample shelter.     

A quantitative description of vehicle exhaust particle size distributions in a highway tunnel

During the period May 18-May 22, 1999, a comprehensive study was conducted in the Tuscarora Mountain Tunnel on the Pennsylvania Turnpike to measure real-world motor-vehicle emissions. As part of this study, size distributions of particle emissions were determined using a scanning mobility particle sizer. Each measured size distribution consisted of two modes: a nucleation mode with midpoint diameter less than 20 nm and an accumulation mode with midpoint diameter less than 100 nm. The nucleation and accumulation components in some distributions also exhibited second maxima, which implies that such particle size distributions are superpositions of two particle size distributions. This hypothesis was utilized in fitting the particle size distributions that exhibited second maxima with four lognormal distributions, two for the nucleation mode and two for the accumulation mode. The fitting assumed that the observed particle size distribution was a combination of two bimodal log-normal distributions, one attributed to the heavy-duty diesel (HDD) vehicles and another attributed either to a different class of HDD vehicles or to the light-duty spark ignition vehicles. Based on this method, estimated particle production rates were 1.8 x 10(13) and 2.8 x 10(14) particles/vehicle-km for light-duty spark ignition and HDD vehicles, respectively, which agreed with independently obtained estimates.     

Estimating fine particulate matter component concentrations and size distributions using satellite-retrieved fractional aerosol optical depth: part 2--a case study

We use the fractional aerosol optical depth (AOD) values derived from Multiangle Imaging Spectroradiometer (MISR) aerosol component measurements, along with aerosol transport model constraints, to estimate ground-level concentrations of fine particulate matter (PM2.5) mass and its major constituents in the continental United States. Regression models using fractional AODs predict PM2.5 mass and sulfate (SO4) concentrations in both the eastern and western United States, and nitrate (NO3) concentrations in the western United States reasonably well, compared with the available ground-level U.S. Environment Protection Agency (EPA) measurements. These models show substantially improved predictive power when compared with similar models using total-column AOD as a single predictor, especially in the western United States. The relative contributions of the MISR aerosol components in these regression models are used to estimate size distributions of EPA PM2.5 species. This method captures the overall shapes of the size distributions of PM2.5 mass and SO4 particles in the east and west, and NO3 particles in the west. However, the estimated PM2.5 and SO4 mode diameters are smaller than those previously reported by monitoring studies conducted at ground level. This is likely due to the satellite sampling bias caused by the inability to retrieve aerosols through cloud cover, and the impact of particle hygroscopicity on measured particle size distributions at ground level.     

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.     

The impact of biomass burning on the environmental aerosol concentration in Gaborone,Botswana

Biomass burning, in the form of savanna fires and firewood for cooking and warmth, is widespread during the dry winter months in Southern Africa. This study was carried out to investigate its impact on the environment in Gaborone, Botswana, which is a small-sized city with very little pollution from industrial sources. Measurements of aerosol size and number concentrations were carried out at the University of Botswana campus in Gaborone from September 1999 to July 2000 using two automatic laser scattering particle counters. Particles were monitored in eight size ranges from 0.1 to 5.0 μm. The mean daily particle concentrations were found to vary from about 200 cm⁻³ on clear visibility days during the summer to a high of over 9000 cm⁻³ on cold winter evenings, when there was a significant smoke haze over the city. Particle concentrations were noticeably higher during the winter than in the summer. During a typical winter day, the total particle concentration peaked between 18 and 23 h, often showing an increase of over four-fold from mid-morning minimum values. The aerosol number size distributions under various conditions were investigated and the corresponding surface area and volume distributions were derived. In general, both the surface and volume distributions were bimodal with peaks close to 0.2 μm and at 5.0 μm or greater. A hand-held counter with a minimum detectable particle size of 0.3 μm was used to monitor the size and number concentrations of aerosols across the city. The results indicate a consistent pattern of maximum concentration in the highly populated areas close to the city centre, falling significantly in the sparsely populated outlying areas by up to an order of magnitude during peak biomass burning, suggesting that much of the smoke particles in the city are removed by wind.     

Pronounced decrease of ambient particle number emissions from diesel traffic in Denmark after reduction of the sulphur content in diesel fuel

Measurements of particle number concentration and size distributions in a Copenhagen street canyon in January–March 1999, and one year later in 2000, have revealed that the number of particles in the ultrafine size range below 100 nm decreased significantly in the period between the two campaigns. The decrease was especially large in the size range below 30 nm. By two common factors, we found high co-variance between ultrafine particles, nitrogen oxides, and carbon monoxide. The co-variation can be used to assess the contributions and size distributions of particles from the two main sources, petrol traffic and diesel traffic. Here, we show that the drop in particle concentrations can be consistently explained by a 56% fall in the average particle emission from the diesel vehicles in the street. In the same period, we found no change in the particle emission from petrol cars. The change is probably due to the reduction of the sulphur content in diesel fuel from approximately 0.05% to less than 0.005%, implemented in all parts of Denmark in July 1999.     

A study of the horizontal and vertical profile of submicrometer particles in relation to a busy road

Epidemiological studies are consistently reporting an association between fine particulate pollution and ill-health. Motor vehicle emissions are considered to be the main source of fine particles in ambient urban air of cities which are not directly influenced by industrial emissions. The aim of this work was to assess the influence of a major arterial road on concentration levels of airborne fine particles in its vicinity. Measurements of over 500 particle size distributions in the particle size range 16–626 nm, were made using two scanning mobility particle sizers (SMPS). A subsequent comparison of the recorded values from differing locations is discussed, with reference made to topographic and climatic influences. Both horizontal and vertical profile measurements of fine particle number size distributions are described; the combination of the two yielding information as to the relative exposures of occupants of buildings in the vicinity of a major arterial route. With the exception of measurements in close proximity to the freeway (about 15 m), the horizontal profile measurements did not provide any evidence of a statistically significant difference in fine particle number concentration with respect to distance at ground level up to a distance of 200 m within the study area. The vertical profile measurements also revealed no significant correlation between particle concentration and height. However, for buildings in the immediate proximity to the arterial road (about 15 m) concentrations around the building envelope are very high, comparable to those in the immediate vicinity of the road, indicating undiluted concentrations drawn directly from the freeway. This finding has a significant implication for management of indoor air quality in the buildings located in the immediate vicinity of major roads.     

Comparisons of aerosol properties measured by impactors and light scattering from individual particles: refractive index,number and volume concentrations,and size distributions

The southeastern aerosol and visibility study (SEAVS) was conducted in Great Smoky Mountains National Park in summer 1995 to investigate variations in ambient aerosol size distributions and their effect on visibility. In this paper, we compare dry aerosol size distribution parameters from a MOUDI impactor and two different optical particle counters (OPCs). Size distributions from the various instruments are expressed in a common measure of size, specifically, optical and aerodynamic diameters are converted to a dry, geometric diameter basis. Comparisons of the real part of particle refractive index obtained directly from light scattering measurements and inferred from aerosol composition measurements are also shown. Real refractive indices from direct measurements and those computed from measured fine aerosol chemical composition were generally within ±0.02. Maximum differences in estimated accumulation mode integrated volume concentrations from all instruments were within ∼22%. Accumulation mode integrated number concentrations and geometric standard deviations from the two OPCs agreed within ∼30% and ∼3%, respectively. Differences between MOUDI- and OPC-derived accumulation mode number concentrations and geometric standard deviations were ∼20% and ∼8%, respectively. The average geometric volume mean diameters derived from the three instruments agreed within 15% or less. The volume median diameters obtained by fitting the CSU number concentration data to a lognormal function were typically the smallest. We show that these discrepancies can be related to the differences and biases in the measurement and data analysis techniques.     

Size distributions of airborne microbes in moisture-damaged and reference school buildings of two construction types

Any risk assessment of moisture-damaged buildings requires an accurate characterization of the factors contributing to the human exposure. In this study, the size distributions of indoor air viable fungi and bacteria and average mean diameters of the most common fungi in school buildings were determined. One special focus was to analyze how the microbial size distributions are affected by the building frame (either wooden or concrete) and moisture damage in the building. The study was performed in 32 school buildings classified as moisture-damaged (index) and non-damaged (reference) schools according to technical building investigations. Sampling for indoor air microbes was carried out using a cascade impactor that collects particles on six stages (range from 0.65 to >7 μm) according to their aerodynamic diameters. Both wooden and concrete schools had their highest fungal levels in the size range of 1.1–4.7 μm. However, the concentrations of fungi in all size classes were higher in wooden schools than in concrete schools. Moisture damage-associated differences in size distribution, in the particle size range of 1.1–2.1 μm, were seen in concrete schools but not in wooden schools. In general, the average geometric mean diameter (d_g,ave) of total viable fungi was smaller in wooden schools than in concrete schools, and smaller in index schools of both construction types than in their reference schools. Variation in particle size, however, by genus was observed. No differences in particle size distributions of viable airborne bacteria were found. Our results on the dependency of the particle size on the building type and presence of moisture damage provide an interesting point to be considered in assessing the complex issue of indoor-related bioaerosol exposures.     

Variation of particle number and mass concentration in various size ranges of ambient aerosols in Eastern Germany

There is an ongoing debate on the question which size fraction of particles in ambient air may be responsible for short-term responses of the respiratory system as observed in several epidemiological studies. However, the available data on ambient particle concentrations in various size ranges are not sufficient to answer this question.Therefore, on 180 days during the winter 1991/92 daily mean size distributions of ambient particles were determined in. Erfurt, a city in Eastern Germany. In the range 0.01–0.3 μm particles were classified by an electrical mobility analyzer and in the range 0.1–2.5 μm by an optical particle counter. From the derived size distributions, number and mass concentrations were calculated.The mean number concentration over this period of time was governed by particles smaller than 0.1 μm (72%), whereas the mean mass concentration was governed by particles in the size range 0.1–0.5 pm (83%). The contribution of particles larger than 0.5 μm to the overall number concentration was negligible and so was the contribution of particles smaller than 0.1 μm to the overall mass concentration. Furthermore, total number and mass concentrations in the range 0.01–2.5 μm were poorly correlated.The results suggest that particles larger than 2.5 μm (or even larger than 0.5 μm) are rare in the European urban environment so that the inhalation of these particles is probably not relevant for human health. Since particle number and mass concentrations can be considered poorly correlated variables, more insight into health-related aspects of particulate air pollution will be obtained by correlating respiratory responses with mass and number concentrations of ambient particles below 0.5 μm.     

A detailed numerical study of the evolution of soot particle size distributions in laminar premixed flames

In this work, two numerical techniques, viz. the method of moments and a discrete h-p-Galerkin method, have been applied for numerical simulation of soot formation in a laminar premixed acetylene/oxygen/argon flame. From the evolution of the PAH and the soot particle size distributions, new insight into the different processes of soot formation is provided. For this, the single submodels have been examined with respect to their influence on the PAH and the soot particle size distributions. The particle inception step was studied in detail by comparing the simulated PAH size distributions with experimental results. Additionally, an estimation of the interaction energy of layered PAH dimers was performed by quantum chemical calculations. From these results, some evidence for the particle inception model employing coalescence of PAH molecules has been found. The numerical results for the gas phase chemical species, the particle number densities and volume fractions of soot as well as for the soot particle size distributions are compared with experimental data. Thereby, the consistency of the entire model is demonstrated.     

Experiments probing the influence of air exchange rates on secondary organic aerosols derived from indoor chemistry

Reactions between ozone and terpenes have been shown to increase the concentrations of submicron particles in indoor settings. The present study was designed to examine the influence of air exchange rates on the concentrations of these secondary organic aerosols as well as on the evolution of their particle size distributions. The experiments were performed in a manipulated office setting containing a constant source of d-limonene and an ozone generator that was remotely turned “on” or “off” at 6 h intervals. The particle number concentrations were monitored using an optical particle counter with eight-channels ranging from 0.1–0.2 to>2.0 μm diameter. The air exchange rates during the experiments were either high (working hours) or low (non-working hours) and ranged from 1.6 to>12 h⁻¹, with intermediate exchange rates. Given the emission rates of ozone and d-limonene used in these studies, at an air exchange rate of 1.6 h⁻¹ particle number concentration in the 0.1–0.2 μm size-range peaked 1.2 h after the ozone generator was switched on. In the ensuing 4.8 h particle counts increased in successive size-ranges up to the 0.5–0.7 μm diameter range. At higher air exchange rates, the resulting concentrations of total particles and particle mass (calculated from particle counts) were smaller, and at exchange rates exceeding 12 h⁻¹, no excess particle formation was detectable with the instrument used in this study. Particle size evolved through accretion and, in some cases, coagulation. There was evidence for coagulation among particles in the smallest size-range at low air exchange rates (high particle concentrations) but no evidence of coagulation was apparent at higher air exchange rates (lower particle concentrations). At higher air exchange rates the particle count or size distributions were shifted towards smaller particle diameters and less time was required to achieve the maximum concentration in each of the size-ranges where discernable particle growth occurred. These results illustrate still another way in which ventilation affects human exposures in indoor settings. However, the ultimate effects of these exposures on health and well being remain to be determined.     

A closure study of extinction apportionment by multiple regression

Multiple regression has been widely used to apportion particle light scattering among distinct chemical species. The resulting scattering budgets are shown here to be unbiased estimates under certain theoretical conditions. The theory allows species’ particle size distributions and water uptakes to vary from sample to sample, as they are known to do in reality. The sole constraint is that variations in each species’ characteristics be statistically independent of all species’ concentrations. Individual violations of this condition cause identifiable biases, and multiple violations can offset each other to yield regression estimates that are accurate by accident. Detailed and summary accountings of statistical errors are illustrated using a mechanistic model derived from measurements in southern California.     

Contamination from electrically conductive silicone tubing during aerosol chemical analysis

Electrically conductive silicone tubing is used to minimize losses in sampling lines during the analysis of airborne particle size distributions and number concentrations. We report contamination from this tubing using gas chromatography–mass spectrometry (GC–MS) of filter-collected samples as well as by particle mass spectrometry. Comparison of electrically conductive silicone and stainless steel tubing showed elevated siloxanes only for the silicone tubing. The extent of contamination increased with length of tubing to which the sample was exposed, and decreased with increasing relative humidity.     

New particle formation in the Midwestern USA: Event characteristics,meteorological context and vertical profiles

Two years of continuous particle size distribution measurements at three heights over and in a deciduous forest in southern Indiana exhibit evidence of particle nucleation on 46% of classifiable days, and clear nucleation with consistent subsequent growth on 14% of days. Events characterized by high ultra-fine particle production and clear growth are most frequent in spring. These events most frequently follow cold front passages and exhibit a higher frequency of northerly back-trajectories. Local meteorological conditions, as described using the Nucleation Parameter (NP) of Boy and Kulmala (2002) and stability indices, indicate a significant association with ultra-fine particle concentrations, and specifically that nucleation was frequently preceded by destabilization of the atmosphere consistent with entrainment of elevated pollution layers. There appears to be little or no dependence of nucleation frequency or intensity on the in situ condensational sink particularly during spring, which is consistent with very high regional emissions of the precursors of ternary nucleation. Vertical gradients of particle size distributions exhibit evidence for nucleation being focused above canopy and accordingly mean ratios of above and below canopy concentrations of ultra-fine particles (6–30 nm) just subsequent to nucleation are 1.8 and 1.7 respectively during leaf-on and leaf-off periods. The difference in vertical concentration ratios during leaf-on and leaf-off are used to infer that of the order of 25% of ultra-fine particles are captured by foliar elements in the canopy during turbulent mixing through the canopy.     

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.