Dissertations / Theses on the topic 'Particle emissions'

Biomass burning started to attract attention since the last decade because of its impacts on the atmosphere and the environmental air quality, as well as significant potential effects on human health and global climate change. Knowledge of particle emission characteristics from biomass burning is crucially important for the quantitative assessment of the potential impacts. This thesis presents the results of study aimed towards comprehensive characterization of particle emissions from biomass burning. The study was conducted both under controlled laboratory conditions, to quantify the particle size distribution and emission factors by taking into account various factors which may affect the particle characteristics, and in the field, to investigate biomass burning processes in the real life situations and to examine vertical profile of particles in the atmosphere. To simulate different environmental conditions, a new technique has been developed for investigating particle emissions from biomass burning in the laboratory. As biomass burning may occur in a field at various wind speeds and burning rates, the technique was designed to allow adjustment of the flow rates of the air introduced into the chamber, in order to control burning under different conditions. In addition, the technique design has enabled alteration of the high particle concentrations, allowing conducting measurements with the instrumentations that had the upper concentration limits exciding the concentrations characteristic to the biomass burning. The technique was applied to characterize particle emissions from burning of several tree species common to Australian forests. The aerosol particles were characterized in terms of size distribution and emission factors, such as PM2.5 particle mass emission factor and particle number emission factor, under various burning conditions. The characteristics of particles over a range of burning phases (e.g., ignition, flaming, and smoldering) were also investigated. The results showed that particle characteristics depend on the type of tree, part of tree, and the burning rate. In particular, fast burning of the wood samples produced particles with the CMD of 60 nm during the ignition phase and 30 nm for the rest of the burning process. Slow burning of the wood samples produced large particles with the CMD of 120 nm, 60 nm and 40 nm for the ignition, flaming and smoldering phases, respectively. The CMD of particles emitted by burning the leaves and branches was found to be 50 nm for the flaming phase and 30 nm for the smoldering phase, under fast burning conditions. Under slow burning conditions, the CMD of particles was found to be between 100 to 200 nm for the ignition and flaming phase, and 50 nm for the smoldering phase. For fast burning, the average particle number emission factors were between 3.3 to 5.7 x 1015 particles/kg for wood and 0.5 to 6.9 x 1015 particles/kg for leaves and branches. The PM2.5 emission factors were between 140 to 210 mg/kg for wood and 450 to 4700 mg/kg for leaves and branches. For slow burning conditions, the average particle number emission factors were between 2.8 to 44.8 x 1013 particles/kg for wood and 0.5 to 9.3 x 1013 particles/kg for leaves and branches, and the PM2.5 emissions factors were between 120 to 480 mg/kg for wood and 3300 to 4900 mg/kg for leaves and branches. The field measurements were conducted to investigate particle emissions from biomass burning in the Northern Territory of Australia over dry seasons. The results of field studies revealed that diameters of particles in ambient air emissions were within the size range observed during laboratory investigations. The laboratory measurements found that the particles released during the controlled burning were of a diameter between 30 and 210 nm, depending on the burning conditions. Under fast burning conditions, smaller particles were produced with a diameter in the range of 30 to 60 nm, whilst larger particles, with a diameter between 60 nm and 210 nm, were produced during slow burning. The airborne field measurements of biomass particles found that most of the particles measured under the boundary layer had a CMD of (83 ± 13) nm during the early dry season (EDS), and (127 ± 6) nm during the late dry season (LDS). The characteristics of ambient particles were found to be significantly different at the EDS and the LDS due to several factors including moisture content of vegetation, location of fires related to the flight paths, intensity of fires, and burned areas. Specifically, the investigations of the vertical profiles of particles in the atmosphere have revealed significant differences in the particle properties during early dry season and late dry season. The characteristics of particle size distribution played a significant role in these differences.

Biomass burning started to attract attention since the last decade because of its impacts on the atmosphere and the environmental air quality, as well as significant potential effects on human health and global climate change. Knowledge of particle emission characteristics from biomass burning is crucially important for the quantitative assessment of the potential impacts. This thesis presents the results of study aimed towards comprehensive characterization of particle emissions from biomass burning. The study was conducted both under controlled laboratory conditions, to quantify the particle size distribution and emission factors by taking into account various factors which may affect the particle characteristics, and in the field, to investigate biomass burning processes in the real life situations and to examine vertical profile of particles in the atmosphere. To simulate different environmental conditions, a new technique has been developed for investigating particle emissions from biomass burning in the laboratory. As biomass burning may occur in a field at various wind speeds and burning rates, the technique was designed to allow adjustment of the flow rates of the air introduced into the chamber, in order to control burning under different conditions. In addition, the technique design has enabled alteration of the high particle concentrations, allowing conducting measurements with the instrumentations that had the upper concentration limits exciding the concentrations characteristic to the biomass burning. The technique was applied to characterize particle emissions from burning of several tree species common to Australian forests. The aerosol particles were characterized in terms of size distribution and emission factors, such as PM2.5 particle mass emission factor and particle number emission factor, under various burning conditions. The characteristics of particles over a range of burning phases (e.g., ignition, flaming, and smoldering) were also investigated. The results showed that particle characteristics depend on the type of tree, part of tree, and the burning rate. In particular, fast burning of the wood samples produced particles with the CMD of 60 nm during the ignition phase and 30 nm for the rest of the burning process. Slow burning of the wood samples produced large particles with the CMD of 120 nm, 60 nm and 40 nm for the ignition, flaming and smoldering phases, respectively. The CMD of particles emitted by burning the leaves and branches was found to be 50 nm for the flaming phase and 30 nm for the smoldering phase, under fast burning conditions. Under slow burning conditions, the CMD of particles was found to be between 100 to 200 nm for the ignition and flaming phase, and 50 nm for the smoldering phase. For fast burning, the average particle number emission factors were between 3.3 to 5.7 x 1015 particles/kg for wood and 0.5 to 6.9 x 1015 particles/kg for leaves and branches. The PM2.5 emission factors were between 140 to 210 mg/kg for wood and 450 to 4700 mg/kg for leaves and branches. For slow burning conditions, the average particle number emission factors were between 2.8 to 44.8 x 1013 particles/kg for wood and 0.5 to 9.3 x 1013 particles/kg for leaves and branches, and the PM2.5 emissions factors were between 120 to 480 mg/kg for wood and 3300 to 4900 mg/kg for leaves and branches. The field measurements were conducted to investigate particle emissions from biomass burning in the Northern Territory of Australia over dry seasons. The results of field studies revealed that diameters of particles in ambient air emissions were within the size range observed during laboratory investigations. The laboratory measurements found that the particles released during the controlled burning were of a diameter between 30 and 210 nm, depending on the burning conditions. Under fast burning conditions, smaller particles were produced with a diameter in the range of 30 to 60 nm, whilst larger particles, with a diameter between 60 nm and 210 nm, were produced during slow burning. The airborne field measurements of biomass particles found that most of the particles measured under the boundary layer had a CMD of (83 ± 13) nm during the early dry season (EDS), and (127 ± 6) nm during the late dry season (LDS). The characteristics of ambient particles were found to be significantly different at the EDS and the LDS due to several factors including moisture content of vegetation, location of fires related to the flight paths, intensity of fires, and burned areas. Specifically, the investigations of the vertical profiles of particles in the atmosphere have revealed significant differences in the particle properties during early dry season and late dry season. The characteristics of particle size distribution played a significant role in these differences.

Vehicle emitted particles are of significant concern based on their potential to influence local air quality and human health. Transport microenvironments usually contain higher vehicle emission concentrations compared to other environments, and people spend a substantial amount of time in these microenvironments when commuting. Currently there is limited scientific knowledge on particle concentration, passenger exposure and the distribution of vehicle emissions in transport microenvironments, partially due to the fact that the instrumentation required to conduct such measurements is not available in many research centres. Information on passenger waiting time and location in such microenvironments has also not been investigated, which makes it difficult to evaluate a passenger’s spatial-temporal exposure to vehicle emissions. Furthermore, current emission models are incapable of rapidly predicting emission distribution, given the complexity of variations in emission rates that result from changes in driving conditions, as well as the time spent in driving condition within the transport microenvironment. In order to address these scientific gaps in knowledge, this work conducted, for the first time, a comprehensive statistical analysis of experimental data, along with multi-parameter assessment, exposure evaluation and comparison, and emission model development and application, in relation to traffic interrupted transport microenvironments. The work aimed to quantify and characterise particle emissions and human exposure in the transport microenvironments, with bus stations and a pedestrian crossing identified as suitable research locations representing a typical transport microenvironment. Firstly, two bus stations in Brisbane, Australia, with different designs, were selected to conduct measurements of particle number size distributions, particle number and PM2.5 concentrations during two different seasons. Simultaneous traffic and meteorological parameters were also monitored, aiming to quantify particle characteristics and investigate the impact of bus flow rate, station design and meteorological conditions on particle characteristics at stations. The results showed higher concentrations of PN20-30 at the station situated in an open area (open station), which is likely to be attributed to the lower average daily temperature compared to the station with a canyon structure (canyon station). During precipitation events, it was found that particle number concentration in the size range 25-250 nm decreased greatly, and that the average daily reduction in PM2.5 concentration on rainy days compared to fine days was 44.2 % and 22.6 % at the open and canyon station, respectively. The effect of ambient wind speeds on particle number concentrations was also examined, and no relationship was found between particle number concentration and wind speed for the entire measurement period. In addition, 33 pairs of average half-hourly PN7-3000 concentrations were calculated and identified at the two stations, during the same time of a day, and with the same ambient wind speeds and precipitation conditions. The results of a paired t-test showed that the average half-hourly PN7-3000 concentrations at the two stations were not significantly different at the 5% confidence level (t = 0.06, p = 0.96), which indicates that the different station designs were not a crucial factor for influencing PN7-3000 concentrations. A further assessment of passenger exposure to bus emissions on a platform was evaluated at another bus station in Brisbane, Australia. The sampling was conducted over seven weekdays to investigate spatial-temporal variations in size-fractionated particle number and PM2.5 concentrations, as well as human exposure on the platform. For the whole day, the average PN13-800 concentration was 1.3 x 104 and 1.0 x 104 particle/cm3 at the centre and end of the platform, respectively, of which PN50-100 accounted for the largest proportion to the total count. Furthermore, the contribution of exposure at the bus station to the overall daily exposure was assessed using two assumed scenarios of a school student and an office worker. It was found that, although the daily time fraction (the percentage of time spend at a location in a whole day) at the station was only 0.8 %, the daily exposure fractions (the percentage of exposures at a location accounting for the daily exposure) at the station were 2.7% and 2.8 % for exposure to PN13-800 and 2.7% and 3.5% for exposure to PM2.5 for the school student and the office worker, respectively. A new parameter, “exposure intensity” (the ratio of daily exposure fraction and the daily time fraction) was also defined and calculated at the station, with values of 3.3 and 3.4 for exposure to PN13-880, and 3.3 and 4.2 for exposure to PM2.5, for the school student and the office worker, respectively. In order to quantify the enhanced emissions at critical locations and define the emission distribution in further dispersion models for traffic interrupted transport microenvironments, a composite line source emission (CLSE) model was developed to specifically quantify exposure levels and describe the spatial variability of vehicle emissions in traffic interrupted microenvironments. This model took into account the complexity of vehicle movements in the queue, as well as different emission rates relevant to various driving conditions (cruise, decelerate, idle and accelerate), and it utilised multi-representative segments to capture the accurate emission distribution for real vehicle flow. This model does not only helped to quantify the enhanced emissions at critical locations, but it also helped to define the emission source distribution of the disrupted steady flow for further dispersion modelling. The model then was applied to estimate particle number emissions at a bidirectional bus station used by diesel and compressed natural gas fuelled buses. It was found that the acceleration distance was of critical importance when estimating particle number emission, since the highest emissions occurred in sections where most of the buses were accelerating and no significant increases were observed at locations where they idled. It was also shown that emissions at the front end of the platform were 43 times greater than at the rear of the platform. The CLSE model was also applied at a signalled pedestrian crossing, in order to assess increased particle number emissions from motor vehicles when forced to stop and accelerate from rest. The CLSE model was used to calculate the total emissions produced by a specific number and mix of light petrol cars and diesel passenger buses including 1 car travelling in 1 direction (/1 direction), 14 cars / 1 direction, 1 bus / 1 direction, 28 cars / 2 directions, 24 cars and 2 buses / 2 directions, and 20 cars and 4 buses / 2 directions. It was found that the total emissions produced during stopping on a red signal were significantly higher than when the traffic moved at a steady speed. Overall, total emissions due to the interruption of the traffic increased by a factor of 13, 11, 45, 11, 41, and 43 for the above 6 cases, respectively. In summary, this PhD thesis presents the results of a comprehensive study on particle number and mass concentration, together with particle size distribution, in a bus station transport microenvironment, influenced by bus flow rates, meteorological conditions and station design. Passenger spatial-temporal exposure to bus emitted particles was also assessed according to waiting time and location along the platform, as well as the contribution of exposure at the bus station to overall daily exposure. Due to the complexity of the interrupted traffic flow within the transport microenvironments, a unique CLSE model was also developed, which is capable of quantifying emission levels at critical locations within the transport microenvironment, for the purpose of evaluating passenger exposure and conducting simulations of vehicle emission dispersion. The application of the CLSE model at a pedestrian crossing also proved its applicability and simplicity for use in a real-world transport microenvironment.

Doutoramento em Ciências e Engenharia do Ambiente
Os incêndios florestais são uma importante fonte de emissão de compostos gasosos e de aerossóis. Em Portugal, onde a maioria dos incêndios ocorre no norte e centro do país, os incêndios destroem todos os anos milhares de hectares, com importantes perdas em termos económicos, de vidas humanas e qualidade ambiental. As emissões podem alterar consideravelmente a química da atmosfera, degradar a qualidade do ar e alterar o clima. Contudo, a informação sobre as caraterísticas das emissões dos incêndios florestais nos países do Mediterrâneo é limitada. Tanto a nível nacional como internacional, existe um interesse crescente na elaboração de inventários de emissões e de regulamentos sobre as emissões de carbono para a atmosfera. Do ponto de vista atmosférico da monitorização atmosférica, os incêndios são considerados um desafio, dada a sua variabilidade temporal e espacial, sendo de esperar um aumento da sua frequência, dimensão e severidade, e também porque as estimativas de emissões dependem das caraterísticas dos biocombustíveis e da fase de combustão. O objetivo deste estudo foi quantificar e caraterizar as emissões de gases e aerossóis de alguns dos mais representativos incêndios florestais que ocorreram no centro de Portugal nos verões de 2009 e de 2010. Efetuou-se a colheita de amostras de gases e de duas frações de partículas (PM2.5 e PM2.5-10) nas plumas de fumo em sacos Tedlar e em filtros de quartzo acoplados a um amostrador de elevado volume, respetivamente. Os hidrocarbonetos totais (THC) e óxidos de carbono (CO e CO2) nas amostras gasosas foram analisados em instrumentos automáticos de ionização de chama e detetores não dispersivos de infravermelhos, respetivamente. Para algumas amostras, foram também quantificados alguns compostos de carbonilo após reamostragem do gás dos sacos Tedlar em cartuchos de sílica gel revestidos com 2,4-dinitrofenilhidrazina (DNPH), seguida de análise por cromatografia líquida de alta resolução. Nas partículas, analisou-se o carbono orgânico e elementar (técnica termo-óptica), iões solúveis em água (cromatografia iónica) e elementos (espectrometria de massa com plasma acoplado por indução ou análise instrumental por ativação com neutrões). A especiação orgânica foi obtida por cromatografia gasosa acoplada a espectrometria de massa após extração com recurso a vários solventes e separação dos extratos orgânicos em diversas classes de diferentes polaridades através do fracionamento com sílica gel. Os fatores de emissão do CO e do CO2 situaram-se nas gamas 52-482 e 822-1690 g kg-1 (base seca), mostrando, respetivamente, correlação negativa e positiva com a eficiência de combustão. Os fatores de emissão dos THC apresentaram valores mais elevados durante a fase de combustão latente sem chama, oscilando entre 0.33 e 334 g kg-1 (base seca). O composto orgânico volátil oxigenado mais abundante foi o acetaldeído com fatores de emissão que variaram desde 1.0 até 3.2 g kg-1 (base seca), seguido pelo formaldeído e o propionaldeído. Observou-se que as emissões destes compostos são promovidas durante a fase de combustão latente sem chama. Os fatores de emissão de PM2.5 e PM10 registaram valores entre 0.50-68 e 0.86-72 g kg-1 (base seca), respetivamente. A emissão de partículas finas e grosseiras é também promovida em condições de combustão lenta. As PM2.5 representaram cerca de 90% da massa de partículas PM10. A fração carbonosa das partículas amostradas em qualquer dos incêndios foi claramente dominada pelo carbono orgânico. Foi obtida uma ampla gama de rácios entre o carbono orgânico e o carbono elementar, dependendo das condições de combustão. Contudo, todos os rácios refletiram uma maior proporção de carbono orgânico em relação ao carbono elementar, típica das emissões de queima de biomassa. Os iões solúveis em água obtidos nas partículas da pluma de fumo contribuíram com valores até 3.9% da massa de partículas PM2.5 e 2.8% da massa de partículas de PM2.5-10. O potássio contribuiu com valores até 15 g mg-1 PM2.5 e 22 g mg-1 PM2.5-10, embora em massa absoluta estivesse maioritariamente presente nas partículas finas. Os rácios entre potássio e carbono elementar e entre potássio e carbono orgânico obtidos nas partículas da pluma de fumo enquadram-se na gama de valores relatados na literatura para emissões de queima de biomassa. Os elementos detetados nas amostras representaram, em média, valores até 1.2% e 12% da massa de PM2.5 e PM2.5-10, respetivamente. Partículas resultantes de uma combustão mais completa (valores elevados de CO2 e baixos de CO) foram caraterizadas por um elevado teor de constituintes inorgânicos e um menor conteúdo de matéria orgânica. Observou-se que a matéria orgânica particulada é composta principalmente por componentes fenólicos e produtos derivados, séries de compostos homólogos (alcanos, alcenos, ácidos alcanóicos e alcanóis), açúcares, biomarcadores esteróides e terpenóides, e hidrocarbonetos aromáticos policíclicos. O reteno, um biomarcador das emissões da queima de coníferas, foi o hidrocarboneto aromático dominante nas amostras das plumas de fumo amostradas durante a campanha que decorreu em 2009, devido ao predomínio de amostras colhidas em incêndios em florestas de pinheiros. O principal açúcar anidro, e sempre um dos compostos mais abundantes, foi o levoglucosano. O rácio levoglucosano/OC obtido nas partículas das plumas de fumo, em média, registaram valores desde 5.8 a 23 mg g-1 OC. Os rácios levoglucosano/manosano e levoglucosano/(manosano+galactosano) revelaram o predomínio de amostras provenientes da queima de coníferas. Tendo em conta que a estimativa das emissões dos incêndios florestais requer um conhecimento de fatores de emissão apropriados para cada biocombustível, a base de dados abrangente obtida neste estudo é potencialmente útil para atualizar os inventários de emissões. Tem vindo a ser observado que a fase de combustão latente sem chama, a qual pode ocorrer simultaneamente com a fase de chama e durar várias horas ou dias, pode contribuir para uma quantidade considerável de poluentes atmosféricos, pelo que os fatores de emissão correspondentes devem ser considerados no cálculo das emissões globais de incêndios florestais. Devido à falta de informação detalhada sobre perfis químicos de emissão, a base de dados obtida neste estudo pode também ser útil para a aplicação de modelos no recetor no sul da Europa.
Wildfires are an importante emission source of gaseous compounds and aerosol particles. In Portugal, where most fire events occur in northern and central areas of the country, wildfires destroy every year thousands of hectares, with important losses in terms of economic disruptions, human lives and environmental quality. Emissions can substantially perturb atmospheric chemistry, degrade air quality and alter weather and climate. However, limited data exist on the emission characteristics from this source in Mediterranean countries. At both national and international levels, there is an increasing focus on the establishment of emission inventories and regulations of regional carbon emissions to the atmosphere. From the standpoint of atmospherically-based carbon monitoring programs, fires are challenging because they tend to be extremely variable in intensity, space and time, they are expected to increase in number and severity in the future, and because emission estimates depend on biofuel characteristics and combustion phase. The aim of this study was to quantify and characterise the emissions of trace gases and aerosol particles from some of the most representative wildfires that occurred in central Portugal during the summers of 2009 and 2010. Gases and particles of two size fractions (PM2.5 and PM2.5-10) were collected from the smoke plumes in Tedlar bags and on quartz filters mounted on a high volume sampler, respectively. The gaseous compounds were subsequently analised for total hydrocarbons (THC) and carbon oxides (CO and CO2) in automatic instruments with flame ionisation and non-dispersive infrared detectors, respectively. For some smoke samples, carbonyls were also quantified after drawing air from the Tedlar bags through cartridges containing silica gel coated with 2,4-dinitrophenylhydrazine (DNPH) reagent and followed by analysis by high performace liquid chromatography. Particles were analysed for organic and elemental carbon (thermal-optical technique), water-soluble ions (ion chromatography) and trace elements (inductively coupled plasma mass spectrometry or instrumental neutron activation analysis). The organic speciation was obtained by gas chromatography coupled to mass spectrometry after multi-solvent extraction and separation of the organic extracts into several classes of different polarities by flash chromatography on silica gel. The CO and CO2 emission factors were in the ranges 52-482 and 822-1690 g kg-1 (dry basis), showing, respectively, negative and positive correlations with the combustion efficiency. The THC emission factors were higher during smouldering conditions with values ranging between 0.33 and 334 g kg-1 (dry basis). The most abundant oxygenated volatile organic compound measured was acetaldehyde with emission factors ranging from 1.0 to 3.2 g kg-1 (dry basis), followed by formaldehyde and propionaldehyde. The emission of these compounds were enhanced during the smouldering phase. PM2.5 and PM10 emission factors were in the ranges 0.50-68 and 0.86-72 g kg-1 (dry basis), respectively. The emission of fine and coarse particles was promoted by smouldering combustion conditions. PM2.5 particles contributed to around 90% of the PM10 mass. The carbonaceous fraction of smoke particulate samples from any of the fires was clearly dominated by organic carbon. A wide range of organic carbon-to-elemental carbon concentration ratios was obtained, depending on the combustion conditions. However, all the ratios reflected a much higher proportion of organic carbon in relation to elemental carbon, typical of biomass burning emissions. The water-soluble ions obtained in smoke particles contributed with values up to 3.9% of the PM2.5 and 2.8% of the PM2.5-10 particles. Potassium contributed up to 15 g mg-1 PM2.5 and 22 g mg-1 PM2.5-10, although in absolute mass it was overwhelmingly present in fine particles. The potassium-to-elemental carbon and potassium-to-organic carbon ratios obtained in smoke particles were in accordance with those reported in the literature for biomass burning sources. Trace elements detected in smoke samples represented, on average, up to 1.2% and 12% of the PM2.5 and PM2.5-10 mass, respectively. Particles from a more complete combustion (higher CO2 and lower CO values) were characterised by a higher content of inorganic constituents and a lower organic content. The particulate organic matter was mainly composed of phenolic compounds and their alteration products, homologous series (n-alkanes, n-alkenes, n-alkanoic acids and n-alkanols), sugar constituents, steroid and terpenoid biomarkers, and polycyclic aromatic hydrocarbons. Retene, a biomarker of softwood smoke, was the dominant aromatic hydrocarbon in smoke samples collected during the 2009 campaign, due to a predominance of samples from wildfires in pine forests. The major anhydrosugar, and always one of the most abundant compounds, was levoglucosan. The levoglucosan/OC ratio obtained in the smoke particles, on average, ranged from 5.8 to 23 mg g-1 OC. The levoglucosan-to-mannosan and the levoglucosan-to-mannosan plus galactosan ratios determined reveal a predominance of samples from softwood combustion. Since estimation of wildfire emissions requires knowledge of fuel-appropriate emissions factors, the comprehensive database obtained in this study is potentially useful to update the current emission inventories. It has been observed that the smouldering phase, which can occur simultaneously with the flaming front and continue for several hours to days, may contribute to significant amounts of atmospheric pollutants and the corresponding emission factors should be considered when calculating the global wildfire emissions. Due to the lack of detailed emission profiles, the databases obtained in this study can also be very helpful for receptor modelling in southern Europe.

Emissions from airport operations are of significant concern because of their potential impact on local air quality and human health. The currently limited scientific knowledge of aircraft emissions is an important issue worldwide, when considering air pollution associated with airport operation, and this is especially so for ultrafine particles. This limited knowledge is due to scientific complexities associated with measuring aircraft emissions during normal operations on the ground. In particular this type of research has required the development of novel sampling techniques which must take into account aircraft plume dispersion and dilution as well as the various particle dynamics that can affect the measurements of the aircraft engine plume from an operational aircraft. In order to address this scientific problem, a novel mobile emission measurement method called the Plume Capture and Analysis System (PCAS), was developed and tested. The PCAS permits the capture and analysis of aircraft exhaust during ground level operations including landing, taxiing, takeoff and idle. The PCAS uses a sampling bag to temporarily store a sample, providing sufficient time to utilize sensitive but slow instrumental techniques to be employed to measure gas and particle emissions simultaneously and to record detailed particle size distributions. The challenges in relation to the development of the technique include complexities associated with the assessment of the various particle loss and deposition mechanisms which are active during storage in the PCAS. Laboratory based assessment of the method showed that the bag sampling technique can be used to accurately measure particle emissions (e.g. particle number, mass and size distribution) from a moving aircraft or vehicle. Further assessment of the sensitivity of PCAS results to distance from the source and plume concentration was conducted in the airfield with taxiing aircraft. The results showed that the PCAS is a robust method capable of capturing the plume in only 10 seconds. The PCAS is able to account for aircraft plume dispersion and dilution at distances of 60 to 180 meters downwind of moving a aircraft along with particle deposition loss mechanisms during the measurements. Characterization of the plume in terms of particle number, mass (PM2.5), gaseous emissions and particle size distribution takes only 5 minutes allowing large numbers of tests to be completed in a short time. The results were broadly consistent and compared well with the available data. Comprehensive measurements and analyses of the aircraft plumes during various modes of the landing and takeoff (LTO) cycle (e.g. idle, taxi, landing and takeoff) were conducted at Brisbane Airport (BNE). Gaseous (NOx, CO2) emission factors, particle number and mass (PM2.5) emission factors and size distributions were determined for a range of Boeing and Airbus aircraft, as a function of aircraft type and engine thrust level. The scientific complexities including the analysis of the often multimodal particle size distributions to describe the contributions of different particle source processes during the various stages of aircraft operation were addressed through comprehensive data analysis and interpretation. The measurement results were used to develop an inventory of aircraft emissions at BNE, including all modes of the aircraft LTO cycle and ground running procedures (GRP). Measurements of the actual duration of aircraft activity in each mode of operation (time-in-mode) and compiling a comprehensive matrix of gas and particle emission rates as a function of aircraft type and engine thrust level for real world situations was crucial for developing the inventory. The significance of the resulting matrix of emission rates in this study lies in the estimate it provides of the annual particle emissions due to aircraft operations, especially in terms of particle number. In summary, this PhD thesis presents for the first time a comprehensive study of the particle and NOx emission factors and rates along with the particle size distributions from aircraft operations and provides a basis for estimating such emissions at other airports. This is a significant addition to the scientific knowledge in terms of particle emissions from aircraft operations, since the standard particle number emissions rates are not currently available for aircraft activities.

Emissions from airport operations are of significant concern because of their potential impact on local air quality and human health. The currently limited scientific knowledge of aircraft emissions is an important issue worldwide, when considering air pollution associated with airport operation, and this is especially so for ultrafine particles. This limited knowledge is due to scientific complexities associated with measuring aircraft emissions during normal operations on the ground. In particular this type of research has required the development of novel sampling techniques which must take into account aircraft plume dispersion and dilution as well as the various particle dynamics that can affect the measurements of the aircraft engine plume from an operational aircraft. In order to address this scientific problem, a novel mobile emission measurement method called the Plume Capture and Analysis System (PCAS), was developed and tested. The PCAS permits the capture and analysis of aircraft exhaust during ground level operations including landing, taxiing, takeoff and idle. The PCAS uses a sampling bag to temporarily store a sample, providing sufficient time to utilize sensitive but slow instrumental techniques to be employed to measure gas and particle emissions simultaneously and to record detailed particle size distributions. The challenges in relation to the development of the technique include complexities associated with the assessment of the various particle loss and deposition mechanisms which are active during storage in the PCAS. Laboratory based assessment of the method showed that the bag sampling technique can be used to accurately measure particle emissions (e.g. particle number, mass and size distribution) from a moving aircraft or vehicle. Further assessment of the sensitivity of PCAS results to distance from the source and plume concentration was conducted in the airfield with taxiing aircraft. The results showed that the PCAS is a robust method capable of capturing the plume in only 10 seconds. The PCAS is able to account for aircraft plume dispersion and dilution at distances of 60 to 180 meters downwind of moving a aircraft along with particle deposition loss mechanisms during the measurements. Characterization of the plume in terms of particle number, mass (PM2.5), gaseous emissions and particle size distribution takes only 5 minutes allowing large numbers of tests to be completed in a short time. The results were broadly consistent and compared well with the available data. Comprehensive measurements and analyses of the aircraft plumes during various modes of the landing and takeoff (LTO) cycle (e.g. idle, taxi, landing and takeoff) were conducted at Brisbane Airport (BNE). Gaseous (NOx, CO2) emission factors, particle number and mass (PM2.5) emission factors and size distributions were determined for a range of Boeing and Airbus aircraft, as a function of aircraft type and engine thrust level. The scientific complexities including the analysis of the often multimodal particle size distributions to describe the contributions of different particle source processes during the various stages of aircraft operation were addressed through comprehensive data analysis and interpretation. The measurement results were used to develop an inventory of aircraft emissions at BNE, including all modes of the aircraft LTO cycle and ground running procedures (GRP). Measurements of the actual duration of aircraft activity in each mode of operation (time-in-mode) and compiling a comprehensive matrix of gas and particle emission rates as a function of aircraft type and engine thrust level for real world situations was crucial for developing the inventory. The significance of the resulting matrix of emission rates in this study lies in the estimate it provides of the annual particle emissions due to aircraft operations, especially in terms of particle number. In summary, this PhD thesis presents for the first time a comprehensive study of the particle and NOx emission factors and rates along with the particle size distributions from aircraft operations and provides a basis for estimating such emissions at other airports. This is a significant addition to the scientific knowledge in terms of particle emissions from aircraft operations, since the standard particle number emissions rates are not currently available for aircraft activities.

Due to their large surface area, complex chemical composition and high alveolar deposition rate, ultrafine particles (UFPs) (< 0.1 ìm) pose a significant risk to human health and their toxicological effects have been acknowledged by the World Health Organisation. Since people spend most of their time indoors, there is a growing concern about the UFPs present in some indoor environments. Recent studies have shown that office machines, in particular laser printers, are a significant indoor source of UFPs. The majority of printer-generated UFPs are organic carbon and it is unlikely that these particles are emitted directly from the printer or its supplies (such as paper and toner powder). Thus, it was hypothesised that these UFPs are secondary organic aerosols (SOA). Considering the widespread use of printers and human exposure to these particles, understanding the processes involved in particle formation is of critical importance. However, few studies have investigated the nature (e.g. volatility, hygroscopicity, composition, size distribution and mixing state) and formation mechanisms of these particles. In order to address this gap in scientific knowledge, a comprehensive study including state-of-art instrumental methods was conducted to characterise the real-time emissions from modern commercial laser printers, including particles, volatile organic compounds (VOCs) and ozone (O3). The morphology, elemental composition, volatility and hygroscopicity of generated particles were also examined. The large set of experimental results was analysed and interpreted to provide insight into: (1) Emissions profiles of laser printers: The results showed that UFPs dominated the number concentrations of generated particles, with a quasi unimodal size distribution observed for all tests. These particles were volatile, non-hygroscopic and mixed both externally and internally. Particle microanalysis indicated that semi-volatile organic compounds occupied the dominant fraction of these particles, with only trace quantities of particles containing Ca and Fe. Furthermore, almost all laser printers tested in this study emitted measurable concentrations of VOCs and O3. A positive correlation between submicron particles and O3 concentrations, as well as a contrasting negative correlation between submicron particles and total VOC concentrations were observed during printing for all tests. These results proved that UFPs generated from laser printers are mainly SOAs. (2) Sources and precursors of generated particles: In order to identify the possible particle sources, particle formation potentials of both the printer components (e.g. fuser roller and lubricant oil) and supplies (e.g. paper and toner powder) were investigated using furnace tests. The VOCs emitted during the experiments were sampled and identified to provide information about particle precursors. The results suggested that all of the tested materials had the potential to generate particles upon heating. Nine unsaturated VOCs were identified from the emissions produced by paper and toner, which may contribute to the formation of UFPs through oxidation reactions with ozone. (3) Factors influencing the particle emission: The factors influencing particle emissions were also investigated by comparing two popular laser printers, one showing particle emissions three orders of magnitude higher than the other. The effects of toner coverage, printing history, type of paper and toner, and working temperature of the fuser roller on particle number emissions were examined. The results showed that the temperature of the fuser roller was a key factor driving the emission of particles. Based on the results for 30 different types of laser printers, a systematic positive correlation was observed between temperature and particle number emissions for printers that used the same heating technology and had a similar structure and fuser material. It was also found that temperature fluctuations were associated with intense bursts of particles and therefore, they may have impact on the particle emissions. Furthermore, the results indicated that the type of paper and toner powder contributed to particle emissions, while no apparent relationship was observed between toner coverage and levels of submicron particles. (4) Mechanisms of SOA formation, growth and ageing: The overall hypothesis that UFPs are formed by reactions with the VOCs and O3 emitted from laser printers was examined. The results proved this hypothesis and suggested that O3 may also play a role in particle ageing. In addition, knowledge about the mixing state of generated particles was utilised to explore the detailed processes of particle formation for different printing scenarios, including warm-up, normal printing, and printing without toner. The results indicated that polymerisation may have occurred on the surface of the generated particles to produce thermoplastic polymers, which may account for the expandable characteristics of some particles. Furthermore, toner and other particle residues on the idling belt from previous print jobs were a very clear contributing factor in the formation of laser printer-emitted particles. In summary, this study not only improves scientific understanding of the nature of printer-generated particles, but also provides significant insight into the formation and ageing mechanisms of SOAs in the indoor environment. The outcomes will also be beneficial to governments, industry and individuals.

Motor vehicles are a major source of gaseous and particulate matter pollution in urban areas, particularly of ultrafine sized particles (diameters < 0.1 µm). Exposure to particulate matter has been found to be associated with serious health effects, including respiratory and cardiovascular disease, and mortality. Particle emissions generated by motor vehicles span a very broad size range (from around 0.003-10 µm) and are measured as different subsets of particle mass concentrations or particle number count. However, there exist scientific challenges in analysing and interpreting the large data sets on motor vehicle emission factors, and no understanding is available of the application of different particle metrics as a basis for air quality regulation. To date a comprehensive inventory covering the broad size range of particles emitted by motor vehicles, and which includes particle number, does not exist anywhere in the world. This thesis covers research related to four important and interrelated aspects pertaining to particulate matter generated by motor vehicle fleets. These include the derivation of suitable particle emission factors for use in transport modelling and health impact assessments; quantification of motor vehicle particle emission inventories; investigation of the particle characteristic modality within particle size distributions as a potential for developing air quality regulation; and review and synthesis of current knowledge on ultrafine particles as it relates to motor vehicles; and the application of these aspects to the quantification, control and management of motor vehicle particle emissions. In order to quantify emissions in terms of a comprehensive inventory, which covers the full size range of particles emitted by motor vehicle fleets, it was necessary to derive a suitable set of particle emission factors for different vehicle and road type combinations for particle number, particle volume, PM1, PM2.5 and PM1 (mass concentration of particles with aerodynamic diameters < 1 µm, < 2.5 µm and < 10 µm respectively). The very large data set of emission factors analysed in this study were sourced from measurement studies conducted in developed countries, and hence the derived set of emission factors are suitable for preparing inventories in other urban regions of the developed world. These emission factors are particularly useful for regions with a lack of measurement data to derive emission factors, or where experimental data are available but are of insufficient scope. The comprehensive particle emissions inventory presented in this thesis is the first published inventory of tailpipe particle emissions prepared for a motor vehicle fleet, and included the quantification of particle emissions covering the full size range of particles emitted by vehicles, based on measurement data. The inventory quantified particle emissions measured in terms of particle number and different particle mass size fractions. It was developed for the urban South-East Queensland fleet in Australia, and included testing the particle emission implications of future scenarios for different passenger and freight travel demand. The thesis also presents evidence of the usefulness of examining modality within particle size distributions as a basis for developing air quality regulations; and finds evidence to support the relevance of introducing a new PM1 mass ambient air quality standard for the majority of environments worldwide. The study found that a combination of PM1 and PM10 standards are likely to be a more discerning and suitable set of ambient air quality standards for controlling particles emitted from combustion and mechanically-generated sources, such as motor vehicles, than the current mass standards of PM2.5 and PM10. The study also reviewed and synthesized existing knowledge on ultrafine particles, with a specific focus on those originating from motor vehicles. It found that motor vehicles are significant contributors to both air pollution and ultrafine particles in urban areas, and that a standardized measurement procedure is not currently available for ultrafine particles. The review found discrepancies exist between outcomes of instrumentation used to measure ultrafine particles; that few data is available on ultrafine particle chemistry and composition, long term monitoring; characterization of their spatial and temporal distribution in urban areas; and that no inventories for particle number are available for motor vehicle fleets. This knowledge is critical for epidemiological studies and exposure-response assessment. Conclusions from this review included the recommendation that ultrafine particles in populated urban areas be considered a likely target for future air quality regulation based on particle number, due to their potential impacts on the environment. The research in this PhD thesis successfully integrated the elements needed to quantify and manage motor vehicle fleet emissions, and its novelty relates to the combining of expertise from two distinctly separate disciplines - from aerosol science and transport modelling. The new knowledge and concepts developed in this PhD research provide never before available data and methods which can be used to develop comprehensive, size-resolved inventories of motor vehicle particle emissions, and air quality regulations to control particle emissions to protect the health and well-being of current and future generations.

Motor vehicles are a major source of gaseous and particulate matter pollution in urban areas, particularly of ultrafine sized particles (diameters < 0.1 µm). Exposure to particulate matter has been found to be associated with serious health effects, including respiratory and cardiovascular disease, and mortality. Particle emissions generated by motor vehicles span a very broad size range (from around 0.003-10 µm) and are measured as different subsets of particle mass concentrations or particle number count. However, there exist scientific challenges in analysing and interpreting the large data sets on motor vehicle emission factors, and no understanding is available of the application of different particle metrics as a basis for air quality regulation. To date a comprehensive inventory covering the broad size range of particles emitted by motor vehicles, and which includes particle number, does not exist anywhere in the world. This thesis covers research related to four important and interrelated aspects pertaining to particulate matter generated by motor vehicle fleets. These include the derivation of suitable particle emission factors for use in transport modelling and health impact assessments; quantification of motor vehicle particle emission inventories; investigation of the particle characteristic modality within particle size distributions as a potential for developing air quality regulation; and review and synthesis of current knowledge on ultrafine particles as it relates to motor vehicles; and the application of these aspects to the quantification, control and management of motor vehicle particle emissions. In order to quantify emissions in terms of a comprehensive inventory, which covers the full size range of particles emitted by motor vehicle fleets, it was necessary to derive a suitable set of particle emission factors for different vehicle and road type combinations for particle number, particle volume, PM1, PM2.5 and PM1 (mass concentration of particles with aerodynamic diameters < 1 µm, < 2.5 µm and < 10 µm respectively). The very large data set of emission factors analysed in this study were sourced from measurement studies conducted in developed countries, and hence the derived set of emission factors are suitable for preparing inventories in other urban regions of the developed world. These emission factors are particularly useful for regions with a lack of measurement data to derive emission factors, or where experimental data are available but are of insufficient scope. The comprehensive particle emissions inventory presented in this thesis is the first published inventory of tailpipe particle emissions prepared for a motor vehicle fleet, and included the quantification of particle emissions covering the full size range of particles emitted by vehicles, based on measurement data. The inventory quantified particle emissions measured in terms of particle number and different particle mass size fractions. It was developed for the urban South-East Queensland fleet in Australia, and included testing the particle emission implications of future scenarios for different passenger and freight travel demand. The thesis also presents evidence of the usefulness of examining modality within particle size distributions as a basis for developing air quality regulations; and finds evidence to support the relevance of introducing a new PM1 mass ambient air quality standard for the majority of environments worldwide. The study found that a combination of PM1 and PM10 standards are likely to be a more discerning and suitable set of ambient air quality standards for controlling particles emitted from combustion and mechanically-generated sources, such as motor vehicles, than the current mass standards of PM2.5 and PM10. The study also reviewed and synthesized existing knowledge on ultrafine particles, with a specific focus on those originating from motor vehicles. It found that motor vehicles are significant contributors to both air pollution and ultrafine particles in urban areas, and that a standardized measurement procedure is not currently available for ultrafine particles. The review found discrepancies exist between outcomes of instrumentation used to measure ultrafine particles; that few data is available on ultrafine particle chemistry and composition, long term monitoring; characterization of their spatial and temporal distribution in urban areas; and that no inventories for particle number are available for motor vehicle fleets. This knowledge is critical for epidemiological studies and exposure-response assessment. Conclusions from this review included the recommendation that ultrafine particles in populated urban areas be considered a likely target for future air quality regulation based on particle number, due to their potential impacts on the environment. The research in this PhD thesis successfully integrated the elements needed to quantify and manage motor vehicle fleet emissions, and its novelty relates to the combining of expertise from two distinctly separate disciplines - from aerosol science and transport modelling. The new knowledge and concepts developed in this PhD research provide never before available data and methods which can be used to develop comprehensive, size-resolved inventories of motor vehicle particle emissions, and air quality regulations to control particle emissions to protect the health and well-being of current and future generations.

This thesis characterizes the mass and chemical composition of the fine particle air pollution over several cities in South Asia and quantifies how major sources impact the observed levels by using Chemical Mass Balance modeling with organic compounds as tracers. During February 1999, as part of the INDOEX program, a study was conducted to measure the size distribution and chemical composition of the fine particles in a remote island in Maldives off the coast of India. We found that the fine particle concentrations were comparable to those found in major cities in the United States, and were surprisingly high for a background site. 10-day backwind trajectories pointed the source region towards the Indian subcontinent; other INDOEX studies confirmed the presence of a thick haze layer over the Indian Ocean and the subcontinent during the time of the experiment. Motivated by these findings, a detailed analysis of ambient PM2.5 was carried out in Delhi, Mumbai, Kolkata, and Chandigarhfour cities located upwind of the island in Maldives. Seasonality of the fine particle concentrations was observed in each of these cities with the highest concentrations occurring during the wintertime and the lowest concentrations during the summer. Size distribution and chemical composition of the fine particle emissions from five Bangladeshi biomass (rice straw, coconut leaves, dried cow dung, synthetic biomass log, and jackfruit wood) and three Asian coals (Bangladeshi, Indian, and Chinese) were characterized and important source signatures were identified. Finally, recently developed chemical tracer techniques were applied to the ambient samples from North India to differentiate between the contributions from the many different source types. The emission profiles and source signatures from the source tests conducted previously along with the ones conducted using the Indian Subcontinent fuels were used as inputs to the model. These results serve several purposes. First, they provide a description of the mass and detailed inorganic and organic chemical characteristics of fine particulate matter conducted for the first time ever in this region. Second, the source apportionment study will help to define the relative importance of those sources that should be included within an air quality control program. Chemical tracer techniques are particularly attractive for application in regions that have not been studied previously because they are able to yield rapid insights into the causes of a local air pollution problem before the completion of an accurate emissions inventory. Third, the source tests results will prove useful in constructing and evaluating regional emission inventory and assessing source impacts on air quality. Fourth, this work has been carried out with collaborations from Georgia Tech and several other Indian research institutions where pollution control personnel in India was trained in the operation of air sampling equipments that were left for continued monitoring, thus contributing to technology transfer and knowledge transfer from the US.

The control of particle emissions from an oil refinery is often difficult, due to changing operational conditions and the limited range of available treatment options. Excessive particle emissions have often been attributed start up problems with Fluidized Catalytic Cracker Units (FCCU) and little information is available regarding the exact composition and nature of these excessive emissions. Due to the complex nature of a FCCU, it has in the past been difficult to identify and control emissions, without the use of expensive end of pipe technologies. An Australian Oil Refinery, concerned with their catalyst emissions, sponsored this study of FCCU particle emissions. Due to the industrial nature of the project, a holistic approach to the management of emissions was taken, instead of a detailed investigation of a single issue. By looking at the broader range of issues, practical and useful outcomes can be achieved for the refinery. Initially, detailed emissions samplings were conducted to investigate the degree of particle emissions under start up conditions. Stack emissions were collected during a standard start up, and analysed to determine the particle size distribution and metal concentration of the emitted material. Three distinct stages of emissions were discovered, initially a high concentration of larger particles, followed by a peak in the very fine particles and finally a reduction of particle emissions to a more steady or normal operational state. The variation in particle emissions was caused by operational conditions, hardware design and catalyst characteristics. Fluctuations in the gas velocity through the system altered the ability of the cyclones to collect catalyst material. Also, the low bed level allowed air bypass to occur more readily, contributing to the increased emissions levels seen during the initial stage of the start up. Reduced fluidity characteristics of the circulating catalyst also affected the diplegs operations, altering the collection efficiency of the cyclone. During the loading of catalyst into the system, abraded material was quickly lost due to its particle size, contributing to fine particle emissions levels. More importantly, thermal fracturing of catalyst particles occurred when the cold catalyst was fed into the hot regenerator. Catalyst particles split causing the generation of large amounts of fine particle material, which is easily lost from the system. This loading of catalyst directly linked to the period of high concentration of fine particles in the emissions stream. It was found that metals, and in particular iron, calcium and silicon form a thick layer on the outside of the catalyst, with large irregular shaped metal ridges, forming along the surface of the particle. These ridges reduce the fluidity of the catalyst, leading to potential disruptions in the regenerator. In addition to this, the metal rich ridges are preferentially removed via attrition, causing metal rich material to be emitted into the atmosphere. To overcome these high particle emissions rates from the FCCU the refinery should only use calcinated catalyst to reduce the influence of thermal process and particle fracture and generation. Although the calcinated catalyst can fracture when added to the system, it is far less than that obtained with uncalicinated catalyst. To further reduce the risk of particle fracture due to thermal stresses the refinery should consider reducing the temperature gradients between the hot and cold catalyst. Due to the economics involved with the regenerator, possible pre-warming of catalyst before addition into system is the preferred option. This pre-heating of catalyst should also incorporate a controlled attrition stage to help remove the build up of metals on the surface of the particles whilst allowing this material to be collected before it can be released into the atmosphere. The remove of the metal crust will also improve the fluidity of the system and reduce the chance of catalyst blockages occurring. Finally, modelling of the system has shown that control of key parameters such as particle size and gas velocity are essential to the management of air emissions. The refinery should look at adjusting start up procedures to remove fluctuations in these key parameters. Also the refinery should be careful in using correlation found in the literature to predicted operational conditions in the system as these correlations are misleading when used under industrial situations.

In this study, we developed and standardized a sanding method to evaluate the emission of airborne particles from products that contain carbon nanotubes (CNTs) under different conditions, including three types of sandpaper and three sanding disc speed. We also characterized the emission of the airborne particles from one neat epoxy test sample, four CNTs-incorporating test samples with different CNTs loading, and two commercial products. The total number concentration, respirable mass concentration, and particle size number/mass distribution of the emitted particles were calculated and compared, followed by an electron microscopy (EM) analysis. These data suggest that the sanding process can produce substantial quantities of airborne particles. Also, the emission of airborne particles was associated with different test conditions. EM analysis of the airborne particle samples showed embedded CNTs protruding from the outer surface, which was different from CNTs-incorporating bulk material. Our study suggests a potential generation of particles during the life cycle event of sanding. Further studies should be carried out to investigate the potential human health hazard in other life cycle events.

The behaviour of particulate matter emissions from a Ford XLD 4T, passengercar diesel engine through a practical exhaust system in place was investigated during transient conditions, namely cold start and fast acceleration. Particulate emissions were measured at four sampling points through the exhaust system and the changes in particulate total mass concentration, total number concentration, particle size distribution and Carbon/SOF fractions were determined for various engine operating conditions. Each cold start test consisted of a step-change cold-start with fast acceleration, reaching one of the following target operation conditions: Idle, 1500rpm - 15kW, 2250rpm - 15kW, 2250rpm-35kW and 3500rpm - 15kW. Two preconditioning procedures were designed to provide repeatable cold start tests. These consisted of a) Idle operation for 4 hours the day before the test, followed by overnight soak; and b)10 minutes at high engine speed operation. Fast acceleration tests consisted of idle preconditioning followed by a step change to the target operation conditions. The particulate matter changes through the exhaust system were shown to be dependent on the previous operational history of the engine, idle conditions being effective at forming particle deposits. The amount of particulate deposited or blown out from the exhaust system constituted a significant fraction of the total engine exhaust emissions in a significant number of cold start and acceleration tests. The changes in particle concentration did not occur throughout the system in the same fashion. The catalyst produced predominantly particle number and mass reduction and the second silencer was a more efficient particle collector than the first silencer. From the first silencer, particles were resuspended more easily and in many more cases. Regarding the chemical composition, high-load conditions produced lower Solvent Organic Fraction (SOF) than their low load counterpart. However, the SOF did not change significantly through the exhaust system. Part of this work consisted of examining the use of the Electrical Low Pressure Impactor (ELP1) to estimate particulate mass emissions. It was observed that the ELP1 tended to overestimate the number of particles in the large (>0.1 (im) size range. This greatly affected the conversion from total particle number concentration to particle mass concentration. A correction based on comparison between the electrical and gravimetric methods (ELPI vs. Andersen Impactors) in the common size range for both techniques was proposed. Transient and steady-state tailpipe emission factors, expressed as grams of particulate per unit of engine work in kWh, were calculated from the test results and used to estimate the effect of transients on total cycle emissions in cycles with a different design from those followed in this work. The ELPI proved to be useful, yet limited for particle collection on Transmission Electron Microscope (TEM) grids in several size ranges. TEM images of particles were analysed and their fractal dimension determined.

Various epidemiological studies have linked exposure to Ultrafine Particles (UFP; diameter< 100 nm) to adverse health impacts. Roadway traffic is one of the major sources of UFPs and heavily influences UFP concentrations in the nearby vicinity of major roadways. Modeling efforts to predict UFPs have been limited due to the scarcity of reliable information on emissions, lack of monitoring data and limited understanding of complex processes affecting UFP concentrations near sources. In this study continuous measurement of ultrafine particle number concentrations (PNC) and mass concentrations of nitric oxide (NO), nitrogen dioxide (NO2) and PM2.5 was conducted near an arterial road and freeway at different seasons and meteorological conditions and integrated with traffic count data. PNC showed high correlation with NO (r=0.64 for arterial; 0.61 for freeway), NO2 (r=0.57 for arterial; 0.53 for freeway) and NOx (NOx=NO+NO2; r=0.63 for arterial; 0.59 for freeway) and moderate to low correlation with traffic volume (r=0.33 for arterial; 0.32 for freeway) and PM2.5 (r=0.28 for arterial; 0.23 for freeway); respectively; for both sites at 15 minute averages. The PNC-NOx relationship prevailed on a shorter term (15 min), hourly, and throughout the day basis. Both PNC and NOx showed comparatively higher correlation with traffic during the morning period but became lower during evening which can be attributed to the higher boundary layer and wind speeds. The variable meteorology in the evening affects both PNC and NOx concentrations in the same way and the correlation between NOx and PNC is maintained high both during morning (r=0.74 for arterial; 0.69 for freeway), and evening (r=0.62 for arterial; 0.59 for freeway) periods. Thus nitrogen oxides can be used as a proxy for traffic-related UFP number concentration reflecting the effect of both traffic intensity and meteorological dilution. The PNC-NOx relation was explored for various meteorological parameters i.e. wind speed and temperature. It is found that NOx emission is temperature independent and can be used to reflect the effect of traffic intensity and meteorological dilution. Once the effect of traffic intensity and dilution is removed, the effect of temperature on PNC-NOx ratio becomes important which can be attributed to the variation in PNC emission factors with temperature. The high morning PNC-NOx ratio found at the arterial road is a result of new particle formation due to lower temperature and low concentration of exhaust gases in the morning air favoring nucleation over condensation. This finding has important implication when calculating emission factors for UFP number concentrations. Thus it can be concluded that roadside concentration of ultrafine particles not only depends on traffic intensity but also on meteorological parameters affecting dilution or new particle formation. High concentrations of ultrafine particle number concentration close to a roadway is expected due to higher traffic intensity , as well as during low wind speed causing low dilution and low temperature conditions favoring new particle formation. Finally a simplified approach of calculating particle number emission factor was developed using existing and easily available emission inventory for traffic related tracer gases. Using NOx emission factors from MOVES emission model, the emission ratio of PNC to NOx was converted to develop particle number emission factors. NOx was selected as the traffic related tracer gas since the number concentration of particles is closely correlated to NOx, NOx and particles are diluted in the same way and NOx emission factors are available for a variety of traffic situations. To ensure contribution of fresh traffic exhaust, the average of the difference of pollutant concentrations at high traffic condition and background condition was used to calculate PNC-NOX ratio. Using nitrogen oxides to define background and high-traffic conditions and MOVES emission factor for NOX to convert corresponding PNC-NOX ratio, an average emission factor of (1.82 ± 0.17) E+ 14 particle/ vehicle-km was obtained, suitable for summertime. When compared to existing particle number emission factors derived from dynamometer tests, it was found that there exits reasonable agreement between the calculated real world particle number emission factors and emission factors from dynamometer tests. The calculated emission factor and R-Line dispersion model was tested in predicting near-road particle number concentrations. Although only 23% of the variability in PNC was explained by the dispersion model, 84.33% of the measurements fell within the factor of two envelope. This suggests that there is potential to effectively use these models and thus warrants more in-depth analysis. Finally, a simple map of PNC gradients from major roads of Portland was developed. The results of this study helped identify proxy-indicators to provide reference values for estimating UFP concentrations and emissions that can be used for simple evaluation of particle concentration near major roadways for environmental and urban planning purposes and to assess expected impact of UFP pollution on population living near roadways exposed to elevated concentrations.

This thesis presents a comprehensive study on the influences of biodiesel chemical composition and physical properties on diesel engine exhaust particle emissions. It examines biodiesels from several feedstocks having wide variations in their chemical composition (carbon chain length, unsaturation and oxygen content) and physical properties (density, viscosity, surface tension, boiling point etc.), and evaluates their influence on exhaust particle emissions. The outcome of this thesis is significant since it reveals the importance of regulating biodiesels chemical composition in order to ensure lowest possible emissions with better overall performance.

Numerous studies have shown that respirable particles contribute to adverse human health outcomes including discomfort in irritated airways, increased asthma attacks, irregular heartbeat, non-fatal heart attacks, and even death. Particle emissions from diesel vehicles are a major source of airborne particles in urban areas. In response to energy security and global climate regulations, the use of biodiesel as an alternative fuel for petrodiesel has significantly increased in recent years. Particle emissions from diesel engines are highly dependent on fuel composition and, as such, the increased use of biodiesel in diesel vehicles may potentially change the concentration, size, and composition of particles in respirable air. One indicator used to evaluate the potential health risk of these particles to humans is particle diameter (Dp). Ultrafine particles (UFPs, Dp Current research in automotive emissions primarily focuses on particle emissions measured on a total particle mass (PM) basis from heavy-duty diesel vehicles. The nation's light-duty diesel fleet is, however, increasing; and because the mass of a UFP is much less than that of larger particles, the total PM metric is not sufficient for characterization of UFP emissions. As such, this research focuses on light-duty diesel engine transient UFP emissions, measured by particle number (PN), from petrodiesel, biodiesel, and blends thereof. The research objectives were to determine: 1) the difference in UFP emissions between petrodiesel and blends of waste vegetable oil-based biodiesel (WVO), 2) the differences between UFP emissions from blends of WVO and soybean oil-based biodiesel (SOY), and 3) the feasibility of using genetic programming (GP) to select the primary engine operating parameters needed to predict UFP emissions from different blends of biodiesel. The results of this research are significant in that: 1) Total UFP number emission rates (ERs) exhibited a non-monotonic increasing trend relative to biodiesel content of the fuel for both WVO and SOY that is contrary to the majority of prior studies and suggests that certain intermediate biodiesel bends may produce lower UFP emissions than lower and higher blends, 2) The data collected corroborate reports in the literature that fuel consumption of diesel engines equipped with pump-line-nozzle fuel injection systems can increase with biodiesel content of the fuel without operational changes, 3) WVO biodiesel blends reduced the overall mean diameter of the particle distribution relative to petrodiesel more so than SOY biodiesel blends, and 4) Feature selection using genetic programming (GP) suggests that the primary model inputs needed to predict total UFP emissions are exhaust manifold temperature, intake manifold air temperature, mass air flow, and the percentage of biodiesel in the fuel; These are different than inputs typically used for emissions modeling such as engine speed, throttle position, and torque suggesting that UFP emissions modeling could be improved by using other commonly measured engine operating parameters.

Non-thermal plasma (NTP) is a promising candidate for controlling engine exhaust emissions. Plasma is known as the fourth state of matter, where both electrons and positive ions co-exist. Both gaseous and particle emissions of diesel exhaust undergo chemical changes when they are exposed to plasma. In this project diesel particulate matter (DPM) mitigation from the actual diesel exhaust by using NTP technology has been studied. The effect of plasma, not only on PM mass but also on PM size distribution, physico-chemical structure of PM and PM removal mechanisms, has been investigated. It was found that NTP technology can significantly reduce both PM mass and number. However, under some circumstances particles can be formed by nucleation. Energy required to create the plasma with the current technology is higher than the benchmark set by the commonly used by the automotive industry. Further research will enable the mechanism of particle creation and energy consumption to be optimised.

The measurement of submicrometre (< 1.0 m) and ultrafine particles (diameter < 0.1 m) number concentration have attracted attention since the last decade because the potential health impacts associated with exposure to these particles can be more significant than those due to exposure to larger particles. At present, ultrafine particles are not regularly monitored and they are yet to be incorporated into air quality monitoring programs. As a result, very few studies have analysed their long-term and spatial variations in ultrafine particle concentration, and none have been in Australia. To address this gap in scientific knowledge, the aim of this research was to investigate the long-term trends and seasonal variations in particle number concentrations in Brisbane, Australia. Data collected over a five-year period were analysed using weighted regression models. Monthly mean concentrations in the morning (6:00-10:00) and the afternoon (16:00-19:00) were plotted against time in months, using the monthly variance as the weights. During the five-year period, submicrometre and ultrafine particle concentrations increased in the morning by 105.7% and 81.5% respectively whereas in the afternoon there was no significant trend. The morning concentrations were associated with fresh traffic emissions and the afternoon concentrations with the background. The statistical tests applied to the seasonal models, on the other hand, indicated that there was no seasonal component. The spatial variation in size distribution in a large urban area was investigated using particle number size distribution data collected at nine different locations during different campaigns. The size distributions were represented by the modal structures and cumulative size distributions. Particle number peaked at around 30 nm, except at an isolated site dominated by diesel trucks, where the particle number peaked at around 60 nm. It was found that ultrafine particles contributed to 82%-90% of the total particle number. At the sites dominated by petrol vehicles, nanoparticles (< 50 nm) contributed 60%-70% of the total particle number, and at the site dominated by diesel trucks they contributed 50%. Although the sampling campaigns took place during different seasons and were of varying duration these variations did not have an effect on the particle size distributions. The results suggested that the distributions were rather affected by differences in traffic composition and distance to the road. To investigate the occurrence of nucleation events, that is, secondary particle formation from gaseous precursors, particle size distribution data collected over a 13 month period during 5 different campaigns were analysed. The study area was a complex urban environment influenced by anthropogenic and natural sources. The study introduced a new application of time series differencing for the identification of nucleation events. To evaluate the conditions favourable to nucleation, the meteorological conditions and gaseous concentrations prior to and during nucleation events were recorded. Gaseous concentrations did not exhibit a clear pattern of change in concentration. It was also found that nucleation was associated with sea breeze and long-range transport. The implications of this finding are that whilst vehicles are the most important source of ultrafine particles, sea breeze and aged gaseous emissions play a more important role in secondary particle formation in the study area.

The measurement of submicrometre (< 1.0 m) and ultrafine particles (diameter < 0.1 m) number concentration have attracted attention since the last decade because the potential health impacts associated with exposure to these particles can be more significant than those due to exposure to larger particles. At present, ultrafine particles are not regularly monitored and they are yet to be incorporated into air quality monitoring programs. As a result, very few studies have analysed their long-term and spatial variations in ultrafine particle concentration, and none have been in Australia. To address this gap in scientific knowledge, the aim of this research was to investigate the long-term trends and seasonal variations in particle number concentrations in Brisbane, Australia. Data collected over a five-year period were analysed using weighted regression models. Monthly mean concentrations in the morning (6:00-10:00) and the afternoon (16:00-19:00) were plotted against time in months, using the monthly variance as the weights. During the five-year period, submicrometre and ultrafine particle concentrations increased in the morning by 105.7% and 81.5% respectively whereas in the afternoon there was no significant trend. The morning concentrations were associated with fresh traffic emissions and the afternoon concentrations with the background. The statistical tests applied to the seasonal models, on the other hand, indicated that there was no seasonal component. The spatial variation in size distribution in a large urban area was investigated using particle number size distribution data collected at nine different locations during different campaigns. The size distributions were represented by the modal structures and cumulative size distributions. Particle number peaked at around 30 nm, except at an isolated site dominated by diesel trucks, where the particle number peaked at around 60 nm. It was found that ultrafine particles contributed to 82%-90% of the total particle number. At the sites dominated by petrol vehicles, nanoparticles (< 50 nm) contributed 60%-70% of the total particle number, and at the site dominated by diesel trucks they contributed 50%. Although the sampling campaigns took place during different seasons and were of varying duration these variations did not have an effect on the particle size distributions. The results suggested that the distributions were rather affected by differences in traffic composition and distance to the road. To investigate the occurrence of nucleation events, that is, secondary particle formation from gaseous precursors, particle size distribution data collected over a 13 month period during 5 different campaigns were analysed. The study area was a complex urban environment influenced by anthropogenic and natural sources. The study introduced a new application of time series differencing for the identification of nucleation events. To evaluate the conditions favourable to nucleation, the meteorological conditions and gaseous concentrations prior to and during nucleation events were recorded. Gaseous concentrations did not exhibit a clear pattern of change in concentration. It was also found that nucleation was associated with sea breeze and long-range transport. The implications of this finding are that whilst vehicles are the most important source of ultrafine particles, sea breeze and aged gaseous emissions play a more important role in secondary particle formation in the study area.

This study investigated methods to characterise nanoparticle emission and transport associated with the operation of laser printers and selected nanotechnology processes in workplace settings. Results showed particle number and mass concentration emission varied by orders of magnitude amongst the different processes, from submicrometre to supermicrometre size. Therefore, a multi-metric particle assessment method must be utilised. Analysis of both real-time particle measurement instrumentation and off-line particle analysis, temporal and spatial particle number and mass concentration, surface area, size, morphology and chemical composition of airborne particles was utilised to develop and validate a three-tiered assessment method designed to assess and control worker exposure.

There is a consensus worldwide that the share of renewable energy sources should be increased to mitigate climate change. The strive to increase the renewable energy fraction can partly be met by an increased utilization of different biomass feedstocks. Many of the "new" feedstocks puts stress on certain challenges such as air pollution emissions and operation stability of the combustion process. The overall objective was to investigate, evaluate, and explain the effects of fuel design and combustion control - fuel engineering - as primary measures for control of slag formation, deposit formation, and fine particle emissions during biomass combustion in small and medium scale fixed-bed appliances. The work in this thesis can be outlined as having two main focus areas, one more applied regarding fuel engineering measures and one more fundamental regarding the time-resolved release of ash forming elements, with particular focus on potassium. The overall conclusion related to the abatement of particle emissions and slag formation, is that the release of fine particle and deposit forming matter can be controlled simultaneously as the slag formation during fixed-bed biomass combustion. The methodology is in this perspective denoted “fuel engineering” and is based on a combined approach including both fuel design and process control measures. The studies on time-resolved potassium release showed that a Macro-TG reactor with single pellet experiments was a valuable tool for studying ash transformation along the fuel conversion. The combination of dedicated release determinations based on accurate mass balance considerations and ICP analysis, with phase composition characterization by XRD, is important for the understanding of potassium release in general and time-resolved data in particular. For wood, the results presented in this work supports the potassium release mechanism from "char-K" but questions the previously suggested release mechanism from decomposition of K-carbonates. For straw, the present data support the idea that the major part of the potassium release is attributed to volatilization of KCl. To further explore the detailed mechanisms, the novel approach developed and applied in this work should be complemented with other experimental and analytical techniques. The research in this thesis has explored some of the challenges related to the combined phenomena of fuel conversion and ash transformation during thermochemical conversion of biomass, and has contributed with novel methods and approaches that have gained new knowledge to be used for the development of more effective bioenergy systems.

Whilst the compression ignition (CI) engine exhibits many design advantages relative to its spark ignition engine counterpart; such as: high thermal efficiency, fuel economy and low carbon monoxide and hydrocarbon emissions, the issue of Diesel Particulate Matter (DPM) emissions continues to be an unresolved problem for the CI engine. Primarily, this thesis investigates a range of DPM mitigation strategies such as alternative fuels, injection technologies and combustion strategies conducted with a view to determine their impact on the physico-chemical properties of DPM emissions, and consequently to shed light on their likely human health impacts. Regulated gaseous emissions, Nitric oxide (NO), Carbon monoxide (CO), and Hydrocarbons (HCs), were measured in all experimental campaigns, although the major focus in this research program was on particulate emissions...

Due to their adverse health effects emissions have been regulated for over three decades. Brake wear particulate matter is the most important non-exhaust source, however current knowledge is mainly limited to observational studies. This thesis aims to investigate relations between the brake system contact conditions and the related emissions on a model scale; validate the results on a component level; and understand to what extent they are significant on a full-scale. Paper A investigates the influence of nominal contact pressure on a model scale. Results show that higher pressure corresponds to higher emissions Paper B investigates the influence of the nominal contact pressure, for different friction materials, on a model scale. A temperature threshold, responsible for a relevant emission increase, is identified. Paper C investigates particle characteristics and wear mechanisms for different nominal contact pressures, on a model scale. Results show an enhanced tribo-layer at higher pressure levels. Paper D investigates the influence of brake system conditions on emissions, on a model scale. Results show that frictional power is the most important parameter. A transition temperature independent of the contact condition is identified. Paper E investigates similarities occurring on a component scale and a model scale in terms of emissions. Results show a promising correlation, and the possibility of using a pin-on-disc tribometer for R&D activities. Paper F investigates analogies occurring on a component scale and a model scale, in terms of friction performance, fictional surface and chemical composition. Results show similar phenomena occurring for the two test stands. Paper G analyses real brake system working conditions in a urban environment defining, by means of an inertia dyno bench, the related emissions. Results reveal emission factors compliant to EURO6 and EURO2 regulations, in terms of number and mass, respectively.
På grund av deras negativa hälsoeffekter har partikel emissioner reglerats i över tre årtionden. Bromsslitagepartiklar är den viktigaste icke-avgaskällan, men nuvarande kunskaper är huvudsakligen begränsade till observationsstudier. Avhandlingen syftar till att undersöka förhållandena mellan bromssystemets kontaktförhållanden och de relaterade utsläppen på modellskala. Validera resultaten på komponentnivå och förstå i vilken utsträckning de är betydande i full skala. Papper A undersöker påverkan av nominellt kontakttryck i en modellskala. Resultat visar att högre tryck motsvarar högre utsläpp. Papper B undersöker påverkan av det nominella kontakttrycket, för olika friktionsmaterial, i modellskala. En temperaturtröskel,  för en emissionsökning identifieras. Papper C undersöker partikelegenskaper och slitagemekanismer för olika nominella kontakttryck, i en modellskala. Resultat visar ett förbättrat triboskikt vid högre trycknivåer. Papper D undersöker påverkan av bromssystemets förhållanden på utsläpp i en modellskala. Resultat visar att friktionskraften är den viktigaste parametern. En övergångstemperatur oberoende av kontaktförhållandet identifieras. Papper E undersöker likheter som uppträder på komponentskala och  modellskala när det gäller emissioner. Resultatet visar en lovande korrelation, och möjligheten att använda en pinne-på-skiva-tribometer för FoU-aktiviteter. Papper F undersöker analogier som förekommer på en komponentskala och en modellskala, vad gäller friktionsprestanda, friktionsyta och kemisk sammansättning. Resultat visar liknande fenomen som förekommer för de två testskalorna. Papper G analyserar verkliga bromssystem arbetsförhållanden i en stadsmiljö som definierar, med hjälp av en tröghetsdyno bänk, de relaterade utsläppen. Resultatet visar utsläppsfaktorer som är förenliga med EURO6 och EURO2-reglerna, i fråga om antal respektive massa.

QC 20170808

REBRAKE Project

It is estimated that around three billion people globally rely on traditional usage of biomass to cover their daily energy needs, which causes health and social inequality problems and contributes to global warming. Thus, the study of particle emissions from cookstoves provides important information that can help improve global welfare.   This study aims to (a) evaluate a new laboratory setup for measurement of particle emissions from cookstoves and (b) use this setup to compare the particle emissions from three cookstove appliances that cover the whole spectra of used technologies, namely a 3-stone fire, an improved cookstove and a gasifier stove. Emissions of total suspended particles (TSP), fine particles (≤ 2500 nm) and other emission components such as carbon dioxide were measured. Results from this study show that the new laboratory setup is appropriate to measure and investigate fine particle emissions from cookstoves as well as cookstove efficiency. Further, it also shows that the 3-stone fire was the cookstove with the highest emission factor of all, followed by the rocket stove and the gasifier stove respectively. The analysis of the data obtained from the transient particle measurement provided some information on the particle size and the soot and salt contained in the overall emitted particles. Finally, some suggestions such as continuous measurements of background particle and CO2 levels are recommended. Additionally, further research ideas are also proposed.

Despite the increasing popularity of hybrid-electric vehicles (HEVs), few studies have quantified their real-world particle emissions from internal combustion engine (ICE) re-ignition events (RIEVs). RIEVs have been known to occur under unstable combustion conditions which frequently result in particle number emission rates (PNERs) that exceed stabilized engine operation. Tailpipe total PN (5 to 560 nm diameter) emission rates (#/s) from a conventional vehicle (CV) and hybrid electric vehicle (HEV) 2010 Toyota Camry were quantified on a 50 km (32 mi) route over a variety of roadways in Chittenden County, Vermont using the Total On-board Tailpipe Emissions Measurement System (TOTEMS). While HEVs are known to have significant fuel conserving benefits compared to conventional vehicles, less is known about the relative emissions performance of HEVs. This study is the first to characterize RIEVs under a range of real-world driving conditions and to directly compare HEV and CV PNER during driving on different road sections. A total of 28 CV and 33 HEV sampling runs were conducted over an 18-month period under ambient temperatures ranging between -4 and 35 °C. A road classification based upon speed and intersection density divided the route into four different road sections: Freeway, Rural, Urban I and Urban II. Due to the distinct on-off cycling of the HEV ICE, a new operational mode framework (ICE OpMode) was developed to characterize shutdown, off, re-ignition and stabilized HEV ICE operation. Road section was found to affect overall ICE OpMode distribution, with HEV engine-off operation averaging 57%, 36% and 5% of total operation for combined Urban, Rural and Freeway road sections, respectively. Re-ignition frequency was found to range between 11 and 133 events per hour, with spatial density ranging between 0.1 and 5.6 events per kilometer of roadway. A total of 3212 re-ignition events were observed and recorded, and mean HEV PNER during RIEVs, on average, ranged between 2.4 and 4.4 times greater than that of HEV Stabilized operation. Approximately 65% of all re-ignition events resulted in a peak PNER exceeding the 95% percentile for all ICE-on activity in both vehicles (9.3 x 1011 #/s), known as a High Emission Event Record (HEER). RIEV operation made up only 7.4% of total ICE-on operation for both vehicles but accounted for 35.4% of all HEERs. Overall, total particles emitted during HEV operation associated with re-ignition events ranged from 5% for Freeway driving to 60% for Urban I driving. Comparisons between vehicles found an average of 37% and 7% fuel conserving benefits of the HEV during Urban I and Freeway driving, respectively. However, a different effect was found for PN emissions. During Urban I driving, where RIEVs were most frequent, on average HEV PNER was 2.3 times greater than overall mean CV PNER. For Freeway driving, where the HEV operated similar to a conventional vehicle, mean CV PNER was 2.4 times greater than mean HEV PNER. PNER from partial re-ignition events following an incomplete ICE shutdown (no period of prior engine off operation) were on average 1.65 times greater than those occurring when the ICE shutdown for at least one second. The typical fuel consumption benefits of HEVs in urban driving are associated with a tradeoff in PN emissions. The HEV ICE operating behavior has implications for the spatial distribution of PN hot-spots as well as the associated micro-scale modeling of alternative vehicle technology emissions. It is likely that building a model of HEV behavior based upon CV activity will be appropriate, with consideration of a hybridization factor and, as a result of these analyses, a re-ignition factor.

Doctor of Philosophy
Department of Biological & Agricultural Engineering
Ronaldo G. Maghirang
Emissions of particulate matter (PM) are an increasing concern for large open beef cattle feedlots. Research is needed to develop science-based information on PM emissions and abatement measures for mitigating those emissions. This research was conducted to (1) measure PM concentrations emitted from large cattle feedlots, (2) compare different samplers for measuring concentrations of PM with equivalent aerodynamic diameter of 10 µm or less (PM10), (3) evaluate the relative effectiveness of pen surface treatments in reducing PM10 emissions, and (4) predict PM control efficiency of vegetative barriers. Concentrations of PM with equivalent aerodynamic diameter of 2.5 µm or less (PM2.5), PM10, and total suspended particulates (TSP) upwind and downwind of two large cattle feedlots (KS1, KS2) in Kansas were measured with gravimetric samplers. The downwind and net concentrations generally decreased with increasing water content (WC) of the pen surface; for effective control of PM emissions from feedlots, it appears that pen surface WC should be at least 20% (wet basis). Three types of samplers for measuring PM10 concentrations in feedlots KS1 and KS2 were compared: Tapered Element Oscillating Microbalance™ (TEOM), high-volume (HV), and low-volume (LV) PM10 samplers. Measured PM10 concentration was generally largest with the TEOM PM10 sampler and smallest with the LV PM10 sampler. A laboratory apparatus was developed for measuring the PM10 emission potential of pen surfaces as affected by surface treatments. The apparatus was equipped with a simulated pen surface, mock cattle hooves that moved horizontally across the pen surface, and PM10 samplers that collected emitted PM10. Of the surface treatments evaluated, application of water (6.4 mm) and hay (723 g/m2) exhibited the greatest percentage reduction in PM10 emission potential (69% and 77%, respectively) compared with the untreated manure layer. Computational fluid dynamics (CFD) was applied to predict airflow and particle collection by a row of trees (2.2 m high × 1.6 m wide). Predicted particle collection efficiencies generally agreed with published data and ranged from less than 1% for 0.875-µm particles to approximately 32% for 15-µm particles.

Intresset för biobränsleproducerad energi har ökat i takt med att kunderna blivit mer miljömedvetna. På grund av detta har efterfrågan på briketter ökat samtidigt som träindustrin har haft det svårt i en sviktande konjunktur. Därför har ett examensarbete utförts i samarbete med E.ON Värme Sverige AB där undersökningar på bränslebyte i pannor avsedda för torra bränslen till fuktigare, stamvedflis har utfört.

För denna undersökning har begränsningar införts på övre och undre effekt i form av uppehållstid och slutförbränningstemperatur. Intervallen är enbart beräknade på stamvedflis med 30 och 40 % fukthalt.

Undersökning visar att det går bra att elda stamvedsflis i briketteldade pannor utan att emissionerna ökar så pass mycket att villkoren för anläggningarna överskrids om lasten hålls inom vissa intervall. Det möjliga effektintervallet ökar med minskad fukthalt på bränslet.

Undersökningen har visat att det är bränslets kvalitet som är den mest begränsande faktorn.

The interest in bioenergy has increased with increased environmental awareness. The increasing demand on biofuels and the decreasing availability of the rawmaterials for making refined biofuels such as wood briquettes and wood pellets have caused the prices of these biofuels to increase. This report is performed in collaboration with E.ON Värme Sverige AB and its purpose is to investigate the possibilities for a change of fuels in existing boilers designed for refined biofuels, from wood briquettes to wood chips.

To be able to calculate a power interval where it would be possible to use wood chips with moisture contents of 30 and 40% by weight respectively, we had to make some assumptions regarding maximum flue gas flow, minimum retention time and the lowest temperature regarding complete combustion of CO.

Our calculations show that it is possible to use woodchips with a moisture content of 30 % w/w without any significant problems in all our boilers. When the moisture content is increased to 40 % w/w the interval for possible power output becomes more narrow. The amount of dust that is being emitted from the boilers does not exceed the limits regulated by environmental law, unless the thermal load of the boiler is too high.

The single most important factor for a successful change of fuel from wood briquettes to woodchips is that the fuel quality is good.

Particulate matter (PM) is regarded as one of the more important components of air pollution causing adverse health effects. A large group of compounds associated with PM are polycyclic aromatic compounds (PACs) which comprises polycyclic aromatic hydrocarbons (PAHs). Several PACs are known for their mutagenic and carcinogenic properties as well as have the ability to induce oxidative stress. With the growing importance of non-exhaust particles relative to vehicular tail-pipe emissions in urban air, it is necessary to investigate the possible contribution of PAHs from the different non-exhaust sources, as these inputs are far less characterized than tail-pipe emissions and their impact on human health is largely unknown. In this thesis automobile tires, an important non-exhaust traffic related source to particles, have been investigated for its content of highly carcinogenic dibenzopyrene isomers. In a separate study benzothiazoles, a class of compounds used as vulcanization accelerators in tire manufacture, were determined to evaluate their use as potential markers for tire wear particles in ambient air. Analysis of the tires showed a substantial variation in the PAH content between different makes of tires, likewise did the benzothiazoles content vary. By determining benzothiazole in air particles collected at a busy street in Stockholm the tire rubber contribution to airborne particles was estimated to 0.7 and 5.5 % for PM10 and all airborne particles, respectively. Together with the determined content of dibenzopyrenes and the relatively low mass contribution of tire wear to airborne particles in the urban air, estimated in this thesis as well as suggested by the literature, tire wear appears to be a minor traffic related contributor of these PAH compounds in the urban air. Nevertheless, tire wear may be an important source to 2-mercaptobenzothiazole in the urban air. Biodiesel, a biofuel produced from plant and animal fats, has been suggested as a suitable replacement for conventional petroleum based diesel fuels. While the majority of studies have focused on health outcomes from petroleum diesel exhaust exposure, human health effects related to biodiesel exhaust exposure is much less investigated. Biodiesel exhaust particles have been compared with conventional petroleum diesel by determining >40 PAHs in two separate studies on two different diesel engines, running on neat rapeseed methyl ester (RME), petroleum diesel and a fuel blend of 3:7 RME : petroleum diesel. One of the biodiesel studies also included determination of four oxygenated PAHs (Oxy-PAHs). The exhaust from biodiesel combustion differed from petroleum diesel combustion with regards to particle size, number of emitted particles, relative amount of volatile material adsorbed on the particles and emission of particle-associated PAHs and Oxy-PAHs. A portion of these volatile compounds originated from unburned or partially combusted biodiesel fuel, which interfered with the analysis. A sample cleanup method was therefore developed for determination of PAH in lipid rich matrices. Biodiesel combustion produced lower emission of PAHs and Oxy-PAH with the exception of a few PAHs with higher molecular weights. In comparison with petroleum diesel, the biodiesel particles had a higher relative composition of PAHs with more than four rings.

At the time of the doctoral defense, the following paper was unpublished and had a status as follows: Paper 5: Manuscript.

Crankcase ventilation contributes significantly to diesel engine particulate emissions. Future regulations will not only limit the mass of particulate matter, but also the number of particles. Controlling the source of crankcase emissions is critical to meeting the perennial legislation. Deficiency in the understanding of crankcase emissions generation and the contribution of lubricating oil has been addressed in detail by the experimental study presented in this thesis. A plethora of high speed laser optical diagnostics techniques have been employed to deduce the main mechanisms of crankcase oil aerosol generation. Novel images have captured oil atomisation and passive oil distribution around the crankcase of an optically accessed, motored, four cylinder, off highway, heavy duty, diesel engine. Rayleigh type ligament breakup of oil films present on the surface of dynamic components, most notably the crankshaft, camshaft and valve rockers generated oil drops below 10 micrometers. Data illustrated not only crankcase oil aerosol generation at source, but it has provided valuable information on methods to control oil aerosol generation and improve oil circuit efficiency. The feasibility of utilising computational fluid dynamics to predict crankcase oil aerosol generation has been successfully assessed using the experimental data. Particle sampling has characterised the crankcase emissions from both a fired and motored diesel engine crankcase. The evolution of submicron crankcase particles down to 5 nm has been recorded from both engines, including the isolated contribution of engine oil, at a wide range of engine test points. Results have provided constructive insight into the generation and control of this complex emission. The main mechanism of crankcase oil aerosol generation was found to be crankshaft oil atomisation. This atomisation process has been analysed in detail, involving high speed imaging of primary and satellite drop generation and high speed digital particle image velocity of the crankshaft air flow. A promising mechanism of regulating and controlling crankcase oil aerosol emissions at source has been studied experimentally.

Die Strahlentherapie ist einer der drei Partner im interdisziplinären Feld der Onkologie. In Europa, Asien und den USA besteht zunehmend die Möglichkeit einer Therapie mit Strahlen aus geladenen Ionen anstelle von Photonen. Eine Anlage in Dresden befindet sich in der Kommissionierungsphase. Die Ionenstrahltherapie bietet den Vorteil einer sehr konformalen Behandlung des Tumorvolumens durch die endliche Reichweite der Strahlen und ein ausgeprägtes Dosismaximum kurz vor dem Ende des Strahlpfades. Da eine Therapie in der Regel über bis zu 30 Sitzungen an verschiedenen Tagen durchgeführt wird und der Strahlweg stark von dem durchdrungenen Gewebe beeinflusst wird, sind Verfahren für eine in vivo Verifikation der Strahlapplikation wünschenswert. Eine dieser Methoden ist die Partikeltherapie–Positronen-Emissions-Tomografie (PT-PET). Sie beruht auf der Messung der vom Therapiestrahl erzeugten β+-Aktivitätsverteilung. Da eine direkte Berechnung der Dosis aus der Aktivität in lebendem Gewebe nicht möglich ist, wird die gemessene Aktivitätsverteilung mit einer berechneten Vorhersage verglichen und anschließend entschieden, ob die nächste Therapiesitzung wie geplant erfolgen kann oder Anpassungen notwendig sind. Die vorliegende Arbeit beschäftigt sich mit drei Themen aus dem Bereich der Datenverarbeitung für die PT-PET. Im ersten Teil wird ein Algorithmus zur Bestimmung von Reichweitendifferenzen aus zwei β+- Aktivitätsverteilungen adaptiert und evaluiert. Dies geschieht zunächst anhand einer Simulationsstudie mit realen Patientendaten. Ein Ansatz für eine automatisierte Analyse der Daten lieferte keine zufriedenstellenden Ergebnisse. Daher wird ein Software-Prototyp für eine semiautomatische, assistierte Datenanalyse entwickelt. Die Evaluierung erfolgt durch Experimente mit Phantomen am 12C-Strahl. Die erzeugte Aktivitätsverteilung wird von physiologischen Prozessen im Organismus beeinflusst. Dies führt zu einer Entfernung von Emittern vom Ort ihrer Erzeugung und damit zu einer Verringerung der diagnostischen Wertigkeit der erfassten Verteilung. Zur Quantifizierung dieses als Washout bezeichneten Effektes existiert ein am Tierexperiment gewonnenes Modell. Dieses Modell wird im zweiten Teil der Arbeit auf reale Patientendaten angewendet. Es konnte gezeigt werden, dass das Modell grundsätzlich anwendbar ist und für die betrachtete Tumorlokalisation Schädelbasis ein Washout mit einer Halbwertszeit von (155,7±4,6) s existiert. Die Berechnung der Vorhersage der β+-Aktivitätsverteilung kann durch übliche Monte-Carlo-Verfahren erfolgen. Dabei werden die Wechselwirkungsquerschnitte zahlreicher Reaktionskanäle benötigt. Als alternatives Verfahren wurde die Verwendung gemessener Ausbeuten (Yields) radioaktiver Nuklide in verschiedenen Referenzmaterialien vorgeschlagen. Auf Basis einer vorhandenen Datenbank dieser Yields und einer existierenden Condensed-History-Monte-Carlo-Simulation wird ein Programm zur Berechnung von Aktivitätsverteilungen auf Yieldbasis entwickelt. Mit der Methode kann die β+-Aktivitätsverteilung in Phantomen und Patienten zufriedenstellend vorhergesagt werden. Die entwickelten Verfahren sollen einen Einsatz der PT-PET im klinischen Umfeld erleichtern und damit einen breiten Einsatz ermöglichen, um das volle Potential der Ionenstrahltherapie nutzbar zu machen.

Even at low concentrations, the criteria air pollutant particulate matter (PM) is an environmental and public health hazard. Emissions levels legislated for modern diesel vehicles are so low (~90% lower than 2003) that it has become difficult to accurately measure PM by the regulatory metric: the mass of particles collected on a filter (i.e., the gravimetric method). Additionally, gravimetric analysis cannot measure real-time emission rates, and therefore is unable to characterize high-emitting transient events (e.g., engine starts, stop-and-go driving). By an alternate method, PM can be estimated by measuring the number-weighted particle size distribution (PSD) and calculating mass with a combination of theoretical and empirical constants (e.g., particle effective density). This integrated particle size distribution (IPSD) method is capable of high measurement sensitivity and real-time resolution. Real-time measurements by the IPSD method require fast-sizing spectrometers, such as the TSI Engine Exhaust Particle Sizer (EEPS), which sizes (between 5.6-560 nm) and counts particles based on their electrical mobility. The EEPS utilizes a unipolar charger to quickly charge particles for sizing and counting, however this mechanism has been shown to produce a less predictable charge distribution than bipolar chargers used in Scanning Mobility Particle Sizer (SMPS) systems – the gold standard 'slow-sizing' spectrometer. Several evaluations have shown deficiencies in EEPS PSD measurements due to charging differences (associated with particle morphology) unaccounted for in the transfer function matrix used to calibrate the EEPS. Specifically, the unipolar charger multiply charges a higher percentage of soot agglomerates (fractal-like particles common in diesel engine exhaust) than bipolar chargers. Because inaccurate PSDs are a primary reason for reported discrepancies between IPSD calculated mass and the gravimetric method, it is important to correct this deficiency in EEPS measurements. Recently, TSI has released additional EEPS calibration matrices ('soot' and 'Compact') which have shown better agreement with SMPS measurements under preliminary test conditions. This study further evaluates the performance of these new matrices relative to the original 'Default' matrix for diesel and biodiesel exhaust particles. Steady-state (75% engine load) emissions were generated by a light-duty diesel engine operating on (1) ultra-low sulfur diesel (ULSD) and (2) 100% soybean biodiesel. Raw EEPS data processed with each matrix were compared to simultaneously collected reference measurements from an SMPS. PSDs were evaluated based on their shape – i.e., multimodal fits of geometric mean diameter (GMD) and geometric standard deviation (GSD) – and concentration at peak particle diameter. For both fuels, all measurements agreed well in terms of the shape of the PSD: primary mode (accumulation) GMD ± 10nm, GSD ± 0.3. For ULSD, EEPS Default, Soot, and Compact concentrations were higher than the SMPS by factors of 1.9, 1.3, and 2.5, respectively. For biodiesel, EEPS Default, Soot, and Compact concentrations were higher than the SMPS by factors of 2.1, 1.7, and 2.4, respectively. Based on these results, the Soot matrix produced acceptable agreement between EEPS and SMPS measurements of ULSD exhaust particles. However, based on the factor of ~2 difference observed here, an additional calibration matrix may be necessary for the EEPS to accurately measure biodiesel exhaust particles. The IPSD method for estimating PM mass was applied to available data sets with corresponding gravimetric measurements (one ULSD transient cycle test and the same biodiesel steady-state test used for PSD evaluation). Real-time PSDs from each of the three EEPS matrices were used in combination with three sets of values assumed for size-dependent particle effective density (representing a range of potential conditions), resulting in nine IPSD estimates of PM mass corresponding to each gravimetric sample (one ULSD, one biodiesel). For the transient ULSD test, a widely used effective density distribution for fractal-like soot agglomerates resulted in good agreement between IPSD estimated mass and the gravimetric measurement (within 9% and 6% for Soot and Compact matrices, respectively). For the steady-state biodiesel test, assuming unit density (1g/cm³ for all particles) resulted in good agreement between IPSD estimated mass and the gravimetric measurement (within 7% and 2% for Soot and Compact matrices, respectively). These results support previous findings that the Soot matrix is currently the best available option for measurement of ULSD exhaust particles by the EEPS and that particle effective density distributions similar to the "fractal-like" one used here are an accurate estimate for ULSD exhaust particles under many conditions. However, based on the discrepancies between the EEPS and SMPS measured biodiesel exhaust PSDs observed here, as well as a current lack of information on the effective density of biodiesel exhaust particles, it is clear that additional research is necessary in order to understand the properties of biodiesel exhaust particles, especially as they relate to electrical mobility measurements and IPSD estimation of PM mass.

An increasing number of cancer patients is treated with proton beams or other light ion beams which allow to deliver dose precisely to the tumor. However, the depth dose distribution of these particles, which enables this precision, is sensitive to deviations from the treatment plan, as e.g. anatomical changes. Thus, to assure the quality of the treatment, a non-invasive in-vivo dose verification is highly desired. This monitoring of particle therapy relies on the detection of secondary radiation which is produced by interactions between the beam particles and the nuclei of the patient’s tissue. Up to now, the only clinically applied method for in-vivo dosimetry is Positron Emission Tomography which makes use of the beta+-activity produced during the irradiation (PT-PET). Since from a PT-PET measurement the applied dose cannot be directly deduced, the simulated distribution of beta+-emitting nuclei is used as a basis for the analysis of the measured PT-PET data. Therefore, the reliable modeling of the production rates and the spatial distribution of the beta+-emitters is required. PT-PET applied during instead of after the treatment is referred to as in-beam PET. A challenge concerning in-beam PET is the design of the PET camera, because a standard full-ring scanner is not feasible. For instance, a double-head PET camera is applicable, but low count rates and the limited solid angle coverage can compromise the image quality. For this reason, a detector system which provides a time resolution allowing the incorporation of time-of-flight information (TOF) into the iterative reconstruction algorithm is desired to improve the quality of the reconstructed images. Secondly, Prompt Gamma Imaging (PGI), a technique based on the detection of prompt gamma-rays, is currently pursued. Concerning the emissions of prompt gamma-rays during particle irradiation, experimental data is not sufficiently available, making simulations necessary. Compton cameras are based on the detection of incoherently scattered photons and are investigated with respect to PGI. Monte Carlo simulations serve for the optimization of the camera design and the evaluation of criteria for the selection of measured events. Thus, for in-beam PET and PGI dedicated detection systems and, moreover, profound knowledge about the corresponding radiation fields are required. Using various simulation codes, this thesis contributes to the modelling of the beta+-emitters and photons produced during particle irradiation, as well as to the evaluation and optimization of hardware for both techniques. Concerning the modeling of the production of the relevant beta+-emitters, the abilities of the Monte Carlo simulation code PHITS and of the deterministic, one-dimensional code HIBRAC were assessed. The Monte Carlo tool GEANT4 was applied for an additional comparison. For irradiations with protons, helium, lithium, and carbon, the depth-dependent yields of the simulated beta+-emitters were compared to experimental data. In general, PHITS underestimated the yields of the considered beta+-emitters in contrast to GEANT4 which provided acceptable values. HIBRAC was substantially extended to enable the modeling of the depth-dependent yields of specific nuclides. For proton beams and carbon ion beams HIBRAC can compete with GEANT4 for this application. Since HIBRAC is fast, compact, and easy to modify, it could be a basis for the simulations of the beta+-emitters in clinical application. PHITS was also applied to the modeling of prompt gamma-rays during proton irradiation following an experimental setup. From this study, it can be concluded that PHITS could be an alternative to GEANT4 in this context. Another aim was the optimization of Compton camera prototypes. GEANT4 simulations were carried out with the focus on detection probabilities and the rate of valid events. Based on the results, the feasibility of a Compton camera setup consisting of a CZT detector and an LSO or BGO detector was confirmed. Several recommendations concerning the design and arrangement of the Compton camera prototype were derived. Furthermore, several promising event selection strategies were evaluated. The GEANT4 simulations were validated by comparing simulated to measured energy depositions in the detector layers. This comparison also led to the reconsideration of the efficiency of the prototype. A further study evaluated if electron-positron pairs resulting from pair productions could be detected with the existing prototype in addition to Compton events. Regarding the efficiency and the achievable angular resolution, the successful application of the considered prototype as pair production camera to the monitoring of particle therapy is questionable. Finally, the application of a PET camera consisting of Resistive Plate Chambers (RPCs) providing a good time resolution to in-beam PET was discussed. A scintillator-based PET camera based on a commercially available scanner was used as reference. This evaluation included simulations of the detector response, the image reconstructions using various procedures, and the analysis of image quality. Realistic activity distributions based on real treatment plans for carbon ion therapy were used. The low efficiency of the RPC-based PET camera led to images of poor quality. Neither visually nor with the semi-automatic tool YaPET a reliable detectability of range deviations was possible. The incorporation of TOF into the iterative reconstruction algorithm was especially advantageous for the considered RPC-based PET camera in terms of convergence and artifacts. The application of the real-time capable back projection method Direct TOF for the RPCbased PET camera resulted in an image quality comparable to the one achieved with the iterative algorihms. In total, this study does not indicate the further investigation of RPC-based PET cameras with similar efficiency for in-beam PET application. To sum up, simulation studies were performed aimed at the progress of in-vivo dosimetry. Regarding the modeling of the beta+-emitter production and prompt gamma-ray emissions, different simulation codes were evaluated. HIBRAC could be a basis for clinical PT-PET simulations, however, a detailed validation of the underlying cross section models is required. Several recommendations for the optimization of a Compton Camera prototype resulted from systematic variations of the setup. Nevertheless, the definite evaluation of the feasibility of a Compton camera for PGI can only be performed by further experiments. For PT-PET, the efficiency of the detector system is the crucial factor. Due to the obtained results for the considered RPC-based PET camera, the focus should be kept to scintillator-based PET cameras for this purpose.

Nano-particle aerosols are one of the major types of air pollutants in the urban indoor and outdoor environments. Therefore, determination of mechanisms of formation, dispersion, evolution, and transformation of combustion aerosols near the major source of this type of air pollution - busy roads and road networks - is one of the most essential and urgent goals. This Thesis addresses this particular direction of research by filling in gaps in the existing physical understanding of aerosol behaviour and evolution. The applicability of the Gaussian plume model to combustion aerosols near busy roads is discussed and used for the numerical analysis of aerosol dispersion. New methods of determination of emission factors from the average fleet on a road and from different types of vehicles are developed. Strong and fast evolution processes in combustion aerosols near busy roads are discovered experimentally, interpreted, modelled, and statistically analysed. A new major mechanism of aerosol evolution based on the intensive thermal fragmentation of nano-particles is proposed, discussed and modelled. A comprehensive interpretation of mutual transformations of particle modes, a strong maximum of the total number concentration at an optimal distance from the road, increase of the proportion of small nano-particles far from the road is suggested. Modelling of the new mechanism is developed on the basis of the theory of turbulent diffusion, kinetic equations, and theory of stochastic evaporation/degradation processes. Several new powerful statistical methods of analysis are developed for comprehensive data analysis in the presence of strong turbulent mixing and stochastic fluctuations of environmental factors and parameters. These methods are based upon the moving average approach, multi-variate and canonical correlation analyses. As a result, an important new physical insight into the relationships/interactions between particle modes, atmospheric parameters and traffic conditions is presented. In particular, a new definition of particle modes as groups of particles with similar diameters, characterised by strong mutual correlations, is introduced. Likely sources of different particle modes near a busy road are identified and investigated. Strong anti-correlations between some of the particle modes are discovered and interpreted using the derived fragmentation theorem. The results obtained in this thesis will be important for accurate prediction of aerosol pollution levels in the outdoor and indoor environments, for the reliable determination of human exposure and impact of transport emissions on the environment on local and possibly global scales. This work will also be important for the development of reliable and scientifically-based national and international standards for nano-particle emissions.

Nano-particle aerosols are one of the major types of air pollutants in the urban indoor and outdoor environments. Therefore, determination of mechanisms of formation, dispersion, evolution, and transformation of combustion aerosols near the major source of this type of air pollution - busy roads and road networks - is one of the most essential and urgent goals. This Thesis addresses this particular direction of research by filling in gaps in the existing physical understanding of aerosol behaviour and evolution. The applicability of the Gaussian plume model to combustion aerosols near busy roads is discussed and used for the numerical analysis of aerosol dispersion. New methods of determination of emission factors from the average fleet on a road and from different types of vehicles are developed. Strong and fast evolution processes in combustion aerosols near busy roads are discovered experimentally, interpreted, modelled, and statistically analysed. A new major mechanism of aerosol evolution based on the intensive thermal fragmentation of nano-particles is proposed, discussed and modelled. A comprehensive interpretation of mutual transformations of particle modes, a strong maximum of the total number concentration at an optimal distance from the road, increase of the proportion of small nano-particles far from the road is suggested. Modelling of the new mechanism is developed on the basis of the theory of turbulent diffusion, kinetic equations, and theory of stochastic evaporation/degradation processes. Several new powerful statistical methods of analysis are developed for comprehensive data analysis in the presence of strong turbulent mixing and stochastic fluctuations of environmental factors and parameters. These methods are based upon the moving average approach, multi-variate and canonical correlation analyses. As a result, an important new physical insight into the relationships/interactions between particle modes, atmospheric parameters and traffic conditions is presented. In particular, a new definition of particle modes as groups of particles with similar diameters, characterised by strong mutual correlations, is introduced. Likely sources of different particle modes near a busy road are identified and investigated. Strong anti-correlations between some of the particle modes are discovered and interpreted using the derived fragmentation theorem. The results obtained in this thesis will be important for accurate prediction of aerosol pollution levels in the outdoor and indoor environments, for the reliable determination of human exposure and impact of transport emissions on the environment on local and possibly global scales. This work will also be important for the development of reliable and scientifically-based national and international standards for nano-particle emissions.

Master of Science
Department of Biological & Agricultural Engineering
Ronaldo G. Maghirang
Large cattle feedlots emit considerable amounts of particulate matter (PM), including TSP (total suspended particulates), PM[subscript]10 (PM with equivalent aerodynamic diameter of 10 μm or less), and PM[subscript]2.5 (PM with equivalent aerodynamic diameter of 2.5 μm or less). Particulate emissions result from pen surface disturbance by cattle hoof action, vehicle traffic on unpaved roads and alleyways, and wind erosion. Research is needed to determine concentrations of various size fractions, size distribution, and emission rates from various sources in feedlots. This research was conducted to measure particle size distribution using laser diffraction method and estimate emissions from unpaved roads and wind erosion. Particle size distribution and concentrations of PM[subscript]10 and PM[subscript]2.5 at a commercial cattle feedlot in Kansas (Feedlot 1) were measured over a 2-yr period. The feedlot had a capacity of 30,000 head and total pen area of 50 ha and was equipped with a sprinkler system for dust control. Collocated low-volume samplers for TSP, PM[subscript]10, and PM[subscript]2.5 were used to measure concentrations of TSP, PM[subscript]10, and PM[subscript]2.5 at the upwind and downwind edges of the feedlot. Dust samples that were collected by TSP samplers were analyzed with a laser diffraction analyzer to determine particle size distribution. Particle size distribution at the downwind edge of the feedlot was also measured with micro-orifice uniform deposit impactor (MOUDI). The laser diffraction method and MOUDI did not differ significantly in mean geometric mean diameter (13.7 vs. 13.0 μm) but differed in mean geometric standard deviation (2.9 vs. 2.3). From laser diffraction and TSP data, PM[subscript]10 and PM[subscript]2.5 concentrations were also calculated and were not significantly different from those measured by low-volume PM[subscript]10 and PM[subscript]2.5 samplers (122 vs. 131 μg/m[superscript]3 for PM[subscript]10; 26 vs. 35 μg/m[superscript]3 for PM[subscript]2.5). Both PM[subscript]10 and PM[subscript]2.5 fractions decreased as pen surface moisture contents increased, while the PM[subscript]2.5/PM[subscript]10 ratio did not change much with pen surface moisture content. Published emission models were used to estimate PM[subscript]10 emissions from unpaved roads and wind erosion at Feedlot 1 and another nearby feedlot (Feedlot 2). Feedlot 2 had a capacity of 30,000 head, total pen surface area of 59 ha, and used water trucks for dust control. Estimated PM[subscript]10 emissions from unpaved roads and wind erosion were less than 20% of total PM[subscript]10 emissions obtained from inverse dispersion modeling. Further research is needed to establish the applicability of published emission estimation models for cattle feedlots.

This thesis is an evaluative study of air pollution emissions from different sources in Australia and overseas. It investigates indoor and outdoor sources, including indoor combustion, electric equipment, asphalt pavement, forest fires and vehicular traffic. Based on evaluating sources, a simple practical method is proposed to identify pollution sources. This research has important scientific implications and potential for future practical applications, given the paucity of quantitative air quality studies available for pollution control.