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.

Depuis la révolution industrielle en Europe (XIXe siècle), les nombreuses activités anthropiques ont provoqué des changements environnementaux globaux considérables. La composition de l'atmosphère terrestre en particulier, a été fortement modifiée par l'émission de polluants gazeux et particulaires. Actuellement, l'industrie métallurgique de seconde fusion contribue de façon significative aux émissions atmosphériques de métaux. C'est pourquoi ce travail de thèse s'est focalisé sur l'étude des transferts et impacts sur les sols, les végétaux et l'homme, des particules émises par le procédé de recyclage du plomb en relation avec leurs propriétés physico-chimiques. Trois sources principales d'émissions de particules ont été identifiées dans le procédé du recyclage du plomb et caractérisées en vue d'étudier les impacts potentiels sur les cibles végétales et humaines. Les particules échantillonnées (postes de travail et émissions canalisées) et ségréguées en fonction de leur taille (PMtot, PM10 et PM2,5) sont principalement composées de métaux (jusqu'à 50% en masse de la composition totale en métaux de transition, alcalins et alcalino-terreux), avec une majeur partie de plomb (25-45 %). Les spéciations majoritaires du plomb sont la galène (PbS), le sulfate du plomb (PbSO4) ou dérivés (xPbO.PbSO4 x=1,2 ou 3). L'étude du transfert des particules dans le sytème sol-plante a montré que, lorsque la taille des particules de process présentes dans le sol diminue (de 10µm à 2.5µm), le tranfert du plomb vers les parties aériennes des salades augmente de 20%. Le transfert foliaire de plomb issu des particules de process a été mis en évidence et des mécanismes d'absorption.ont été proposés. Enfin, l'étude exploratoire des particules riches en plomb sur la santé humaine a permis de montrer que la diminition de la taille des particules ingérées augmentait la bioaccessibilité gastrique du plomb. Dans le cas de l'inhalation, il a été démontré que les particules n'induisaient pas de cytotoxicité jusqu'à 50µg/cm2, mais provoquaient une réponse inflammatoire dose-dépendante des cellules épithéliales pulmonaires. / Since the Industrial Revolution in Europe (XIXe century), human activities have caused significant global environmental changes. The composition of the atmosphere in particular, has been extensively modified by the emission of gaseous and particulate pollutants. Currently, the secondary (or recycling) metallurgical industry contributes significantly to air emissions of metals. Therefore, this thesis focused on the study of transfers and impacts on soils, plants and humans, of particles from the recycling process of lead in relation to their physicochemical properties. Three main sources of particulate emissions have been identified in the process of recycling lead and characterized, to study the potential impacts on plant and human targets. The particles sampled (workstations and channelled emissions), and segregated according to their size (PMtot, PM10 and PM2, 5), are mainly composed of metals (up to 50% by weight of the total composition in transition metals alkaline and alkaline), with a major part of lead (25-45%). The major speciations of lead are galena (PbS), lead sulfate (PbSO4) or derivatives (xPbO.PbSO4 x = 1,2 or 3). The study of transfer of particles in the soil-plant system has shown that when the particle size of processes in the soil decreases (from 2.5µm to 10µm), the transfer of lead into the aerial parts of lettuce growing at 20 %. The uptake of lead from particles process by leaves has been demonstrated and mechanisms of absorption have been proposed. Finally, exploratory study of lead-rich particles on human health has shown that diminution of the size of particles ingested increased gastric bioaccessibility of lead. In the case of inhalation, it was shown that the particles did not induce cytotoxicity up 50µg/cm2, but caused a dose-dependent inflammatory response of lung epithelial cells

Epidemiological research around the world has shown that exposure of urban populations to fine microparticles (PM2.5) suspended in air from, among other things, car combustion, is responsible for many cases of lung and cardiovascular disease and even mortality. However, most of these studies examine urban centers as ensembles without considering that population exposure to microparticles is not homogeneous across an urban space. For example, individuals living near major arterial roads are much more exposed to microparticles than others living in low traffic neighborhoods. Unfortunately, ground stations measuring PM2.5 are few and far between to generate accurate microparticle concentration maps at fine scales. One way to spatialize information on microparticle concentrations is to introduce remotely sensed images that allows to calculate an optical parameter of aerosols, their optical depth. The use of medium-to-fine-resolution images is not common in this area. So, we wanted to look at their potential. Tests with hyperspectral and multispectral images at these resolutions have shown that optical depth can be estimated with enough accuracy. The AODFinder software developed for this purpose performs well. Unfortunately, the small sample of AOD values and PM2.5 concentration measurements did not allow us to conclude on the possibility of using AOD as a proxy for PM2.5 and thus on the possibility of refining microparticle monitoring at the local level. / Des recherches épidémiologiques à travers le monde ont mis en évidence que l’exposition des populations urbaines aux microparticules fines (PM2.5) en suspension dans l’air provenant, entre autres, de la combustion automobile, est à l’origine des nombreux cas des maladies pulmonaires et cardiovasculaires et même des cas de mortalité. Cependant, la plupart de ces études examinent les centres urbains comme des ensembles sans tenir compte que l’exposition des populations aux microparticules n’est pas homogène à travers un espace urbain. À titre d’exemple, les individus demeurant à proximité de grandes artères routières sont beaucoup plus exposés aux microparticules que d’autres demeurant dans des quartiers de faible circulation. Malheureusement, les stations terrestres de mesure des PM2.5 sont peu nombreuses pour permettre de générer des cartes de concentration des microparticules précises à des échelles fines. Un moyen pour spatialiser l’information sur les concentrations des microparticules est d’introduire l’imagerie de télédétection qui permet de calculer un paramètre optique des aérosols, leur profondeur optique. L’utilisation des images à résolution moyenne à fine n’est pas chose courante dans ce domaine. Ainsi nous avons voulu examiner leur potentiel. Les tests avec des images hyperspectrale et multispectrale à ces résolutions ont montré que la profondeur optique peut être estimer avec suffisamment de précision. Le logiciel AODFinder développé à cette fin se comporte bien. Malheureusement le faible échantillon des valeurs de AOD et des mesures des concentrations des PM2.5 ne nous a pas permis de se prononcer sur la possibilité d’utiliser le AOD comme proxy des PM2.5 et ainsi sur la possibilité de raffiner le monitoring des microparticules à l’échelle locale.

Contexte : L’influence de la végétation urbaine sur le développement de l’asthme infantile est controversée. Il est avancé que les arbres (canopée urbaine) réduisent la pollution atmosphérique, un facteur de risque de l’asthme mais également, que certains peuvent émettre des pollens et des composés organiques volatils biogéniques, tout-autant des facteurs de risque pour le développement de l’asthme chez l’enfant. Cependant, les risques associés à la canopée urbaine ont été étudiés à l’aide de données rudimentaires souvent, sans considération pour la saison. Objectifs : 1) Caractériser l’association entre la végétation urbaine et le développement de l’asthme en distinguant la végétation totale et de la canopée des feuillus et de conifères, en fonction des saisons de production de pollens et de feuilles des arbres. 2) Évaluer l’influence de la canopée d’arbres sur l’association entre les particules fines (PM2.5) et le développement de l’asthme infantile. Méthodes : Nous avons utilisé les données d’une cohorte de naissance ouverte contenant tous les enfants nés sur l’île de Montréal (Canada) entre 2000 et 2015 et suivis jusqu’à leurs 12 ans, créée à partir de données médico-administratives agrégées. L’exposition à la végétation totale a été estimée à l’aide d’une mesure satellitaire appelée l’indice de végétation par différence normalisée (NDVI) et l’exposition à la canopée urbaine, a été estimée à l’aide de données de télédétection laser aéroporté - LiDAR permettant d’estimer l’aire de la canopée des feuillus et des conifères dans un rayon de 250 m autour de la résidence des participants, tout au long du suivi. En dehors des saisons de pollens et de feuilles des arbres, les variables d’expositions ont été fixées à zéro. Des modèles de risque proportionnels de Cox ont été développés pour estimer le risque associé au NDVI et aux canopées d’arbres lors de la saison de pollens et de feuilles des arbres. La non-linéarité a été modélisée à l’aide de catégories et de splines cubiques pour les expositions. Nous avons ensuite évalué l’effet de la canopée urbaine sur l’association entre les particules fines (PM2.5) et le développement de la maladie. Résultats : Parmi les 352 946 enfants inclus dans la cohorte et suivis pour un total de 1,7 millions de personnes-années, 30 816 nouveaux cas d'asthme ont été identifiés pour un taux moyen de nouveaux cas d’asthme était de 17,79 nouveaux cas par 1 000 personnes-années. Le NDVI moyen annuel s’élevait à 0,365 (Écart-type (ET) : 0,106) dans un rayon de 250 m centré sur la résidence des participants. En saison de pollens, le NDVI moyen se réduisait à 0,089 (ET : 0,106) et à 0,15 (ET : 0,185) en saison de feuilles. En moyenne, les enfants étaient exposés à trois fois plus de canopées de feuillus (moyenne = 12,3 (ET : 17,0) ×103 m2) que de conifères en saison de feuilles (moyenne= 4,5 (ET : 4,3) ×103 m2), et sept fois plus en saison de pollens. Nos analyses ont révélé des associations distinctes en fonction des saisons pour le NDVI et la canopée de feuillus. Trop peu de conifères étaient présents pour tirer des conclusions quant à leur effet. Les analyses à l’aide des splines cubiques pour les expositions ont indiqué la présence de relations non-linéaires. La catégorisation des expositions a indiqué que des niveaux moyens de canopée de feuillus en saisons de feuilles avaient un effet protecteur lorsque comparés aux non-exposés (Rapport de Risque (RR): 0,694 ; Intervalle de confiance (IC95%) : 0,680 – 0,708). À l’inverse, pour les journées de pollens, la canopée de feuillus autour de la résidence était associée à l’augmentation du risque (RR =1,082 (IC95% 1,056 – 1,108)). Pour les catégories de NDVI annuel (non subdivisé par saisons), aucune association n’a été détectée. Pour finir, la canopée d’arbres et le NDVI n’ont influencé que très faiblement l’association entre les PM2.5 régionaux et le développement de l’asthme infantile. Cependant, une légère interaction a été observée entre les feuillus en saison de feuilles et les PM2.5. Des niveaux élevés de feuillus autour de la résidence en période de feuilles diminueraient le risque d’asthme associé à l’exposition aux PM2.5. Discussions : Les résultats suggèrent que l’effet de la végétation varie en fonction des saisons. L’effet capté par le NDVI semble être en grande partie attribuable à la canopée de feuillus. L’influence de la végétation sur l’association entre les PM2.5 et le développement de l’asthme est très faible. / Background: The influence of urban vegetation and tree canopy on the development of childhood asthma is controversial. It is argued that trees reduce air pollution, a risk factor for asthma, but at the same time, some species emit pollens and biogenic volatile organic compounds, all of which are risk factors for the development of asthma in children. Yet, the risks associated with the urban canopy have been studied using rudimentary data, often without consideration for the season. Objectives: 1) To characterize the association between urban vegetation and asthma development by distinguishing between total vegetation and deciduous and evergreen tree canopy, according to the pollen and leaf-on seasons. 2) To assess the influence of tree canopy on the association between fine particulate matter (PM2.5) and the development of childhood asthma. Methods: We used data from an open birth cohort containing all children born on the island of Montreal, Canada, between 2000 and 2015 and followed up until their 13th birthday, created from aggregated medico-administrative data. Exposure to total vegetation was estimated using a satellite measure called the normalized difference vegetation index (NDVI). Exposure to the urban canopy was estimated using LiDAR, an airborne remote laser sensing technology that was used to estimate the area of the deciduous and coniferous canopy within a 250 m buffer centered on participants' residential postal codes, updated throughout the follow-up. Outside of the pollen and tree leaf-on seasons, exposure variables were set to zero. Cox proportional hazard models were developed to estimate the risk associated with NDVI and tree canopies for the pollen and tree leaf-on seasons. Nonlinearity was modeled using categories and restricted cubic splines for exposures variables. We then assessed the effect of the urban canopy on the association between fine particulate matter (PM2.5) and asthma development. Results: Among the 352,946 children included in the cohort and followed for a total of 1.7 million person-years, 30,816 new asthma cases were detected, for an average incidence rate of 17.79 new cases per 1,000 person-years. The mean annual NDVI was 0.365 (Standard Deviation (SD): 0.106) within a 250 m buffer centered on participants' residential postal codes. In the pollen season, the mean NDVI was reduced to 0.089 (SD: 0.106) and to 0.15 (SD: 0.185) for the leaf-on season. On average, children were exposed to three times as much deciduous canopy (mean= 12.3 (SD: 17.0) ×103 m2) as coniferous canopy in leaf-on season (mean= 4.5 (SD: 4.3) ×103 m2), and seven times as much in pollen season. Our analyses revealed distinct associations by season for NDVI and deciduous trees. Too few evergreens were present to draw conclusions about their effect. Cubic spline analyses for exposures indicated the presence of nonlinear relationships. Exposure categorization indicated that average levels of deciduous trees canopy in the leaf-on season had a protective effect when compared to unexposed (Hazard Ratio (HR): 0.694; Confidence Interval (CI95%): 0.680 - 0.708). Conversely, for pollen days, the residential deciduous canopy was associated with increased risk (HR =1.082 (CI95% 1.056 - 1.108)). For annual NDVI categories (not subdivided by season), no association was detected. Finally, tree canopy and NDVI only weakly influenced the association between regional PM2.5 and childhood asthma development. However, a slight interaction was observed between leaf-on-season deciduous canopy and PM2.5. High levels of deciduous trees canopy at residential postal codes during the leaf-on season decrease the risk of asthma associated with PM2.5 exposure. Discussion: Our results suggest that the effect of vegetation varies with season. The effect captured by NDVI appears to be largely due to the deciduous canopy. The influence of vegetation on the association between PM2.5 and asthma development appeared to be marginal.

Atmospheric fine particulate matter (PM2.5), which is mostly formed in the atmosphere from precursor gases, contributes to numerous environmental and health concerns. Quantifying the ambient concentrations of PM2.5 and precursor gases can be challenging. Hence, many scientific questions about the formation, chemical composition, and gas/particle partitioning of PM2.5 remain unanswered. Ambient Ion Monitor - Ion Chromatography (AIM-IC) was characterized and utilized to measure the water-soluble composition of PM2.5 (dominated by pNH4+, pSO42-, and pNO3-) and associated precursor gases (dominated by NH3(g), SO2(g), and HNO3(g)) during two field campaigns. The AIM-IC detection limits for hourly sampling were determined to be 3 - 45 ng m-3. The response time for “sticky” gases was significantly improved with a nylon denuder membrane. A novel inlet configuration for the AIM-IC, which minimizes sampling inlet losses and carryover in sample analyses, was implemented. Measurements from the BAQS-Met 2007 campaign were utilized to assess the accuracy of the AURAMS model and investigate gas/particle partitioning in SW Ontario. Due to high sulphate levels, NH3(g) was the limiting chemical factor in the formation and gas/particle partitioning of PM2.5. The errors in the predictions of relative humidity and free ammonia were responsible for the poor agreement iii between modelled and measured pNO3- values. The AIM-IC measurements from the CalNex 2010 study were compared to the CMAQ model and utilized to investigate the gas/particle partitioning in Bakersfield, CA. Very high NH3(g) concentrations were observed, and the formation and partitioning of PM2.5 was limited by HNO3(g) and H2SO4. Evidence of rapid removal of HNO3(g) by interactions with super-micron dust particles, and possibly with the alkaline surface was found. CMAQ exhibited significant biases in the predicted concentrations of pSO42-, NH3(g) and HNO3(g).

Atmospheric fine particulate matter (PM2.5), which is mostly formed in the atmosphere from precursor gases, contributes to numerous environmental and health concerns. Quantifying the ambient concentrations of PM2.5 and precursor gases can be challenging. Hence, many scientific questions about the formation, chemical composition, and gas/particle partitioning of PM2.5 remain unanswered. Ambient Ion Monitor - Ion Chromatography (AIM-IC) was characterized and utilized to measure the water-soluble composition of PM2.5 (dominated by pNH4+, pSO42-, and pNO3-) and associated precursor gases (dominated by NH3(g), SO2(g), and HNO3(g)) during two field campaigns. The AIM-IC detection limits for hourly sampling were determined to be 3 - 45 ng m-3. The response time for “sticky” gases was significantly improved with a nylon denuder membrane. A novel inlet configuration for the AIM-IC, which minimizes sampling inlet losses and carryover in sample analyses, was implemented. Measurements from the BAQS-Met 2007 campaign were utilized to assess the accuracy of the AURAMS model and investigate gas/particle partitioning in SW Ontario. Due to high sulphate levels, NH3(g) was the limiting chemical factor in the formation and gas/particle partitioning of PM2.5. The errors in the predictions of relative humidity and free ammonia were responsible for the poor agreement iii between modelled and measured pNO3- values. The AIM-IC measurements from the CalNex 2010 study were compared to the CMAQ model and utilized to investigate the gas/particle partitioning in Bakersfield, CA. Very high NH3(g) concentrations were observed, and the formation and partitioning of PM2.5 was limited by HNO3(g) and H2SO4. Evidence of rapid removal of HNO3(g) by interactions with super-micron dust particles, and possibly with the alkaline surface was found. CMAQ exhibited significant biases in the predicted concentrations of pSO42-, NH3(g) and HNO3(g).

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.