Emissions, dynamics and dispersion of particles in polluted air

Sammanfattning: The main objective of this thesis is to yield information on how atmospheric fine and ultrafine particles are dispersed in populated areas. Quantitative information on emissions, transport and removal is needed to assess the health risks of inhalable particles. Most effort is dedicated to describe, on the local and urban scales, the distribution of ultrafine particles (and thereby also total number concentrations) originating from traffic emissions. A minor part addresses the dispersion of toxic particles of industrial origin, dispersed over regional scales. The importance of aerosol dynamics for the distribution of ultrafine particles is assessed by coupling a three-dimensional dispersion model to a monodisperse aerosol model. Meteorological forcing, sometimes in a complex geometry, is simulated by a CFD model on the local scale and by a weather forecast model on the larger scales.The principal result of the study is that particle number concentrations can, at least for Swedish conditions, be simulated and quantitatively assessed in urban models in a similar way as particle mass or gaseous pollutants. The variability of the emissions and the removal effects of coagulation and dry deposition are investigated. Vehicle emissions of particle number vary with a factor of two depending on ambient temperature, with higher concentrations during cold conditions. Other important factors that determine particle emissions are fleet composition, vehicle speed (especially for gasoline-fueled cars) and the dilution rate in the microenvironment where emissions take place. Coagulation affects particle number concentrations in highly polluted environments like car tunnels or street canyons under low wind speed conditions, while it is of less importance in the urban background (reduced number concentrations of a few percent, as compared to completely inert particles). Dry deposition is effective over the road surface, due to the velocities and turbulence produced by moving vehicles. Dry deposition also has significant effects on the urban background concentrations, reducing average levels with up to 20-30%. Dry deposition is also shown to be an important mechanism to remove fine particulate mass on the regional scale.Simulated particle number concentrations, based on emission factors determined for the local vehicle fleet and influenced by aerosol dynamic processes, are evaluated against measured concentrations for three different traffic microenvironments and also for the entire Stockholm area. Regional dispersion of arsenic in PM10 is assessed and model results compared to measurements in Central and Northern Chile.