| 21. |
- Rissler, Jenny, et al.
(författare)
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Effective Density and Mixing State of Aerosol Particles in a Near-Traffic Urban Environment.
- 2014
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Ingår i: Environmental Science & Technology. - : American Chemical Society (ACS). - 1520-5851 .- 0013-936X. ; 48:11, s. 6300-6308
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Tidskriftsartikel (refereegranskat)abstract
- In urban environments, airborne particles are continuously emitted, followed by atmospheric aging. Also, particles emitted elsewhere, transported by winds, contribute to the urban aerosol. We studied the effective density (mass-mobility relationship) and mixing state with respect to the density of particles in central Copenhagen, in wintertime. The results are related to particle origin, morphology, and aging. Using a differential mobility analyzer-aerosol particle mass analyzer (DMA-APM), we determined that particles in the diameter range of 50-400 nm were of two groups: porous soot aggregates and more dense particles. Both groups were present at each size in varying proportions. Two types of temporal variability in the relative number fraction of the two groups were found: soot correlated with intense traffic in a diel pattern and dense particles increased during episodes with long-range transport from polluted continental areas. The effective density of each group was relatively stable over time, especially of the soot aggregates, which had effective densities similar to those observed in laboratory studies of fresh diesel exhaust emissions. When heated to 300 °C, the soot aggregate volatile mass fraction was ∼10%. For the dense particles, the volatile mass fraction varied from ∼80% to nearly 100%.
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| 26. |
- Wittbom, Cerina, et al.
(författare)
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Cloud droplet activity changes of soot aerosol upon smog chamber ageing
- 2014
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 14:18, s. 9831-9854
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Tidskriftsartikel (refereegranskat)abstract
- Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC), to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA) precursors were processed by UV radiation in a 6m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations <= 2 %, i. e. the BC core coated with primary organic aerosol (POA) from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatility organic compounds (IVOCs) in the diesel engine exhaust. The change of cloud condensation nuclei (CCN) properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I) organic fraction of the particle, (II) chemical properties of this fraction (e. g. primary or secondary organic aerosol), (III) particle size, and (IV) particle morphology. Applying kappa-K hler theory, using a kappa SOA value of 0.13 (derived from independent input parameters describing the organic material), showed good agreement with cloud droplet activation measurements for particles with a SOA mass fraction >= 0.12 (slightly aged particles). The activation properties are enhanced with only a slight increase in organic material coating the soot particles (SOA mass fraction < 0.12), however not as much as predicted by K hler theory. The discrepancy between theory and experiments during the early stages of ageing might be due to solubility limitations, unevenly distributed organic material or hindering particle morphology. The change in properties of soot nanoparticles upon photochemical processing clearly increases their hygroscopicity, which affects their behaviour both in the atmosphere and in the human respiratory system.
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