In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3-3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20-54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·10 15 (kg fuel ) −1 in a roadside environment, 2.6·10 15 (kg fuel ) −1 in a street canyon, and 2.9·10 15 (kg fuel ) −1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·10 12 (kg fuel ) −1 to a high value of 4.3·10 15 (kg fuel ) −1 . These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.nanocluster aerosol | atmospheric aerosol | combustion-derived nanoparticles | air pollution | traffic emission D etailed characterization of aerosol sources is required to understand climate impacts and health effects of atmospheric aerosols, as well as to develop technologies and policies capable of mitigating air pollution in urbanized areas. In densely populated areas, one of the most significant source of particles is traffic (1, 2). Owing to their small size and complicated chemical and physical characteristics (3-6), atmospheric particles resulting from traffic emissions pose a significant risk to human health (7-12), and also contribute to anthropogenic forcing of climate (13,14). Previous research on vehicular emissions has demonstrated the presence of soot and ash (3, 15) and solid sub-10-nm core particles (4-6) in primary emissions from vehicles and engines and their variation, depending on vehicle technologies (4, 6), the properties of fuels and lubricant oils (15, 16), and driving conditions (15-17). In addition to particles, exhaust typically contains species that reside in the gaseous phase in the undiluted high-temperature exhaust (5, 18, 19) but condense or even nucleate to the particle phase immediately after the exhaust is released to the atmosphere. Here, we term such aerosols delayed primary aerosols, because particle precursors exist already in the u...
Abstract. The assessment of the climatic impacts and adverse health effects of atmospheric aerosol particles requires detailed information on particle properties. However, very limited information is available on the morphology and phase state of secondary organic aerosol (SOA) particles. The physical state of particles greatly affects particulatephase chemical reactions, and thus the growth rates of newly formed atmospheric aerosol. Thus verifying the physical phase state of SOA particles gives new and important insight into their formation, subsequent growth, and consequently potential atmospheric impacts. According to our recent study, biogenic SOA particles produced in laboratory chambers from the oxidation of real plant emissions as well as in ambient boreal forest atmospheres can exist in a solid phase in size range >30 nm. In this paper, we extend previously published results to diameters in the range of 17-30 nm. The physical phase of the particles is studied by investigating particle bounce properties utilizing electrical low pressure impactor (ELPI). We also investigate the effect of estimates of particle density on the interpretation of our bounce observations. According to the results presented in this paper, particle bounce clearly decreases with decreasing particle size in sub 30 nm size range. The comparison measurements by ammonium sulphate and investigation of the particle impaction velocities strongly suggest that the deCorrespondence to: A. Virtanen (annele.virtanen@tut.fi) creasing bounce is caused by the differences in composition and phase of large (diameters greater than 30 nm) and smaller (diameters between 17 and 30 nm) particles.
Abstract. Changes in vehicle emission reduction technologies significantly affect traffic-related emissions in urban areas. In many densely populated areas the amount of traffic is increasing, keeping the emission level high or even increasing. To understand the health effects of traffic-related emissions, both primary (direct) particulate emission and secondary particle formation (from gaseous precursors in the exhaust emissions) need to be characterized. In this study, we used a comprehensive set of measurements to characterize both primary and secondary particulate emissions of a Euro 5 level gasoline passenger car. Our aerosol particle study covers the whole process chain in emission formation, from the tailpipe to the atmosphere, and also takes into account differences in driving patterns. We observed that, in mass terms, the amount of secondary particles was 13 times higher than the amount of primary particles. The formation, composition, number and mass of secondary particles was significantly affected by driving patterns and engine conditions. The highest gaseous and particulate emissions were observed at the beginning of the test cycle when the performance of the engine and the catalyst was below optimal. The key parameter for secondary particle formation was the amount of gaseous hydrocarbons in primary emissions; however, also the primary particle population had an influence.
Abstract. The phase state of atmospheric aerosols has an impact on their chemical aging and their deliquescence and thus their ability to act as cloud condensation nuclei (CCN). The phase change of particles can be induced by the deliquescence or efflorescence of water or by chemical aging.Existing methods, such as tandem differential mobility analysis rely on the size change of particles related to the water uptake or release.To address the need to study the phase change induced by mass-preserving and nearly mass-preserving processes a new method has been developed. The method relies on the physical impaction of particles on a smooth substrate and subsequent counting of bounced particles by a condensation particle counter (CPC). The connection between the bounce probability and physical properties of particles is so far qualitative.To evaluate the performance of this method, the phase state of ammonium sulfate and levoglucosan, crystalline and amorphous solid, in the presence of water vapor was studied. The results show a marked difference in particle bouncing properties between substances -not only at the critical relative humidity level, but also on the slope of the bouncing probability with respect to humidity. This suggests that the method can be used to differentiate between amorphous and crystalline substances as well as to differentiate between liquid and solid phases.
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