| 1. |
- Karjalainen, Panu, et al.
(author)
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Time-resolved characterization of primary particle emissions and secondary particle formation from a modern gasoline passenger car
- 2016
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:13, s. 8559-8570
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Journal article (peer-reviewed)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.
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| 2. |
- Lee, Ben H, et al.
(author)
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Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets.
- 2016
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In: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 1091-6490. ; 113:6, s. 1516-21
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Journal article (peer-reviewed)abstract
- Speciated particle-phase organic nitrates (pONs) were quantified using online chemical ionization MS during June and July of 2013 in rural Alabama as part of the Southern Oxidant and Aerosol Study. A large fraction of pONs is highly functionalized, possessing between six and eight oxygen atoms within each carbon number group, and is not the common first generation alkyl nitrates previously reported. Using calibrations for isoprene hydroxynitrates and the measured molecular compositions, we estimate that pONs account for 3% and 8% of total submicrometer organic aerosol mass, on average, during the day and night, respectively. Each of the isoprene- and monoterpenes-derived groups exhibited a strong diel trend consistent with the emission patterns of likely biogenic hydrocarbon precursors. An observationally constrained diel box model can replicate the observed pON assuming that pONs (i) are produced in the gas phase and rapidly establish gas-particle equilibrium and (ii) have a short particle-phase lifetime (∼2-4 h). Such dynamic behavior has significant implications for the production and phase partitioning of pONs, organic aerosol mass, and reactive nitrogen speciation in a forested environment.
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| 3. |
- Lee, Shan Hu, et al.
(author)
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Isoprene suppression of new particle formation : Potential mechanisms and implications
- 2016
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In: Journal of Geophysical Research: Atmospheres. - 2169-897X. ; 121:24, s. 14-635
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Journal article (peer-reviewed)abstract
- Secondary aerosols formed from anthropogenic pollutants and natural emissions have substantial impacts on human health, air quality, and the Earth's climate. New particle formation (NPF) contributes up to 70% of the global production of cloud condensation nuclei (CCN), but the effects of biogenic volatile organic compounds (BVOCs) and their oxidation products on NPF processes in forests are poorly understood. Observations show that isoprene, the most abundant BVOC, suppresses NPF in forests. But the previously proposed chemical mechanism underlying this suppression process contradicts atmospheric observations. By reviewing observations made in other forests, it is clear that NPF rarely takes place during the summer when emissions of isoprene are high, even though there are sufficient concentrations of monoterpenes. But at present it is not clear how isoprene and its oxidation products may change the oxidation chemistry of terpenes and how NOx and other atmospheric key species affect NPF in forest environments. Future laboratory experiments with chemical speciation of gas phase nucleation precursors and clusters and chemical composition of particles smaller than 10 nm are required to understand the role of isoprene in NPF. Our results show that climate models can overpredict aerosol's first indirect effect when not considering the absence of NPF in the southeastern U.S. forests during the summer using the current nucleation algorithm that includes only sulfuric acid and total concentrations of low-volatility organic compounds. This highlights the importance of understanding NPF processes as function of temperature, relative humidity, and BVOC compositions to make valid predictions of NPF and CCN at a wide range of atmospheric conditions.
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