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Discussion papers
https://doi.org/10.5194/acp-2019-330
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-330
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 18 Apr 2019

Research article | 18 Apr 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Dual effect of anthropogenic emissions on the formation of biogenic SOA

Eetu Kari1, Liqing Hao1, Arttu Ylisirniö1, Angela Buchholz1, Ari Leskinen1,2, Pasi Yli-Pirilä3, Ilpo Nuutinen3,6, Kari Kuuspalo3,6, Jorma Jokiniemi3, Celia Faiola4,5, Siegfried Schobesberger1, and Annele Virtanen1 Eetu Kari et al.
  • 1Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
  • 2Finnish Meteorological Institute, Kuopio, Finland
  • 3Department of Environmental and Biological Sciences, University of Eastern Finland, Kuopio, Finland
  • 4Department of Ecology and Evolutionary Biology, University of California Irvine, Irvine, CA, USA
  • 5Department of Chemistry, University of California Irvine, Irvine, CA, USA
  • 6current address: Savonia University of Applied Sciences, Kuopio, Finland

Abstract. The fraction of gasoline direct injection (GDI) vehicles comprising the total vehicle pool is projected to increase in the future. However, thorough knowledge about the influence of GDI engines on important atmospheric chemistry processes is missing—from their contribution to secondary organic aerosol (SOA) precursor emissions, SOA formation, and potential role in biogenic-anthropogenic interactions. The objectives of this study were to 1) characterize emissions from modern GDI vehicle and investigate their role in SOA formation chemistry and 2) investigate biogenic-anthropogenic interactions related to SOA formation from a mixture of GDI vehicle emissions and a model biogenic compound, α-pinene. Specifically, we studied SOA formation from modern GDI vehicle emissions during the constant load driving. In this study we show that SOA formation from GDI vehicle emissions was observed in each experiment. VOCs measured with the PTR-ToF-MS could account for 19−42% of total SOA mass generated in each experiments. This suggests there were lower volatility intermediate-VOCs (IVOCs) and semi-VOCs (SVOCs) in the GDI exhaust that likely contributed to SOA production but were not detected with the instrumentation used in this study. This study also demonstrates that two distinct mechanisms caused by anthropogenic emissions suppress α-pinene SOA mass yield. The first suppressing effect was the presence of NOx. This mechanism is consistent with previous reports demonstrating suppression of biogenic SOA formation in the presence of anthropogenic emissions. Our results imply that the second suppressing effect was the presence of anthropogenic gas-phase species that suppressed biogenic SOA formation by changing the gas-phase chemistry of α-pinene. This change in oxidation pathways led to formation of α-pinene oxidation products that most likely do not have vapor pressures low enough to partition into the particle phase. Overall, the presence of gasoline vehicle exhaust caused more than 50 % suppression in α-pinene SOA mass yield compared to the α-pinene SOA mass yield measured in the absence of an anthropogenic influence.

Eetu Kari et al.
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Short summary
We present for the first time dual effect of GDI vehicle exhaust on α-pinene SOA mass yield suppression. The first effect is well-known NOx effect, but the second effect is more complex. Our results imply that this second effect is related to change of reaction pathways of α-pinene in the presence of GDI exhaust. Overall, the presence of vehicle exhaust caused more than 50 % suppression in α-pinene SOA mass yield compared to the α-pinene SOA mass yield measured in the absence of GDI emissions.
We present for the first time dual effect of GDI vehicle exhaust on α-pinene SOA mass yield...
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