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https://doi.org/10.5194/acp-2017-433
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-2017-433
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

  15 Jun 2017

15 Jun 2017

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This preprint was under review for the journal ACP but the revision was not accepted.

Influence of NO2 on secondary organic aerosol formation from ozonolysis of limonene

Changjin Hu1,*, Qiao Ma1,2,*, Zhi Liu1, Yue Cheng1, Liqing Hao3, Nana Wei1, Yanbo Gai1, Xiaoxiao Lin1, Xuejun Gu1, Weixiong Zhao1, Mingqiang Huang1,4, Zhenya Wang1, and Weijun Zhang1,2,5 Changjin Hu et al.
  • 1Laboratory of Atmospheric Physico-Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, Anhui, China
  • 2University of Science and Technology of China, Hefei 230026, Anhui, China
  • 3Department of Applied Physics, University of Eastern Finland, Kuopio 70211, Finland
  • 4College of Chemistry & Environment, Minnan Normal University, Zhangzhou 363000, P. R. China
  • 5School of Environmental Science and Optoelectronic Technology, University of Science and Technology of China, Hefei 230026, Anhui, China
  • *These authors contributed equally to this work.

Abstract. Limonene has a strong tendency to undergo ozonolysis to form semi-volatile and low-volatility compounds that contribute to secondary organic aerosols (SOAs) both outdoors and indoors. The influence of NO2 on SOA formation from ozonolysis of limonene has been evaluated using chamber experiments and the Master Chemical Mechanism (MCM) coupled with a gas-particle partitioning model in this work. A series of 21 indoor chamber experiments were carried out with or without NO2 under different [O3]0 / [VOC]0 ratios, and these experimental data were compared with the model simulations. Agreement in SOA yields was observed between the experimental observations and model simulations under varying conditions. Generally, SOA mass yields are positively dependent on [O3]0 / [VOC]0 without the presence of NO2. However, the introduction of NO2 leads to a more complicated change in SOA yield, which is shown to be related to initial [O3] / [VOC] ratios. When [O3]0 / [VOC]0 > 2, the introduction of NO2 results in an increase of SOA yield in the range of NO2 studied in this work; whereas a weak negative effect was found for SOA formation according to the introduction of ~ 250 ppbv NO2 under [O3]0 / [VOC]0 < 2 conditions. It was suggested that the effect of NO2 on SOA formation yields from limonene ozonolysis is related to the competition between O3- and NO3-initiated oxidation of limonene as well as the competition between RO2 + HO2 and RO2 + NO2 (or NO3). Analysis of aerosol chemical composition with Fourier-transform infrared spectroscopy (FTIR) and modeling further confirmed that the formation of peroxy acyl nitrates (PANs) and organic nitrates plays an important role in aerosol particle formation from limonene ozonolysis at the presence of NO2. The findings here indicate that accurately constraining SOA yields from NO3 oxidation is essential to evaluate the influence of NO2 on SOA formation in some real atmosphere, for example, regions with both biogenic and anthropogenic influences.

Changjin Hu et al.

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Changjin Hu et al.

Changjin Hu et al.

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Short summary
The effect of NO2 on SOA formation from oxidation of limonene is found to be related to the competition between O3- and NO3-initiated oxidation as well as the competition between RO2 + HO2 and RO2 + NO2 (or NO3) following the initial ozonolysis, and organic nitrates is believed to play an important role in aerosol particle formation. It is suggested that SOA formation in the regions with substantial anthropogenic-biogenic interactions should be evaluated more systematically than before.
The effect of NO2 on SOA formation from oxidation of limonene is found to be related to the...
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