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Discussion papers
https://doi.org/10.5194/acp-2019-807
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-807
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 07 Oct 2019

Submitted as: research article | 07 Oct 2019

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

Formation of highly oxygenated organic molecules from chlorine atom initiated oxidation of alpha-pinene

Yonghong Wang1, Matthieu Riva1,2, Hongbin Xie3,1, Liine Heikkinen1, Simon Schallhart1, Qiaozhi Zha1, Chao Yan1, Xucheng He1, Otso Peräkylä1, and Mikael Ehn1 Yonghong Wang et al.
  • 1Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, P.O. Box 64, 00014 University of Helsinki, Helsinki, Finland
  • 2Univ Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON, F-69626, Villeurbanne, France
  • 3Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China

Abstract. Highly oxygenated organic molecules (HOMs) from atmospheric oxidation of alpha-pinene can irreversibly condense to particles and contribute to secondary organic aerosol (SOA) formation. Recently, the formation of nitryl chloride (ClNO2) from heterogeneous reactions, followed by its subsequent photolysis is suggested to be an important source of chlorine atoms in many parts of the atmosphere. However, the oxidation of monoterpenes such as alpha-pinene by chlorine atoms has received very little attention, and the ability of this reaction to form HOM is completely unstudied. Here, chamber experiments were conducted with alpha-pinene and chlorine under low and high nitrogen oxide (NOx) conditions. A NO3-based CI-APi-TOF was used to measure HOM products. Clear distributions of monomers with 9–10 carbon atoms and dimers with 18–20 carbon atoms were observed under low NOx conditions. With increased concentration of NOx within the chamber, the formation of dimers was suppressed due to the reactions of peroxy radicals with NO. We estimated the HOM yields from chlorine-initiated oxidation of alpha-pinene under low-NOx conditions to be around 1.8 %, though with a substantial uncertainty range (0.8–4 %) due to lack of suitable calibration methods. Corresponding yields at high NOx could not be determined because of concurrent ozonolysis reactions. Our study demonstrates that chlorine atoms also initiated oxidation of alpha-pinene and yields low volatility organic compounds.

Yonghong Wang et al.
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Short summary
Chamber experiments were conducted with alpha-pinene and chlorine under low and high nitrogen oxide (NOx) conditions.We estimated the HOM yields from chlorine-initiated oxidation of alpha-pinene under low-NOX conditions to be around 1.8 %, though with a uncertainty range (0.8–4 %) due to lack of suitable calibration methods. Our study clearly demonstrates that the chlorine atom initiated oxidation of alpha-pinene can produce low volatility organic compounds.
Chamber experiments were conducted with alpha-pinene and chlorine under low and high nitrogen...
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