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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  17 Sep 2020

17 Sep 2020

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This preprint is currently under review for the journal ACP.

Temperature and acidity dependence of secondary organic aerosol formation from α-pinene ozonolysis with a compact chamber system

Yange Deng, Satoshi Inomata, Kei Sato, Sathiyamurthi Ramasamy, Yu Morino, Shinichi Enami, and Hiroshi Tanimoto Yange Deng et al.
  • National Institute for Environmental Studies, Tsukuba 305-8506, Japan

Abstract. Secondary organic aerosol (SOA) is of great importance, affecting human health and the prediction of climate change; however, the factors (e.g., temperature, acidity of pre-existing particles, and oxidants) influencing its formation are not sufficiently resolved. In this study, a compact Teflon atmospheric simulation chamber is developed, in which reactions in atmospheric pressure conditions can be performed with controlled temperature, humidity, oxidation agents, and seed particle acidity. Using the chamber, α-pinene ozonolysis SOA formation was simulated under temperatures of 278 K, 288 K, and 298 K with neutral/acidic seed aerosols. The SOA components of m / z less than 400 were analyzed using negative electrospray ionization liquid-chromatography time-of-flight mass spectrometry. The temperature and acidity dependence of SOA yields and chemical components were investigated. From the slightly negative temperature dependence of the SOA yields, the enthalpy of vaporization in neutral and acidic seed conditions was estimated to be 25 and 44 kJ mol−1, respectively. With these values, the volatility distributions of the identified SOA compounds were consistently explained. Acidity dependence analysis of the chemical formula, molecular mass, and O : C ratio of the detected compounds indicated the enhanced formation of many oligomers in the wide molecular mass range with a wide range of O : C ratios under acidic seed conditions. The acidity dependence of certain major compounds could be explained by acid-catalyzed heterogeneous reactions (e.g., m / z 171, 185, 343, and 357) or acid-catalyzed decomposition of hydroperoxides (e.g., m / z 215 and 197). In addition, the formation of organosulfates (OS) was observed under acidic seed conditions. We proposed that six of the eleven detected OS were possibly formed through the aldehyde + HSO4 pathway. Further studies on the OS formation during α-pinene ozonolysis are warranted.

Yange Deng et al.

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Yange Deng et al.


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Short summary
The temperature and acidity dependence of yields and chemical compositions of the α-pinene ozonolysis SOA were systematically investigated using a newly developed compact chamber system. Increases of SOA yields were observed with the decrease of temperature and under acidic seed conditions. The differences in chemical compositions between acidic and neutral seed conditions were characterized and explained from the viewpoints of acid-catalyzed reactions. Some organosulfates were newly detected.
The temperature and acidity dependence of yields and chemical compositions of the α-pinene...