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Discussion papers
https://doi.org/10.5194/acp-2019-388
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-388
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 02 May 2019

Submitted as: research article | 02 May 2019

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

Chemical Composition and Hydrolysis of Organic Nitrate Aerosol Formed from Hydroxyl and Nitrate Radical Oxidation of α-pinene and β-pinene

Masayuki Takeuchi1 and Nga L. Ng2,3 Masayuki Takeuchi and Nga L. Ng
  • 1School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia, 30332, USA
  • 2School of Chemical and Bimolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, 30332, USA
  • 3School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, 30332, USA

Abstract. Atmospheric organic nitrate (ON) is thought to play a crucial role in the formation potential of ozone and aerosol, which are the leading air pollutants of concern across the world. Limited fundamental knowledge and understanding of the life cycles of ON currently hinders the ability to quantitatively assess its impacts on the formation of these pollutants. Although hydrolysis is currently considered as an important loss mechanism of ON based on prior field measurement studies, this process for atmospherically relevant ON has not been well constrained by fundamental laboratory studies. In this comprehensive study, we investigated the chemical composition and hydrolysis process of particulate ON (pON) formed from the oxidation of α-pinene and β-pinene by hydroxyl and nitrate radicals. For pON that undergoes hydrolysis, the hydrolysis lifetime is determined to be no more than 30 min for all systems explored. This is significantly shorter than those reported in previous chamber studies (i.e., 3–6 h) but is consistent with the reported lifetime from bulk solution measurement studies (i.e., 0.02–8.8 h). The discrepancy appears to stem from the choice of proxy used to estimate the hydrolysis lifetime. The measured hydrolyzable fractions of pON (FH) in the α-pinene+OH, β-pinene+OH, α-pinene+NO3, and β-pinene+NO3 systems are 23–32, 27–34, 9–17, and 9–15 %, respectively. While a very low FH for the nitrate radical oxidation system is expected based on prior studies, FH for the hydroxyl radical oxidation system is surprisingly lower than predicted in past studies. Overall, the hydrolysis lifetime as well as FH obtained in this study serve as experimentally constrained parameters that are required in regional and global chemical transport models to accurately evaluate the impacts of ON on nitrogen budget and formation of ozone and aerosol.

Masayuki Takeuchi and Nga L. Ng
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Masayuki Takeuchi and Nga L. Ng
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Short summary
Organic nitrate is ubiquitous in the atmosphere and impacts the formation of aerosol and ozone, two leading air pollutants of concern worldwide. We conducted a comprehensive laboratory study to investigate the hydrolysis process of organic nitrate aerosol formed from monoterpenes, which are important reactive chemicals emitted by plants. Our results provide experimentally constrained parameters required to assess the role of organic nitrate in the formation of the air pollutants of our concern.
Organic nitrate is ubiquitous in the atmosphere and impacts the formation of aerosol and ozone,...
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