Preprints
https://doi.org/10.5194/egusphere-2022-1068
https://doi.org/10.5194/egusphere-2022-1068
 
26 Oct 2022
26 Oct 2022
Status: this preprint is open for discussion.

SO2 enhances aerosol formation from anthropogenic volatile organic compound ozonolysis by producing sulfur-containing compounds

Zhaomin Yang1, Kun Li1, Narcisse T. Tsona1, Xin Luo2, and Lin Du1 Zhaomin Yang et al.
  • 1Environment Research Institute, Shandong University, Qingdao, 266237, China
  • 2Technology Center of Qingdao Customs, Qingdao, 266003, China

Abstract. Sulfur dioxide (SO2) can affect aerosol formation in the atmosphere, but the underlying mechanisms remain unclear. Here, we investigate aerosol formation and composition from the ozonolysis of cyclooctene with and without SO2 addition in a smog chamber. Liquid chromatography equipped with high-resolution tandem mass spectrometry measurements indicate that monomer carboxylic acids and corresponding dimers with acid anhydride and aldol structures are important components in particles formed in the absence of SO2. A 9.4–12.6 time increase in particle maximum number concentration is observed in the presence of 14–192 ppb SO2. This increase is largely attributed to sulfuric acid (H2SO4) formation from the reactions of stabilized Criegee intermediates with SO2. In addition, a number of organosulfates (OSs) are detected in the presence of SO2, which are likely products formed from the heterogeneous reactions of oxygenated species with H2SO4. The molecular structures of OSs are also identified based on tandem mass spectrometry analysis. It should be noted that some of these OSs have been found in previous field studies but were classified as compounds from unknown sources or of unknown structures. The observed OSs are less volatile than their precursors and therefore are more effective contributors to particle formation and growth, partially leading to the increase in particle volume concentration under SO2-presence conditions. Our results provide an in-depth molecular-level insight into how SO2 alters particle formation and composition.

Zhaomin Yang et al.

Status: open (until 07 Dec 2022)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2022-1068', Anonymous Referee #1, 31 Oct 2022 reply
  • RC2: 'Review of egusphere-2022-1068', Anonymous Referee #2, 22 Nov 2022 reply

Zhaomin Yang et al.

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Short summary
SO2 significantly promotes particle formation during cyclooctene ozonolysis. Carboxylic acids and their dimers were major products in particles formed in the absence of SO2. SO2 can induce the production of organosulfates with stronger particle formation ability than their precursors, leading to the enhancement in particle formation. Formation mechanisms and structures of organosulfates were proposed, which is helpful for better understanding how SO2 perturbs the formation and fate of particles.