Preprints
https://doi.org/10.5194/egusphere-2023-1649
https://doi.org/10.5194/egusphere-2023-1649
09 Aug 2023
 | 09 Aug 2023

Organosulfate Produced from Consumption of SO3 Speeds up Sulfuric Acid-Dimethylamine Atmospheric Nucleation

Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin

Abstract. Although sulfuric acid (SA) and dimethylamine (DMA) driven nucleation mainly dominants the new particle formation (NPF) process in the atmosphere, seeking the involvement of other gaseous species remains crucial to better understand the NPF. Organosulfate has been detected in gas phase and abundantly in atmospheric fine particles. However, its molecular formation mechanism and its impact on the NPF are still much less understood. Here, we explored the gas phase reaction of Glycolic acid (GA) with SO3, and evaluated the enhancing potential of its products on the SA-DMA driven NPF using a combination of quantum chemical calculations and kinetics modeling. We found that the considerable concentration of glycolic acid sulfate (GAS) is thermodynamically accessible from the reaction of GA with SO3, efficiently catalyzed by SA or H2O molecules. The produced GAS can form stable clusters with SA and DMA, and speeds up the nucleation rate of SA-DMA system obviously. Notably, the enhancement by GAS on the SA-DMA-based particle formation rate can be up to ~ 800 times in the region where the concentration of SA is about 104 molecules cm-3. Supported by observations of atmospheric NPF events at Mt. Tai in China, our proposed ternary GAS-SA-DMA nucleation mechanism further indicates that the organosulfates produced from the consumption of SO3 may play an important role for the unexpected high NPF rates observed in areas with relatively low concentrations of SA. The presented reaction and nucleation mechanisms provide a new feasible source of organosulfates in atmospheric new particles. Based on our findings, the impact of organosulfates on the atmospheric NPF in multiple regions around the world was estimated and discussed.

Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-1649', Anonymous Referee #1, 14 Aug 2023
    • AC1: 'Reply on RC1', Shi Yin, 18 Sep 2023
  • RC2: 'Comment on egusphere-2023-1649', Anonymous Referee #2, 14 Sep 2023

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-1649', Anonymous Referee #1, 14 Aug 2023
    • AC1: 'Reply on RC1', Shi Yin, 18 Sep 2023
  • RC2: 'Comment on egusphere-2023-1649', Anonymous Referee #2, 14 Sep 2023
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin

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Short summary
Atmospheric new particle formation (NPF) has a significant influence on global climate, local air quality, and human health. Using a combination of quantum chemical calculations and kinetics modeling, we found gas phase organosulfate produced from consumption of SO3 can significantly enhance SA-DMA nucleation in the polluted boundary layer, resulting in nonnegligible contribution to NPF. Our findings provide important insights on effect of organic sulfur on atmospheric aerosol formation.