Preprints
https://doi.org/10.5194/acp-2022-636
https://doi.org/10.5194/acp-2022-636
 
13 Sep 2022
13 Sep 2022
Status: this preprint is currently under review for the journal ACP.

Large differences of highly oxygenated organic molecules (HOMs) and low volatile species in SOA formed from ozonolysis of β-pinene and limonene

Dandan Liu1,, Yun Zhang2,3,, Shujun Zhong1, Shuang Chen1, Qiaorong Xie1, Donghuan Zhang1, Qiang Zhang1, Wei Hu1, Junjun Deng1, Libin Wu1, Chao Ma1, Haijie Tong4,5, and Pingqing Fu1 Dandan Liu et al.
  • 1Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
  • 2Innovation Center of Pesticide Research, Department of Applied Chemistry, College of Science, China Agricultural University, Beijing 100193, China
  • 3Institute of Chemistry, Johannes Gutenberg University, Mainz 55128, Germany
  • 4Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz 55128, Germany
  • 5Institute of Surface Science, Helmholtz-Zentrum Hereon, Geesthacht 21502, Germany
  • These authors contributed to this study equally.

Abstract. Secondary organic aerosols (SOA) play a key role in climate change and public health. However, the oxidation state and volatility of SOA are still not well understood. Here, we investigated the highly oxygenated organic molecules (HOMs) in SOA formed from ozonolysis of β-pinene and limonene. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) was used to characterize HOMs, and a scanning mobility particle sizer (SMPS) was used to measure the concentration and size distribution of SOA particles. The abundance of HOMs in limonene SOA was 5–13 % higher than in β-pinene SOA (3–13 %) exhibiting different trends with increasing ozone concentrations. β-pinene oxidation-derived HOMs prefer to stabilize at high ozone concentration, accompanied by substantial formation of ultra-low-volatility organic compounds (ULVOCs). Limonene-oxidation-derived HOMs prefer to stabilize at moderate ozone concentrations, with semi-, low-, and extremely low-volatility organic compounds (SVOCs, LOVCs, and ELVOCs) play a major role. Combined experimental evidence and theoretical analysis indicate that oxygen-increasing-based peroxy radical chemistry is a plausible mechanism for the formation of compounds with 10 carbon atoms. Our findings show that HOMs and low volatile species in β-pinene and limonene SOA are largely different. The ozone concentration-driven SOA formation and evolution mechanism of monoterpenes is suggested to be considered in future climate or exposure risk models, which may enable more accurate air quality prediction and management.

Dandan Liu et al.

Status: open (until 25 Oct 2022)

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  • RC1: 'Comment on acp-2022-636', Anonymous Referee #1, 16 Sep 2022 reply

Dandan Liu et al.

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Short summary
Based on ultra-high resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) prefer to stabilize at high ozone concentration, while limonene oxidation-derived HOMs prefer to stabilize at moderate ozone concentration. The distinct molecular response of HOMs and low volatile species in different biogenic SOA to ozone concentrations provides a new clue for more accurate air quality prediction and management.
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