Preprints
https://doi.org/10.5194/acp-2021-1069
https://doi.org/10.5194/acp-2021-1069

  10 Jan 2022

10 Jan 2022

Review status: this preprint is currently under review for the journal ACP.

Molecular Characteristics of Organosulfur Compounds in Guangzhou, South China: Heterogeneous Secondary Reactions Drivers the Molecular Distribution

Hongxing Jiang1,2,3,6, Jun Li1,3, Jiao Tang1,3, Min Cui4, Shizhen Zhao1,3, Yangzhi Mo1,3, Chongguo Tian5, Xiangyun Zhang1,3, Bin Jiang1,3, Yuhong Liao1,3, Yinjun Chen2, and Gan Zhang1,3 Hongxing Jiang et al.
  • 1State Key Laboratory of Organic Geochemistry and Guangdong province Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou, 510640, China
  • 2Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, Shanghai 200433, China
  • 3CAS Center for Excellence in Deep Earth Science, Guangzhou, 510640, China
  • 4College of Environmental Science and Engineering, Yangzhou university, 225009, Yangzhou, China
  • 5Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai, 264003, China
  • 6University of Chinese Academy of Sciences, Beijing, 100049, China

Abstract. Organosulfur compounds (OrgSs), especially organosulfates, have been widely reported at large quantities in particulate organic matter found in various atmospheric environments. Despite various kinds of organosulfates and their formation mechanisms being previously identified, a large fraction of OrgSs remain unexplained at the molecular level, impeding further knowledge on additional formation pathways and critical environmental parameters that help to explain their concentrations. In this work, the abundance and molecular composition of OrgSs in fine particulate samples collected in Guangzhou was reported. Our results revealed that organic sulfur can averagely contribute to 30 % of total particulate sulfur, and showed positively correlations with the SO2 (r = 0.37, p < 0.05) and oxidants (NOx+O3, r = 0.40, p < 0.01). Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) results presented that more than 80 % by number of the detected OrgSs in our samples have the elemental composition of O/(4S+3N)  ≥ 1, indicating that they were largely in the form of oxidized organosulfates and/or nitrooxy organosulfates. Many OrgSs, which are tentatively attributed to previously identified biogenic and anthropogenic origins, were also present in aerosols derived from freshly-emitted combustion sources. Results show that the formation of OrgSs through an epoxide intermediate pathway could be as much as 46 %, and the oxidants levels could explain 20 % variation of organic sulfur mass. The analysis from our large FT-ICR MS dataset suggests that relative humidity, oxidation of biogenic volatile organic compounds via ozonolysis, and NOx-related nitrooxy organosulfate formations were the major reasons for the molecular variation of OrgSs, possibly highlighting the importance of heterogeneous reactions involving either the uptake of SO2 or the heterogeneous oxidations of particulate organosulfates into additional unrecognized OrgSs.

Hongxing Jiang et al.

Status: open (until 21 Feb 2022)

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Hongxing Jiang et al.

Hongxing Jiang et al.

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Short summary
We conducted field observation employing Fourier transform ion cyclotron resonance mass spectrometry to characterize the molecular composition and major formation pathways or sources of organosulfur compounds in Guangzhou, where is heavily influenced by biogenic−anthropogenic interactions and has high relative humidity and temperature. We suggested that heterogeneous reactions such as SO2 uptake and heterogeneous oxidations are important to the molecular variations of organosulfur compounds.
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