22 Apr 2022
22 Apr 2022
Status: a revised version of this preprint was accepted for the journal ACP.

Significant formation of sulfate aerosols contributed by the heterogeneous drivers of dust surface

Tao Wang1, Yangyang Liu1, Hanyun Cheng1, Zhenzhen Wang1, Hongbo Fu1, Jianmin Chen1, and Liwu Zhang1,2 Tao Wang et al.
  • 1Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, National Observations and Research Station for Wetland Ecosystems of the Yangtze Estuary, IRDR international Center of Excellence on Risk Interconnectivity and Governance on Weather, Department of Environmental Science & Engineering, Fudan University, Shanghai, 200433, Peoples’ Republic of China
  • 2Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, Peoples’ Republic of China

Abstract. The importance of dust heterogeneous chemistry in the removal of atmospheric SO2 and formation of sulfate aerosols is not adequately understood. In this study, the Fe, Ti, Al-bearing components, Na+, Cl-, K+, and Ca2+ of the dust surface were discovered to be closely associated with the heterogeneous formation of sulfate. Regression models were then developed to accurately predict the heterogeneous reactivity by the particle chemical compositions. Further, the recognized gas-phase, aqueous-phase and heterogeneous oxidation routes were quantitatively assessed and kinetically compared by combining the laboratory work with modeling study. In the presence of 55 μg m-3 airborne dust, heterogeneous chemistry accounts for approximately 28.6 % of the secondary sulfate aerosols during nighttime, while the proportion decreases to 13.1 % in the presence of solar irradiation. On the dust surface, heterogeneous drivers (e.g. transition metal constituents, water-soluble ions) are more efficient than surface adsorbed oxidants (e.g. H2O2, NO2, O3) in the conversion of SO2, particularly during nighttime. Dust heterogeneous chemistry offers an opportunity to explain the missing sulfate source during severe haze pollution events, and its contribution proportion in the complex atmospheric environments could be even higher than the current calculation results. Overall, the dust surface drivers are responsible for the significant formation of sulfate aerosols and have profound impacts on the atmospheric sulfur cycling.

Tao Wang et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2022-227', Anonymous Referee #2, 04 May 2022
    • AC1: 'Reply on RC1', Liwu Zhang, 06 Jul 2022
  • RC2: 'Comment on acp-2022-227', Anonymous Referee #3, 13 Jun 2022
    • AC2: 'Reply on RC2', Liwu Zhang, 06 Jul 2022

Tao Wang et al.


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Short summary
This study compared the gas-phase, aqueous-phase and heterogeneous SO2 oxidation pathways by combining laboratory work with modeling study. The heterogeneous chemistry, particularly that induced by the dust surface drivers, presents positive implications for the removal of airborne SO2 and formation of sulfate aerosols. This work highlighted the atmospheric significance of dust-driven chemistry and suggested a comparison model to evaluate the following heterogeneous laboratory research.