Droplet surface spontaneous oxidation as a dominant formation pathway of organosulfates in the marine atmosphere

Lin Du (), Yaru Song, Jianlong Li, Yibei Wan, Huan Yu, Xueqi Ma, Zhaomin Yang, Jie Hu, Kuanyun Hu, Xuxu Gao, Qinyi Li, Christian George, Maofa Ge and Kun Li ()
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Lin Du: Shandong University, Qingdao Key Laboratory for Prevention and Control of Atmospheric Pollution in Coastal Cities, School of Environmental Science and Engineering
Yaru Song: Shandong University, Qingdao Key Laboratory for Prevention and Control of Atmospheric Pollution in Coastal Cities, School of Environmental Science and Engineering
Jianlong Li: Shandong University, Environment Research Institute
Yibei Wan: China University of Geosciences, Department of Atmospheric Science, School of Environmental Studies
Huan Yu: China University of Geosciences, Department of Atmospheric Science, School of Environmental Studies
Xueqi Ma: Shandong University, Environment Research Institute
Zhaomin Yang: Shandong University, Environment Research Institute
Jie Hu: Shandong University, Environment Research Institute
Kuanyun Hu: Shandong University, Environment Research Institute
Xuxu Gao: Shandong University, Institute of Marine Science and Technology
Qinyi Li: Shandong University, Environment Research Institute
Christian George: Shandong University, Qingdao Key Laboratory for Prevention and Control of Atmospheric Pollution in Coastal Cities, School of Environmental Science and Engineering
Maofa Ge: Chinese Academy of Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry
Kun Li: Shandong University, Environment Research Institute

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Organosulfates (OSs) have been widely detected in marine aerosols and have various potential formation pathways in the atmosphere. However, the key formation mechanism of OSs in the marine environment remains unclear. Here, by combining field measurements, laboratory experiments, and model calculations, we suggest that the surface spontaneous oxidation of sea spray aerosol (SSA) particles produces OSs rapidly and is the dominant formation pathway of OSs in the marine atmosphere. SSA microdroplets provide a large surface area for the spontaneous formation of OH radicals, inducing the oxidization of dimethyl sulfide into sulfate (SO42–), sulfuric acid, and organic acids, thereby acidifying the droplets. Subsequently, SO42– reacts with dissolved alcohols under such acidic conditions to produce OSs. This process is fast enough to be a major source of detected OSs in the aerosol samples collected in the marine atmosphere. This pathway contributes to a global OS production of 13.96 ± 10.99 Tg yr–1, comparable to global isoprene-derived OS production. This study reveals that rapid secondary processes are the main source of OSs in the marine atmosphere and highlights the important role of the droplet surface spontaneous oxidation process in atmospheric chemistry over the ocean.

Date: 2025
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DOI: 10.1038/s41467-025-65008-3

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