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Highly oxygenated organic molecules with high unsaturation formed upon photochemical aging of soot

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Andreae,  Meinrat O.
Multiphase Chemistry, Max Planck Institute for Chemistry, Max Planck Society;

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Pöschl,  Ulrich
Multiphase Chemistry, Max Planck Institute for Chemistry, Max Planck Society;

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Su,  Hang
Multiphase Chemistry, Max Planck Institute for Chemistry, Max Planck Society;

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Cheng,  Yafang
Multiphase Chemistry, Max Planck Institute for Chemistry, Max Planck Society;

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Citation

Li, M., Li, J., Zhu, Y., Chen, J., Andreae, M. O., Pöschl, U., et al. (2022). Highly oxygenated organic molecules with high unsaturation formed upon photochemical aging of soot. Chem, 8. doi:10.1016/j.chempr.2022.06.011.


Cite as: https://hdl.handle.net/21.11116/0000-000A-CF50-3
Abstract
Highly oxygenated organic molecules are a key component of atmospheric secondary organic aerosol. The origin and formation mechanism of highly oxygenated organic molecules with high unsaturation (HU-HOMs) commonly observed in the atmosphere, however, remain unknown. Through molecular-level investigations of the photochemical aging of soot by O2 in the air, we find that the multigenerational photo-oxidation of large polycyclic aromatic hydrocarbons (PAHs) on soot by singlet oxygen (1O2) and superoxide anion radicals (O2⋅−) can be an important source of the unexplained HU-HOMs. The PAH-derived HU-HOMs exhibit lactone and anhydride functional groups and can substantially increase the hydrophilicity of soot. As PAHs are a characteristic and ubiquitous component of combustion aerosols, their photochemical oxidation can generate substantial amounts of HU-HOMs, influencing the atmospheric fate and effects of combustion aerosols.