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Triplet-state organic matter in atmospheric aerosols: Formation characteristics and potential effects on aerosol aging
https://orcid.org/0000-0001-8208-0558
Abstract Triplet-state organic matter could be generated by chromophoric organic aerosols under light exposure, which furtherly induce aerosol aging. The characteristics of triplet-state generation have not been fully investigated to date in organic aerosols. Here, we conduct a comprehensive investigation of the generation characteristics of triplet-state chromophoric dissolved organic matter (3CDOM*) in primary, secondary and ambient aerosols. The results show that biomass combustion have the strongest capacity of 3CDOM* generation, while vehicle emissions are the weakest. In ambient aerosol, there is a stronger ability to generate 3CDOM* in winter than in summer. The various types of CDOM are identified by the EEM-PARAFAC method, and the structure-activity relationship between the type of CDOM and the capacity of 3CDOM* generation is investigated. The results show that two types of CDOM, which are usually identified as N-containing substances, contributed 88% to triplet-state generation. According to the spin trapping and electron paramagnetic resonance technique, we estimate that 3CDOM* induce at least 30% of the singlet oxygen (1O2) and 31% of the hydroxyl radical (•OH) in aerosols. The estimated generation rate of 3CDOM* reached ~100 μmol m−3 h−1 in the atmosphere in Xi'an, China, which is approximately one hundred thousand times that of •OH. These results indicate that 3CDOM* is likely a significant contributor to aerosol aging in the actual atmosphere.
Graphical abstract Display Omitted
Highlights Biomass combustion has the strongest triplet state generation capacity. The main precursors to formation of triplet states in aerosols was identified. Triplet state involved reactions have contributed to the aerosol photochemistry. The triplet state drives a third of 1O2 and .•OH in aerosol photochemical reactions.
Triplet-state organic matter in atmospheric aerosols: Formation characteristics and potential effects on aerosol aging
https://orcid.org/0000-0001-8208-0558
Abstract Triplet-state organic matter could be generated by chromophoric organic aerosols under light exposure, which furtherly induce aerosol aging. The characteristics of triplet-state generation have not been fully investigated to date in organic aerosols. Here, we conduct a comprehensive investigation of the generation characteristics of triplet-state chromophoric dissolved organic matter (3CDOM*) in primary, secondary and ambient aerosols. The results show that biomass combustion have the strongest capacity of 3CDOM* generation, while vehicle emissions are the weakest. In ambient aerosol, there is a stronger ability to generate 3CDOM* in winter than in summer. The various types of CDOM are identified by the EEM-PARAFAC method, and the structure-activity relationship between the type of CDOM and the capacity of 3CDOM* generation is investigated. The results show that two types of CDOM, which are usually identified as N-containing substances, contributed 88% to triplet-state generation. According to the spin trapping and electron paramagnetic resonance technique, we estimate that 3CDOM* induce at least 30% of the singlet oxygen (1O2) and 31% of the hydroxyl radical (•OH) in aerosols. The estimated generation rate of 3CDOM* reached ~100 μmol m−3 h−1 in the atmosphere in Xi'an, China, which is approximately one hundred thousand times that of •OH. These results indicate that 3CDOM* is likely a significant contributor to aerosol aging in the actual atmosphere.
Graphical abstract Display Omitted
Highlights Biomass combustion has the strongest triplet state generation capacity. The main precursors to formation of triplet states in aerosols was identified. Triplet state involved reactions have contributed to the aerosol photochemistry. The triplet state drives a third of 1O2 and .•OH in aerosol photochemical reactions.
Triplet-state organic matter in atmospheric aerosols: Formation characteristics and potential effects on aerosol aging
https://orcid.org/0000-0001-8208-0558
Abstract Triplet-state organic matter could be generated by chromophoric organic aerosols under light exposure, which furtherly induce aerosol aging. The characteristics of triplet-state generation have not been fully investigated to date in organic aerosols. Here, we conduct a comprehensive investigation of the generation characteristics of triplet-state chromophoric dissolved organic matter (3CDOM*) in primary, secondary and ambient aerosols. The results show that biomass combustion have the strongest capacity of 3CDOM* generation, while vehicle emissions are the weakest. In ambient aerosol, there is a stronger ability to generate 3CDOM* in winter than in summer. The various types of CDOM are identified by the EEM-PARAFAC method, and the structure-activity relationship between the type of CDOM and the capacity of 3CDOM* generation is investigated. The results show that two types of CDOM, which are usually identified as N-containing substances, contributed 88% to triplet-state generation. According to the spin trapping and electron paramagnetic resonance technique, we estimate that 3CDOM* induce at least 30% of the singlet oxygen (1O2) and 31% of the hydroxyl radical (•OH) in aerosols. The estimated generation rate of 3CDOM* reached ~100 μmol m−3 h−1 in the atmosphere in Xi'an, China, which is approximately one hundred thousand times that of •OH. These results indicate that 3CDOM* is likely a significant contributor to aerosol aging in the actual atmosphere.
Graphical abstract Display Omitted
Highlights Biomass combustion has the strongest triplet state generation capacity. The main precursors to formation of triplet states in aerosols was identified. Triplet state involved reactions have contributed to the aerosol photochemistry. The triplet state drives a third of 1O2 and .•OH in aerosol photochemical reactions.
Triplet-state organic matter in atmospheric aerosols: Formation characteristics and potential effects on aerosol aging
Chen, Qingcai (author) / Mu, Zhen (author) / Xu, Li (author) / Wang, Mamin (author) / Wang, Jin (author) / Shan, Ming (author) / Fan, Xingjun (author) / Song, Jianzhong (author) / Wang, Yuqin (author) / Lin, Pengchuan (author)
Atmospheric Environment ; 252
2021-03-09
Article (Journal)
Electronic Resource
English