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Biogenic and Anthropogenic Contributions to Atmospheric Organosulfates in a Typical Megacity in Eastern China.

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Title: Biogenic and Anthropogenic Contributions to Atmospheric Organosulfates in a Typical Megacity in Eastern China.
Authors: Huang, Liubin1,2 (AUTHOR), Wang, Yao1,3 (AUTHOR), Zhao, Yue1 (AUTHOR) yuezhao20@sjtu.edu.cn, Hu, Huilin1 (AUTHOR), Yang, Yu2 (AUTHOR), Wang, Yuchen4 (AUTHOR), Yu, Jian‐Zhen4,5 (AUTHOR), Chen, Tianshu2 (AUTHOR), Cheng, Zhen1 (AUTHOR), Li, Chenxi1 (AUTHOR), Li, Ziyue1 (AUTHOR), Xiao, Huayun1 (AUTHOR)
Source: Journal of Geophysical Research. Atmospheres. Sep2023, Vol. 128 Issue 17, p1-17. 17p.
Subject Terms: *Atmospheric aerosols, *Particulate matter, Megalopolis, Monoterpenes, Liquid chromatography-mass spectrometry, Atmospheric oxygen, Matrix decomposition
Geographic Terms: Shanghai (China), China
Abstract: Organosulfates (OSs) are important components of secondary organic aerosols (SOA) in the atmosphere. Despite the frequent observation of OSs in field and laboratory studies, the sources and detailed formation pathways of these species, particularly in polluted regions, are still not well understood. In this study, a total of 156 ambient PM2.5 filter samples were collected in a Chinese megacity (Shanghai) over four seasons in both 2015–2016 and 2018–2019. More than 270 OS formulas were detected in ambient aerosols using high‐resolution liquid chromatography‐mass spectrometry. Interestingly, a series of alkyl OSs, CnH2n+1O4S− (C5–C11), were observed, which are most likely to be produced from the heterogeneous reactions of organic peroxides with sulfur dioxide or sulfate. The observation of these compounds provides the first field evidence for atmospheric OS formation involving organic peroxides. By employing a positive matrix factorization model, the possible precursors of OSs were classified into six groups, that is, isoprene‐derived, monoterpene‐derived, aromatic, short‐chain aliphatic, long‐chain aliphatic, and anthropogenic C2/C3 OSs. Biogenic (isoprene and monoterpenes) and anthropogenic sources (the remaining factors) contributed to 57.2% and 42.8% of OS formation in 2015–2016, respectively, and their contributions just slightly changed in 2018–2019. In addition, the OS sources exhibited strong seasonality. Isoprene‐derived OSs contributed to the largest fraction of total OSs in summer, while anthropogenic sources dominated OS formation in other seasons. Our findings provide valuable insight into OS sources and formation mechanisms in the atmosphere and highlight the importance of both biogenic and anthropogenic emissions for the formation of OSs in a typical Chinese megacity. Plain Language Summary: Secondary organic aerosols (SOA) constitute a major fraction of ambient fine particle matter (PM2.5) and play a significant role in the atmospheric physicochemical processes as well as in determining the climate and health impacts of aerosols. As important tracers of SOA, the chemical behaviors of organosulfates (OSs) have become of great interest to the atmospheric community. In this study, two field campaigns (across four different seasons in both 2015–2016 and 2018–2019) were conducted to explore the sources and formation mechanisms of OSs in atmospheric aerosols in Shanghai, China. A group of alkyl OSs, CnH2n+1O4S− (C5–C11) were observed and inferred to be formed from the heterogeneous reactions of organic peroxides with sulfur dioxide or sulfate, which provides first field observational evidence for the organic peroxide‐involved OS formation mechanism proposed in laboratory studies. Source apportionment with a positive matrix factorization model identified two biogenic and four anthropogenic OS sources, which contributed to 57% and 43% of the total OSs, respectively. Our findings contribute to an improved understanding of the OS formation mechanism in the atmosphere and highlight the importance of both biogenic and anthropogenic emissions for OS formation in a typical Chinese megacity. Key Points: Field evidence for OS formation involving organic peroxides is providedTwo biogenic and four anthropogenic OS sources were identified, which exhibited pronounced seasonal and interannual variabilityBoth anthropogenic and biogenic emissions contributed significantly to OS formation in Shanghai [ABSTRACT FROM AUTHOR]
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Description
Abstract:Organosulfates (OSs) are important components of secondary organic aerosols (SOA) in the atmosphere. Despite the frequent observation of OSs in field and laboratory studies, the sources and detailed formation pathways of these species, particularly in polluted regions, are still not well understood. In this study, a total of 156 ambient PM2.5 filter samples were collected in a Chinese megacity (Shanghai) over four seasons in both 2015–2016 and 2018–2019. More than 270 OS formulas were detected in ambient aerosols using high‐resolution liquid chromatography‐mass spectrometry. Interestingly, a series of alkyl OSs, CnH2n+1O4S− (C5–C11), were observed, which are most likely to be produced from the heterogeneous reactions of organic peroxides with sulfur dioxide or sulfate. The observation of these compounds provides the first field evidence for atmospheric OS formation involving organic peroxides. By employing a positive matrix factorization model, the possible precursors of OSs were classified into six groups, that is, isoprene‐derived, monoterpene‐derived, aromatic, short‐chain aliphatic, long‐chain aliphatic, and anthropogenic C2/C3 OSs. Biogenic (isoprene and monoterpenes) and anthropogenic sources (the remaining factors) contributed to 57.2% and 42.8% of OS formation in 2015–2016, respectively, and their contributions just slightly changed in 2018–2019. In addition, the OS sources exhibited strong seasonality. Isoprene‐derived OSs contributed to the largest fraction of total OSs in summer, while anthropogenic sources dominated OS formation in other seasons. Our findings provide valuable insight into OS sources and formation mechanisms in the atmosphere and highlight the importance of both biogenic and anthropogenic emissions for the formation of OSs in a typical Chinese megacity. Plain Language Summary: Secondary organic aerosols (SOA) constitute a major fraction of ambient fine particle matter (PM2.5) and play a significant role in the atmospheric physicochemical processes as well as in determining the climate and health impacts of aerosols. As important tracers of SOA, the chemical behaviors of organosulfates (OSs) have become of great interest to the atmospheric community. In this study, two field campaigns (across four different seasons in both 2015–2016 and 2018–2019) were conducted to explore the sources and formation mechanisms of OSs in atmospheric aerosols in Shanghai, China. A group of alkyl OSs, CnH2n+1O4S− (C5–C11) were observed and inferred to be formed from the heterogeneous reactions of organic peroxides with sulfur dioxide or sulfate, which provides first field observational evidence for the organic peroxide‐involved OS formation mechanism proposed in laboratory studies. Source apportionment with a positive matrix factorization model identified two biogenic and four anthropogenic OS sources, which contributed to 57% and 43% of the total OSs, respectively. Our findings contribute to an improved understanding of the OS formation mechanism in the atmosphere and highlight the importance of both biogenic and anthropogenic emissions for OS formation in a typical Chinese megacity. Key Points: Field evidence for OS formation involving organic peroxides is providedTwo biogenic and four anthropogenic OS sources were identified, which exhibited pronounced seasonal and interannual variabilityBoth anthropogenic and biogenic emissions contributed significantly to OS formation in Shanghai [ABSTRACT FROM AUTHOR]
ISSN:2169897X
DOI:10.1029/2023JD038848