Increase of High Molecular Weight Organosulfate With Intensifying Urban Air Pollution in the Megacity Beijing

Qiaorong Xie; Ying Li; Siyao Yue; Sihui Su; Dong Cao; Yisheng Xu; Jing Chen; Haijie Tong; Hang Su; Yafang Cheng; Wanyu Zhao; Wei Hu; Zhe Wang; Ting Yang; Xiaole Pan; Yele Sun; Zifa Wang; Cong Qiang Liu; Kimitaka Kawamura; Guibin Jiang; Manabu Shiraiwa; Pingqing Fu

doi:10.1029/2019JD032200

Increase of High Molecular Weight Organosulfate With Intensifying Urban Air Pollution in the Megacity Beijing

Qiaorong Xie, Ying Li, Siyao Yue, Sihui Su, Dong Cao, Yisheng Xu, Jing Chen, Haijie Tong, Hang Su, Yafang Cheng, Wanyu Zhao, Wei Hu, Zhe Wang, Ting Yang, Xiaole Pan, Yele Sun, Zifa Wang, Cong Qiang Liu, Kimitaka Kawamura, Guibin JiangManabu Shiraiwa, Pingqing Fu

Research output: Journal article publication › Journal article › Academic research › peer-review

38 Citations (Scopus)

Abstract

Organosulfates (OSs), a key component of secondary organic aerosols (SOA), account for up to one third of organic matter in the atmosphere. However, high molecular weight (HMW, 500–800 Da) OSs in ambient aerosols are poorly characterized at a molecular level, due to experimental difficulties. With Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICRMS), we are able to identify more than 8,000 OSs in wintertime aerosols in Beijing. We found that both the number and signal magnitudes of HMW OSs with low H/C and O/C ratios and degrees of unsaturation were greatly enhanced during hazy days, indicating that most HMW OSs were freshly formed during stagnant air pollution episodes. They are most likely to be the oxidation products of semivolatility to low-volatility precursors (e.g., polycyclic aromatic hydrocarbons and fatty acids) and have showed a strong influence of anthropogenic emissions. The molecular corridor analysis suggests that the high abundance of HMW aromatic-like and aliphatic OSs considerably decreases the volatility of organic aerosols in the urban atmosphere.

Original language	English
Article number	e2019JD032200
Journal	Journal of Geophysical Research: Atmospheres
Volume	125
Issue number	10
DOIs	https://doi.org/10.1029/2019JD032200
Publication status	Published - 27 May 2020
Externally published	Yes

Keywords

FT-ICR MS
Organic aerosol
Organosulfates
Secondary organic aerosol
Volatile organic compounds

ASJC Scopus subject areas

Geophysics
Forestry
Oceanography
Aquatic Science
Ecology
Water Science and Technology
Soil Science
Geochemistry and Petrology
Earth-Surface Processes
Atmospheric Science
Earth and Planetary Sciences (miscellaneous)
Space and Planetary Science
Palaeontology

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

More information

10.1029/2019JD032200

Cite this

Xie, Q., Li, Y., Yue, S., Su, S., Cao, D., Xu, Y., Chen, J., Tong, H., Su, H., Cheng, Y., Zhao, W., Hu, W., Wang, Z., Yang, T., Pan, X., Sun, Y., Wang, Z., Liu, C. Q., Kawamura, K., ... Fu, P. (2020). Increase of High Molecular Weight Organosulfate With Intensifying Urban Air Pollution in the Megacity Beijing. Journal of Geophysical Research: Atmospheres, 125(10), Article e2019JD032200. https://doi.org/10.1029/2019JD032200

@article{8436647c2e6b451386d05522aa20967d,

title = "Increase of High Molecular Weight Organosulfate With Intensifying Urban Air Pollution in the Megacity Beijing",

abstract = "Organosulfates (OSs), a key component of secondary organic aerosols (SOA), account for up to one third of organic matter in the atmosphere. However, high molecular weight (HMW, 500–800 Da) OSs in ambient aerosols are poorly characterized at a molecular level, due to experimental difficulties. With Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICRMS), we are able to identify more than 8,000 OSs in wintertime aerosols in Beijing. We found that both the number and signal magnitudes of HMW OSs with low H/C and O/C ratios and degrees of unsaturation were greatly enhanced during hazy days, indicating that most HMW OSs were freshly formed during stagnant air pollution episodes. They are most likely to be the oxidation products of semivolatility to low-volatility precursors (e.g., polycyclic aromatic hydrocarbons and fatty acids) and have showed a strong influence of anthropogenic emissions. The molecular corridor analysis suggests that the high abundance of HMW aromatic-like and aliphatic OSs considerably decreases the volatility of organic aerosols in the urban atmosphere.",

keywords = "FT-ICR MS, Organic aerosol, Organosulfates, Secondary organic aerosol, Volatile organic compounds",

author = "Qiaorong Xie and Ying Li and Siyao Yue and Sihui Su and Dong Cao and Yisheng Xu and Jing Chen and Haijie Tong and Hang Su and Yafang Cheng and Wanyu Zhao and Wei Hu and Zhe Wang and Ting Yang and Xiaole Pan and Yele Sun and Zifa Wang and Liu, {Cong Qiang} and Kimitaka Kawamura and Guibin Jiang and Manabu Shiraiwa and Pingqing Fu",

note = "Funding Information: This work was supported by the National Natural Science Foundation of China (Grants 41625014, 41475117, and 41571130024). The authors acknowledge stimulating exchange with U. P?schl (Max Planck Institute for Chemistry, Germany). We thank L. Wei, L. Li, and Q. Zhao (Institute of Atmospheric Physics, Chinese Academy of Sciences, China) and L. Ren and H. Ren (Tianjin University, China) for their helpful discussions. The authors declare no competing financial interests. Supporting description of figures and tables are provided in the supporting information. The data used in this manuscript are listed in the tables, figures, and supporting information. The data can be found online (at https://zenodo.org/record/3740839#.XoqGuy276QI). Publisher Copyright: {\textcopyright}2020. American Geophysical Union. All Rights Reserved. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.",

year = "2020",

month = may,

day = "27",

doi = "10.1029/2019JD032200",

language = "English",

volume = "125",

journal = "Journal of Geophysical Research: Atmospheres",

issn = "2169-897X",

publisher = "Wiley-Blackwell",

number = "10",

}

Xie, Q, Li, Y, Yue, S, Su, S, Cao, D, Xu, Y, Chen, J, Tong, H, Su, H, Cheng, Y, Zhao, W, Hu, W, Wang, Z, Yang, T, Pan, X, Sun, Y, Wang, Z, Liu, CQ, Kawamura, K, Jiang, G, Shiraiwa, M & Fu, P 2020, 'Increase of High Molecular Weight Organosulfate With Intensifying Urban Air Pollution in the Megacity Beijing', Journal of Geophysical Research: Atmospheres, vol. 125, no. 10, e2019JD032200. https://doi.org/10.1029/2019JD032200

TY - JOUR

T1 - Increase of High Molecular Weight Organosulfate With Intensifying Urban Air Pollution in the Megacity Beijing

AU - Xie, Qiaorong

AU - Li, Ying

AU - Yue, Siyao

AU - Su, Sihui

AU - Cao, Dong

AU - Xu, Yisheng

AU - Chen, Jing

AU - Tong, Haijie

AU - Su, Hang

AU - Cheng, Yafang

AU - Zhao, Wanyu

AU - Hu, Wei

AU - Wang, Zhe

AU - Yang, Ting

AU - Pan, Xiaole

AU - Sun, Yele

AU - Wang, Zifa

AU - Liu, Cong Qiang

AU - Kawamura, Kimitaka

AU - Jiang, Guibin

AU - Shiraiwa, Manabu

AU - Fu, Pingqing

N1 - Funding Information: This work was supported by the National Natural Science Foundation of China (Grants 41625014, 41475117, and 41571130024). The authors acknowledge stimulating exchange with U. P?schl (Max Planck Institute for Chemistry, Germany). We thank L. Wei, L. Li, and Q. Zhao (Institute of Atmospheric Physics, Chinese Academy of Sciences, China) and L. Ren and H. Ren (Tianjin University, China) for their helpful discussions. The authors declare no competing financial interests. Supporting description of figures and tables are provided in the supporting information. The data used in this manuscript are listed in the tables, figures, and supporting information. The data can be found online (at https://zenodo.org/record/3740839#.XoqGuy276QI). Publisher Copyright: ©2020. American Geophysical Union. All Rights Reserved. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.

PY - 2020/5/27

Y1 - 2020/5/27

N2 - Organosulfates (OSs), a key component of secondary organic aerosols (SOA), account for up to one third of organic matter in the atmosphere. However, high molecular weight (HMW, 500–800 Da) OSs in ambient aerosols are poorly characterized at a molecular level, due to experimental difficulties. With Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICRMS), we are able to identify more than 8,000 OSs in wintertime aerosols in Beijing. We found that both the number and signal magnitudes of HMW OSs with low H/C and O/C ratios and degrees of unsaturation were greatly enhanced during hazy days, indicating that most HMW OSs were freshly formed during stagnant air pollution episodes. They are most likely to be the oxidation products of semivolatility to low-volatility precursors (e.g., polycyclic aromatic hydrocarbons and fatty acids) and have showed a strong influence of anthropogenic emissions. The molecular corridor analysis suggests that the high abundance of HMW aromatic-like and aliphatic OSs considerably decreases the volatility of organic aerosols in the urban atmosphere.

AB - Organosulfates (OSs), a key component of secondary organic aerosols (SOA), account for up to one third of organic matter in the atmosphere. However, high molecular weight (HMW, 500–800 Da) OSs in ambient aerosols are poorly characterized at a molecular level, due to experimental difficulties. With Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICRMS), we are able to identify more than 8,000 OSs in wintertime aerosols in Beijing. We found that both the number and signal magnitudes of HMW OSs with low H/C and O/C ratios and degrees of unsaturation were greatly enhanced during hazy days, indicating that most HMW OSs were freshly formed during stagnant air pollution episodes. They are most likely to be the oxidation products of semivolatility to low-volatility precursors (e.g., polycyclic aromatic hydrocarbons and fatty acids) and have showed a strong influence of anthropogenic emissions. The molecular corridor analysis suggests that the high abundance of HMW aromatic-like and aliphatic OSs considerably decreases the volatility of organic aerosols in the urban atmosphere.

KW - FT-ICR MS

KW - Organic aerosol

KW - Organosulfates

KW - Secondary organic aerosol

KW - Volatile organic compounds

UR - http://www.scopus.com/inward/record.url?scp=85085310257&partnerID=8YFLogxK

U2 - 10.1029/2019JD032200

DO - 10.1029/2019JD032200

M3 - Journal article

AN - SCOPUS:85085310257

SN - 2169-897X

VL - 125

JO - Journal of Geophysical Research: Atmospheres

JF - Journal of Geophysical Research: Atmospheres

IS - 10

M1 - e2019JD032200

ER -

Increase of High Molecular Weight Organosulfate With Intensifying Urban Air Pollution in the Megacity Beijing

Abstract

Keywords

ASJC Scopus subject areas

UN SDGs

More information

Other files and links

Fingerprint

Cite this