Unprecedented Ambient Sulfur Trioxide (SO3) Detection: Possible Formation Mechanism and Atmospheric Implications

Lei Yao; Xiaolong Fan; Chao Yan; Theo Kurtén; Kaspar R. Daellenbach; Chang Li; Yonghong Wang; Yishuo Guo; Lubna Dada; Matti P. Rissanen; Jing Cai; Yee Jun Tham; Qiaozhi Zha; Shaojun Zhang; Wei Du; Miao Yu; Feixue Zheng; Ying Zhou; Jenni Kontkanen; Tommy Chan; Jiali Shen; Joni T. Kujansuu; Juha Kangasluoma; Jingkun Jiang; Lin Wang; Douglas R. Worsnop; Tuukka Petäjä; Veli Matti Kerminen; Yongchun Liu; Biwu Chu; Hong He; Markku Kulmala; Federico Bianchi

doi:10.1021/acs.estlett.0c00615

Unprecedented Ambient Sulfur Trioxide (SO₃) Detection: Possible Formation Mechanism and Atmospheric Implications

Lei Yao, Xiaolong Fan, Chao Yan, Theo Kurtén, Kaspar R. Daellenbach, Chang Li, Yonghong Wang, Yishuo Guo, Lubna Dada, Matti P. Rissanen, Jing Cai, Yee Jun Tham, Qiaozhi Zha, Shaojun Zhang, Wei Du, Miao Yu, Feixue Zheng, Ying Zhou, Jenni Kontkanen, Tommy ChanJiali Shen, Joni T. Kujansuu, Juha Kangasluoma, Jingkun Jiang, Lin Wang, Douglas R. Worsnop, Tuukka Petäjä, Veli Matti Kerminen, Yongchun Liu, Biwu Chu, Hong He, Markku Kulmala, Federico Bianchi

Physics

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Abstract

Sulfur trioxide (SO₃) is a crucial compound for atmospheric sulfuric acid (H₂SO₄) formation, acid rain formation, and other atmospheric physicochemical processes. During the daytime, SO₃is mainly produced from the photo-oxidation of SO₂by OH radicals. However, the sources of SO₃during the early morning and night, when OH radicals are scarce, are not fully understood. We report results from two field measurements in urban Beijing during winter and summer 2019, using a nitrate-CI-APi-LTOF (chemical ionization-Atmospheric pressure interface-long-Time-of-flight) mass spectrometer to detect atmospheric SO₃and H₂SO₄. Our results show the level of SO₃was higher during the winter than during the summer, with high SO₃levels observed especially during the early morning (05:00 to 08:30) and night (18:00 to 05:00 the next day). On the basis of analysis of SO₂, NO_x, black carbon, traffic flow, and atmospheric ions, we suggest SO₃could be formed from the catalytic oxidation of SO₂on the surface of traffic-related black carbon. This previously unidentified SO₃source results in significant H₂SO₄formation in the early morning and thus promotes sub-2.5 nm particle formation. These findings will help in understanding urban SO₃and formulating policies to mitigate secondary particle formation in Chinese megacities.

Original language	English
Pages (from-to)	809-818
Number of pages	10
Journal	Environmental Science and Technology Letters
Volume	7
Issue number	11
DOIs	https://doi.org/10.1021/acs.estlett.0c00615
Publication status	Published - 10 Nov 2020
Publication type	A1 Journal article-refereed

Publication forum classification

Publication forum level 1

ASJC Scopus subject areas

Environmental Chemistry
Ecology
Water Science and Technology
Waste Management and Disposal
Pollution
Health, Toxicology and Mutagenesis

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Unprecedented ambient sulfur trioxide 2020
CC BY
Final published version, 3.89 MBLicence: CC BY

http://urn.fi/URN:NBN:fi:tuni-202101151365Licence: CC BY

Cite this

Yao, L., Fan, X., Yan, C., Kurtén, T., Daellenbach, K. R., Li, C., Wang, Y., Guo, Y., Dada, L., Rissanen, M. P., Cai, J., Tham, Y. J., Zha, Q., Zhang, S., Du, W., Yu, M., Zheng, F., Zhou, Y., Kontkanen, J., ... Bianchi, F. (2020). Unprecedented Ambient Sulfur Trioxide (SO₃) Detection: Possible Formation Mechanism and Atmospheric Implications. Environmental Science and Technology Letters, 7(11), 809-818. https://doi.org/10.1021/acs.estlett.0c00615

@article{b63ce6b0edea4ffc81e3de4be9a781ed,

title = "Unprecedented Ambient Sulfur Trioxide (SO3) Detection: Possible Formation Mechanism and Atmospheric Implications",

abstract = "Sulfur trioxide (SO3) is a crucial compound for atmospheric sulfuric acid (H2SO4) formation, acid rain formation, and other atmospheric physicochemical processes. During the daytime, SO3is mainly produced from the photo-oxidation of SO2by OH radicals. However, the sources of SO3during the early morning and night, when OH radicals are scarce, are not fully understood. We report results from two field measurements in urban Beijing during winter and summer 2019, using a nitrate-CI-APi-LTOF (chemical ionization-Atmospheric pressure interface-long-Time-of-flight) mass spectrometer to detect atmospheric SO3and H2SO4. Our results show the level of SO3was higher during the winter than during the summer, with high SO3levels observed especially during the early morning (05:00 to 08:30) and night (18:00 to 05:00 the next day). On the basis of analysis of SO2, NOx, black carbon, traffic flow, and atmospheric ions, we suggest SO3could be formed from the catalytic oxidation of SO2on the surface of traffic-related black carbon. This previously unidentified SO3source results in significant H2SO4formation in the early morning and thus promotes sub-2.5 nm particle formation. These findings will help in understanding urban SO3and formulating policies to mitigate secondary particle formation in Chinese megacities.",

author = "Lei Yao and Xiaolong Fan and Chao Yan and Theo Kurt{\'e}n and Daellenbach, {Kaspar R.} and Chang Li and Yonghong Wang and Yishuo Guo and Lubna Dada and Rissanen, {Matti P.} and Jing Cai and Tham, {Yee Jun} and Qiaozhi Zha and Shaojun Zhang and Wei Du and Miao Yu and Feixue Zheng and Ying Zhou and Jenni Kontkanen and Tommy Chan and Jiali Shen and Kujansuu, {Joni T.} and Juha Kangasluoma and Jingkun Jiang and Lin Wang and Worsnop, {Douglas R.} and Tuukka Pet{\"a}j{\"a} and Kerminen, {Veli Matti} and Yongchun Liu and Biwu Chu and Hong He and Markku Kulmala and Federico Bianchi",

note = "Funding Information: The work is supported by Academy of Finland (Center of Excellence in Atmospheric Sciences, project no. 307331, and PROFI3 funding, 311932), the European Research Council via ATM-GTP (742206) and via CHAPAs (850614) and the EMME-CARE project which has received funding from the European Union{\textquoteright}s Horizon 2020 Research and Innovation Programme, under Grant Agreement No. 856612. Publisher Copyright: {\textcopyright} 2020 American Chemical Society. All rights reserved. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.",

year = "2020",

month = nov,

day = "10",

doi = "10.1021/acs.estlett.0c00615",

language = "English",

volume = "7",

pages = "809--818",

number = "11",

}

Yao, L, Fan, X, Yan, C, Kurtén, T, Daellenbach, KR, Li, C, Wang, Y, Guo, Y, Dada, L, Rissanen, MP, Cai, J, Tham, YJ, Zha, Q, Zhang, S, Du, W, Yu, M, Zheng, F, Zhou, Y, Kontkanen, J, Chan, T, Shen, J, Kujansuu, JT, Kangasluoma, J, Jiang, J, Wang, L, Worsnop, DR, Petäjä, T, Kerminen, VM, Liu, Y, Chu, B, He, H, Kulmala, M & Bianchi, F 2020, 'Unprecedented Ambient Sulfur Trioxide (SO₃) Detection: Possible Formation Mechanism and Atmospheric Implications', Environmental Science and Technology Letters, vol. 7, no. 11, pp. 809-818. https://doi.org/10.1021/acs.estlett.0c00615

TY - JOUR

T1 - Unprecedented Ambient Sulfur Trioxide (SO3) Detection

T2 - Possible Formation Mechanism and Atmospheric Implications

AU - Yao, Lei

AU - Fan, Xiaolong

AU - Yan, Chao

AU - Kurtén, Theo

AU - Daellenbach, Kaspar R.

AU - Li, Chang

AU - Wang, Yonghong

AU - Guo, Yishuo

AU - Dada, Lubna

AU - Rissanen, Matti P.

AU - Cai, Jing

AU - Tham, Yee Jun

AU - Zha, Qiaozhi

AU - Zhang, Shaojun

AU - Du, Wei

AU - Yu, Miao

AU - Zheng, Feixue

AU - Zhou, Ying

AU - Kontkanen, Jenni

AU - Chan, Tommy

AU - Shen, Jiali

AU - Kujansuu, Joni T.

AU - Kangasluoma, Juha

AU - Jiang, Jingkun

AU - Wang, Lin

AU - Worsnop, Douglas R.

AU - Petäjä, Tuukka

AU - Kerminen, Veli Matti

AU - Liu, Yongchun

AU - Chu, Biwu

AU - He, Hong

AU - Kulmala, Markku

AU - Bianchi, Federico

N1 - Funding Information: The work is supported by Academy of Finland (Center of Excellence in Atmospheric Sciences, project no. 307331, and PROFI3 funding, 311932), the European Research Council via ATM-GTP (742206) and via CHAPAs (850614) and the EMME-CARE project which has received funding from the European Union’s Horizon 2020 Research and Innovation Programme, under Grant Agreement No. 856612. Publisher Copyright: © 2020 American Chemical Society. All rights reserved. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.

PY - 2020/11/10

Y1 - 2020/11/10

N2 - Sulfur trioxide (SO3) is a crucial compound for atmospheric sulfuric acid (H2SO4) formation, acid rain formation, and other atmospheric physicochemical processes. During the daytime, SO3is mainly produced from the photo-oxidation of SO2by OH radicals. However, the sources of SO3during the early morning and night, when OH radicals are scarce, are not fully understood. We report results from two field measurements in urban Beijing during winter and summer 2019, using a nitrate-CI-APi-LTOF (chemical ionization-Atmospheric pressure interface-long-Time-of-flight) mass spectrometer to detect atmospheric SO3and H2SO4. Our results show the level of SO3was higher during the winter than during the summer, with high SO3levels observed especially during the early morning (05:00 to 08:30) and night (18:00 to 05:00 the next day). On the basis of analysis of SO2, NOx, black carbon, traffic flow, and atmospheric ions, we suggest SO3could be formed from the catalytic oxidation of SO2on the surface of traffic-related black carbon. This previously unidentified SO3source results in significant H2SO4formation in the early morning and thus promotes sub-2.5 nm particle formation. These findings will help in understanding urban SO3and formulating policies to mitigate secondary particle formation in Chinese megacities.

AB - Sulfur trioxide (SO3) is a crucial compound for atmospheric sulfuric acid (H2SO4) formation, acid rain formation, and other atmospheric physicochemical processes. During the daytime, SO3is mainly produced from the photo-oxidation of SO2by OH radicals. However, the sources of SO3during the early morning and night, when OH radicals are scarce, are not fully understood. We report results from two field measurements in urban Beijing during winter and summer 2019, using a nitrate-CI-APi-LTOF (chemical ionization-Atmospheric pressure interface-long-Time-of-flight) mass spectrometer to detect atmospheric SO3and H2SO4. Our results show the level of SO3was higher during the winter than during the summer, with high SO3levels observed especially during the early morning (05:00 to 08:30) and night (18:00 to 05:00 the next day). On the basis of analysis of SO2, NOx, black carbon, traffic flow, and atmospheric ions, we suggest SO3could be formed from the catalytic oxidation of SO2on the surface of traffic-related black carbon. This previously unidentified SO3source results in significant H2SO4formation in the early morning and thus promotes sub-2.5 nm particle formation. These findings will help in understanding urban SO3and formulating policies to mitigate secondary particle formation in Chinese megacities.

U2 - 10.1021/acs.estlett.0c00615

DO - 10.1021/acs.estlett.0c00615

M3 - Article

AN - SCOPUS:85093941588

SN - 2328-8930

VL - 7

SP - 809

EP - 818

JO - Environmental Science and Technology Letters

JF - Environmental Science and Technology Letters

IS - 11

ER -