Unprecedented Ambient Sulfur Trioxide (SO3) Detection: Possible Formation Mechanism and Atmospheric Implications,Environmental Science & Technology Letters

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Unprecedented Ambient Sulfur Trioxide (SO3) Detection: Possible Formation Mechanism and Atmospheric Implications
Environmental Science & Technology Letters ( IF 10.9 ) Pub Date : 2020-09-25 , DOI: 10.1021/acs.estlett.0c00615
Lei Yao _{1,

2} , Xiaolong Fan ₁ , Chao Yan ₂ , Theo Kurtén ₃ , Kaspar R. Daellenbach ₂ , Chang Li ₁ , Yonghong Wang ₂ , Yishuo Guo ₁ , Lubna Dada ₂ , Matti P. Rissanen ₄ , Jing Cai ₂ , Yee Jun Tham ₂ , Qiaozhi Zha ₂ , Shaojun Zhang ₅ , Wei Du ₂ , Miao Yu ₆ , Feixue Zheng ₁ , Ying Zhou ₁ , Jenni Kontkanen ₂ , Tommy Chan ₂ , Jiali Shen ₂ , Joni T. Kujansuu _{1,

2} , Juha Kangasluoma _{1,

2} , Jingkun Jiang ₅ , Lin Wang ₇ , Douglas R. Worsnop ₈ , Tuukka Petäjä ₂ , Veli-Matti Kerminen ₂ , Yongchun Liu ₁ , Biwu Chu _{2,

9,

10} , Hong He _{9,

10} , Markku Kulmala _{1,

2,

11} , Federico Bianchi _{1,

2}

Affiliation

Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100089, China
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki 00560, Finland
Department of Chemistry, University of Helsinki, Helsinki 00014, Finland
Aerosol Physics Laboratory, Physics Unit, Tampere University, Tampere 33100, Finland
State Key Joint Laboratory of Environment Simulation and Pollution Control, State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, School of Environment, Tsinghua University, Beijing 100084, China
Institute of Urban Meteorology, China Meteorological Administration, Beijing 100081, China
Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University, Shanghai 200438, China
Aerodyne Research Inc., Billerica, Massachusetts 01821, United States
State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
Joint International Research Laboratory of Atmospheric and Earth System Sciences (JirLATEST), Nanjing University, Nanjing 210023, China

Sulfur trioxide (SO₃) is a crucial compound for atmospheric sulfuric acid (H₂SO₄) formation, acid rain formation, and other atmospheric physicochemical processes. During the daytime, SO₃ is mainly produced from the photo-oxidation of SO₂ by OH radicals. However, the sources of SO₃ during 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 SO₃ and H₂SO₄. Our results show the level of SO₃ was higher during the winter than during the summer, with high SO₃ levels 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 SO₃ could be formed from the catalytic oxidation of SO₂ on the surface of traffic-related black carbon. This previously unidentified SO₃ source results in significant H₂SO₄ formation in the early morning and thus promotes sub-2.5 nm particle formation. These findings will help in understanding urban SO₃ and formulating policies to mitigate secondary particle formation in Chinese megacities.

更新日期：2020-11-12

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