30 Mar 2020

30 Mar 2020

Review status: a revised version of this preprint was accepted for the journal ACP.

Formation of Nighttime Sulfuric Acid from the Ozonolysis of Alkenes in Beijing

Yishuo Guo1, Chao Yan1,2, Chang Li1, Zemin Feng1, Ying Zhou1, Zhuohui Lin1, Lubna Dada2, Dominik Stolzenburg2, Rujing Yin3, Jenni Kontkanen2, Kaspar R. Daellenbach2, Juha Kangasluoma1,2, Lei Yao2, Biwu Chu2, Yonghong Wang2, Runlong Cai2, Federico Bianchi2, Yongchun Liu1, and Markku Kulmala1,2 Yishuo Guo et al.
  • 1Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China
  • 2Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Finland
  • 3State 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, China

Abstract. Gaseous sulfuric acid (SA) has received a lot of attention for its crucial role in atmospheric new particle formation (NPF), and for this reason, studies until now have mainly focused on daytime SA when most NPF events occur. While daytime SA production is driven by SO2 oxidation of OH radicals from photochemical origin, the formation of SA during night and its potential influence on particle formation remains poorly understood. Here we present evidence for significant nighttime SA production in urban Beijing during winter, yielding concentrations between 1.0 and 3.0 × 106 cm−3. We found a high frequency (~ 30 %) of nighttime SA events, which are defined by the appearance of a distinct SA peak observed between 20:00 and 04:00 local time, and with the maximum concentration exceeding 1.0 × 106 cm−3. These events mostly occurred during unpolluted nights with low vapor condensation sink. Furthermore, we found that under very clean conditions (visibility > 16.0 km) with abundant ozone (concentration > 2.0 × 1011 cm−3, ~ 7 ppb), the overall sink of SA was strongly correlated with the products of O3, alkenes and SO2 concentrations, suggesting that the ozonolysis of alkenes played a major role in nighttime SA formation under such conditions. This is in light with previous studies showing that the ozonolysis of alkenes can form OH radical and stabilized Criegee intermediate (sCI), both of which are able to oxidize SO2 leading to SA formation. However, we also need to point out that there exist additional sources of SA under more polluted condition, which are not investigated in this study. Moreover, there was a strong correlation between SA concentration and the number concentration of sub-3 nm particles in both clean and polluted nights. Different from forest environments, where oxidized biogenic vapors are the main driver of nighttime clustering, our study demonstrates that the formation of nighttime cluster mode particles in urban environments is mainly driven by nighttime SA production.

Yishuo Guo et al.

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Yishuo Guo et al.


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Short summary
Fog, cloud, haze are very common natural phenomena and all of them have a great impact on global climate. Sulfuric acid (SA) is one of the key compounds forming these suspended particles (aerosols), and therefore the concentration, source and sink of SA is very important. Daytime SA production is driven by OH radical oxiation, and here this article shows that ozonolysis of alkenes played a major role in nighttime SA formation in urabn Beijing under clean conditions.