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Discussion papers
https://doi.org/10.5194/acp-2018-1132
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1132
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 29 Nov 2018

Research article | 29 Nov 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

A proxy for atmospheric daytime gaseous sulfuric acid concentration in urban Beijing

Yiqun Lu1, Chao Yan2, Yueyun Fu3, Yan Chen4, Yiliang Liu1, Gan Yang1, Yuwei Wang1, Federico Bianchi2, Biwu Chu2, Ying Zhou5, Rujing Yin3, Rima Baalbaki2, Olga Garmash2, Chenjuan Deng3, Weigang Wang4, Yongchun Liu5, Tuukka Petäjä2,5,6, Veli-Matti Kerminen2, Jingkun Jiang3, Markku Kulmala2,5, and Lin Wang1,7,8 Yiqun Lu et al.
  • 1Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Jiangwan Campus, Fudan University, Shanghai 200438, China
  • 2Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
  • 3State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
  • 4Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
  • 5Aerosol and Haze Laboratory, Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
  • 6Joint International Research Laboratory of Atmospheric and Earth System Sciences (JirLATEST), School of Atmospheric Sciences, Nanjing University, Nanjing 210023, China
  • 7Institute of Atmospheric Sciences, Jiangwan Campus, Fudan University, Shanghai 200438, China
  • 8Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China

Abstract. Gaseous sulfuric acid is known as one of the key precursors for atmospheric new particle formation processes, but its measurement remains a major challenge. A proxy method that is able to derive gaseous sulfuric acid concentrations from parameters that can be measured relatively easily and accurately is therefore highly desirable among the atmospheric chemistry community. Although such methods are available for clean atmospheric environments, a proxy that works well in a polluted atmosphere, such as those in Chinese megacities, is yet to be developed. In this study, the gaseous sulfuric acid concentration was measured in February–March, 2018, in urban Beijing by a nitrate based – Long Time-of-Flight Chemical Ionization Mass Spectrometer (LToF-CIMS). A number of atmospheric parameters were recorded concurrently including the ultraviolet radiation B (UVB) intensity, concentrations of O3, NOx, SO2 and HONO, and aerosol particle number size distributions. A proxy for atmospheric daytime gaseous sulfuric acid concentration was derived using a statistical analysis method by using the UVB intensity, [SO2], condensation sink (CS), [O3], and [HONO] (or [NOx]) as the predictor variables. In this proxy method, we considered the formation of gaseous sulfuric acid from reactions of SO2 and OH radicals during the daytime, and loss of gaseous sulfuric acid due to its condensation onto the pre-existing particles. In addition, we explored formation of OH radicals from the conventional gas-phase photochemistry using ozone as a proxy and from the photolysis of heterogeneously-formed HONO using HONO (and subsequently NOx) as a proxy. Our results showed that the UVB intensity and [SO2] are dominant factors for the production of gaseous sulfuric acid, and that the simplest proxy could be constructed with the UVB intensity and [SO2] alone, resulting in up to 29% relative deviations when sulfuric acid concentrations were larger than 2.0×106moleculescm−3. When the OH radical production from both homogenously- and heterogeneously-formed precursors were considered, the relative deviations were lower than 24%.

Yiqun Lu et al.
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Short summary
Gaseous sulfuric acid is one of the key precursors for atmospheric new particle formation processes, but its measurement remains a major challenge. This work develops an estimation method for gaseous sulfuric acid concentration in an urban environment in China using multiple atmospheric variables that are easier to measure. Consideration of heterogeneous formation of HONO and subsequent photo-production of OH radicals improves the performance of the estimation method.
Gaseous sulfuric acid is one of the key precursors for atmospheric new particle formation...
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