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Volume 18, issue 17 | Copyright

Special issue: Regional transport and transformation of air pollution in...

Atmos. Chem. Phys., 18, 13155-13171, 2018
https://doi.org/10.5194/acp-18-13155-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 12 Sep 2018

Research article | 12 Sep 2018

Heterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China: roles of aerosol water content and chemical composition

Yee Jun Tham1,2, Zhe Wang1, Qinyi Li1,a, Weihao Wang1, Xinfeng Wang3, Keding Lu4, Nan Ma5, Chao Yan2, Simonas Kecorius5, Alfred Wiedensohler5, Yuanhang Zhang4, and Tao Wang1 Yee Jun Tham et al.
  • 1Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hong Kong, China
  • 2Institute for Atmospheric and Earth System Research/Physics, University of Helsinki, 00014, Helsinki, Finland
  • 3Environment Research Institute, Shandong University, Jinan, Shandong, China
  • 4State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China
  • 5Leibniz Institute for Tropospheric Research, Permoserstr. 15, 04318 Leipzig, Germany
  • anow at: Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Madrid 28006, Spain

Abstract. Heterogeneous uptake of dinitrogen pentoxide (N2O5) and production of nitryl chloride (ClNO2) are important nocturnal atmospheric processes that have significant implications for the production of secondary pollutants. However, the understanding of N2O5 uptake processes and ClNO2 production remains limited, especially in China. This study presents a field investigation of the N2O5 heterogeneous uptake coefficient (γ(N2O5)) and ClNO2 production yield (ϕ) in a polluted area of northern China during the summer of 2014. The N2O5 uptake coefficient and ClNO2 yield were estimated by using the simultaneously measured ClNO2 and total nitrate in 10 selected cases, which have concurrent increases in the ClNO2 and nitrate concentrations and relatively stable environmental conditions. The determined γ(N2O5) and ϕ values varied greatly, with an average of 0.022 for γ(N2O5) (±0.012, standard deviation) and 0.34 for ϕ (±0.28, standard deviation). The variations in γ(N2O5) could not be fully explained by the previously derived parameterizations of N2O5 uptake that consider nitrate, chloride, and the organic coating. Heterogeneous uptake of N2O5 was found to have a strong positive dependence on the relative humidity and aerosol water content. This result suggests that the heterogeneous uptake of N2O5 in Wangdu is governed mainly by the amount of water in the aerosol, and is strongly water limited, which is different from most of the field observations in the US and Europe. The ClNO2 yield estimated from the parameterization was also overestimated comparing to that derived from the observation. The observation-derived ϕ showed a decreasing trend with an increasing ratio of acetonitrile to carbon monoxide, an indicator of biomass burning emissions, which suggests a possible suppressive effect on the production yield of ClNO2 in the plumes influenced by biomass burning in this region. The findings of this study illustrate the need to improve our understanding and to parameterize the key factors for γ(N2O5) and ϕ to accurately assess photochemical and haze pollution.

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This study addresses the limited understanding of heterogeneous N2O5 uptake and ClNO2 production in the polluted environment of China. The results showed that N2O5 uptake and ClNO2 yield cannot be well explained by previous parameterizations and were largely influenced by factors like aerosol water content and biomass burning emission. Our findings illuminate the need to realistically parameterize these heterogeneous processes for better simulation of photochemical and haze pollution in China.
This study addresses the limited understanding of heterogeneous N2O5 uptake and ClNO2 production...
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