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Volume 18, issue 2
Atmos. Chem. Phys., 18, 673-689, 2018
https://doi.org/10.5194/acp-18-673-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 3.0 License.

Special issue: HD(CP)2 Observational Prototype Experiment (AMT/ACP...

Atmos. Chem. Phys., 18, 673-689, 2018
https://doi.org/10.5194/acp-18-673-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 19 Jan 2018

Research article | 19 Jan 2018

A parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: improvement of particulate nitrate prediction

Ying Chen1,2,a, Ralf Wolke1, Liang Ran3, Wolfram Birmili1,4, Gerald Spindler1, Wolfram Schröder1, Hang Su2,5, Yafang Cheng2,5, Ina Tegen1, and Alfred Wiedensohler1 Ying Chen et al.
  • 1Leibniz-Institute for Tropospheric Research (TROPOS), 04318 Leipzig, Germany
  • 2Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
  • 3Key Laboratory of Middle Atmosphere and Global Environment Observation, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China
  • 4German Environment Agency, 06844 Dessau-Roßlau, Germany
  • 5Institute for Environmental and Climate Research, Jinan University, Guangzhou, China
  • anow at: Lancaster Environment Centre, Lancaster University, Lancaster, LA1 4YQ, UK

Abstract. The heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R = 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO–MUSCAT, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10–25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3] was significantly overestimated for this period by a factor of 5–19, with the corrected NH3 emissions (reduced by 50%) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3] by  ∼ 35%. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17–18 and 25 September 2013) when [NO3] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3] of less than 2% on average and 20% at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.

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The heterogeneous hydrolysis of N2O5 on particle surfaces is crucial for the nitrogen cycle in the atmosphere. The reaction rate is determined by meteorological and particle properties, but its parameterization in previous 3-D modelling studies did not comprehensively consider these parameters. We propose a parameterization to take these into account and improve nitrate prediction; we report that the organic coating suppression on the N2O5 reaction is not as important as expected in the EU.
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