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© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 21 Nov 2019

Submitted as: research article | 21 Nov 2019

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

Multiphase MCM/CAPRAMmodeling of formation and processing of secondary aerosol constituents observed at the Mt. Tai summer campaign 2014

Yanhong Zhu1,2,a, Andreas Tilgner2, Erik Hans Hoffmann2, Hartmut Herrmann2,3, Kimitaka Kawamura4,b, Lingxiao Yang1, Likun Xue1, and Wenxing Wang1 Yanhong Zhu et al.
  • 1Environment Research Institute, Shandong University, 266237 Qingdao, China
  • 2Leibniz Institute for Tropospheric Research (TROPOS), Atmospheric Chemistry Department (ACD), 04318 Leipzig, Germany
  • 3School of Environmental Science and Engineering, Shandong University, 266237 Qingdao, China
  • 4Institute of Low Temperature Science, Hokkaido University, Sapporo 060-0819, Japan
  • anow at: Department of Atmospheric Sciences, School of Earth Sciences, Zhejiang University, 310012 Hangzhou, China
  • bnow at: Chubu Institute for Advanced Studies, Chubu University, Kasugai 487-8501, Japan

Abstract. Despite the high abundance of secondary aerosols in the atmosphere, their formation mechanisms remain poorly understood. In this study, MCM/CAPRAM mechanism is used to investigate the multiphase formation and processing of secondary aerosol constituents during the advection of air masses towards the measurement site of Mt. Tai in North China. Trajectories with and without chemical cloud interaction are modeled. Modeled radical and non-radical concentrations demonstrate that the summit of Mt. Tai, with an altitude of ∼1.5 km a.m.s.l., is characterized by a sub-urban oxidants budget. The modeled maximum gas-phase concentrations of OH radical are 3.2 × 106 molecules cm−3 and 3.5 × 106 molecules cm−3 in simulations with and without cloud passages in the air parcel, respectively. Different to previous studies at Mt. Tai, this study has modeled chemical formation processes of secondary aerosol constituents under day vs. night and cloud vs. non-cloud cases along the trajectories to Mt. Tai in detail. The model studies show that sulfate is mainly produced in simulations where the air parcel is influenced by cloud chemistry. Under the simulated conditions, the aqueous reaction of HSO3 with H2O2 is the major contributor to sulfate formation, contributing 67 % and 60 % in the simulations with cloud and non-cloud passages, respectively. The modeled nitrate formation is higher at nighttime than at daytime. The major pathway is aqueous-phase N2O5 hydrolysis, with a contribution of 72 % when cloud passages are considered and 70 % when not. Secondary organic aerosol (SOA) compounds, e.g. glyoxylic, oxalic, pyruvic and malonic acid, are found to be mostly produced from the aqueous oxidations of hydrated glyoxal, hydrated glyoxylic acid, nitro 2-oxopropanoate and hydrated 3-oxopropanoic acid, respectively. Sensitivity studies reveal that gaseous VOC emissions have a huge impact on the concentrations of modeled secondary aerosol compounds. Increasing the VOC emissions by a factor of two leads to linearly increased concentrations of the corresponding SOA compounds. Studies using the relative incremental reactivity (RIR) method have identified isoprene, 1,3-butadiene and toluene as the key precursors for glyoxylic and oxalic acid, but only isoprene is found to be a key precursor for pyruvic acid. Additionally, the model investigations demonstrate that an increased aerosol partitioning of glyoxal can play an important role in the aqueous-phase formation of glyoxylic and oxalic acid. Overall, the present study is the first that provides more detailed insights in the formation pathways of secondary aerosol constituents at Mt. Tai and clearly emphasizes the importance of aqueous-phase chemical processes on the production of multifunctional carboxylic acids.

Yanhong Zhu et al.
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Yanhong Zhu et al.
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Short summary
The formation and processing of secondary inorganic and organic compounds at Mt. Tai – the highest mountain over the North China Plain are modeled using a multiphase chemical model. The concentrations of key radical and non-radical oxidations in the formation processes are investigated. Sensitivity tests assess the impacts of emission data and glyoxal partitioning constants on modeled results. The key precursors of secondary organic compounds are also identified.
The formation and processing of secondary inorganic and organic compounds at Mt. Tai – the...