Preprints
https://doi.org/10.5194/acp-2020-1186
https://doi.org/10.5194/acp-2020-1186

  18 Dec 2020

18 Dec 2020

Review status: a revised version of this preprint was accepted for the journal ACP and is expected to appear here in due course.

Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid-dimethylamine nucleation

Ling Liu1, Fangqun Yu2, Kaipeng Tu1, Zhi Yang1, and Xiuhui Zhang1 Ling Liu et al.
  • 1Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
  • 2Atmospheric Sciences Research Center, University at Albany, Albany, New York 12203, USA

Abstract. Ambient measurements combined with theoretical simulations have shown evidence that the tropospheric degradation end-products of Freon alternatives, trifluoroacetic acid (TFA), one of the most important and abundant atmospheric organic substances, can enhance the process of sulfuric acid (SA) – dimethylamine (DMA) – based nucleation process in urban environments. However, TFA is widespread all over the world with different atmospheric conditions, such as temperature and nucleation precursor concentration, which are the most important factors potentially influencing the atmospheric nucleation process and thus inducing different nucleation mechanisms. Herein, using the Density Functional Theory combined with the Atmospheric Cluster Dynamics Code, the influence of temperature and nucleation precursor concentration on the role of TFA in the SA-DMA nucleation has been investigated. The results indicate that the growth trends of clusters involving TFA can increase with the decrease of temperature. The enhancement of particle formation rate by TFA and the contributions of SA-DMA-TFA cluster to the cluster formation pathways can be up to as much as 227 times and 95 %, respectively, at relatively low temperature, low SA concentration, high TFA concentration and high DMA concentration, such as in winter or at relatively high atmospheric boundary layer and in megacities far away from industrial sources of sulfur-containing pollutants. These results provide the perspective of the realistic role of TFA in different atmospheric environments, revealing the potential influence of the tropospheric degradation of Freon alternatives under a wide range of atmospheric conditions.

Ling Liu et al.

 
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Ling Liu et al.

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Short summary
Trifluoroacetic acid (TFA), was previously proved to participate in sulfuric acid (SA)-dimethylamine (DMA) nucleation in Shanghai, China. However, complex atmospheric environments can influence the nucleation of aerosol significantly. We show the influence of different atmospheric conditions on the SA-DMA-TFA nucleation and find the enhancement by TFA can be significant in cold and polluted areas, which provides the perspective of the realistic role of TFA in different atmospheric environments.
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