Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation
<p>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 nucleation process based on...
| Main Authors: | , , , , |
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2021-04-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://acp.copernicus.org/articles/21/6221/2021/acp-21-6221-2021.pdf |
| _version_ | 1818669410070560768 |
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| author | L. Liu F. Yu K. Tu Z. Yang X. Zhang |
| author_facet | L. Liu F. Yu K. Tu Z. Yang X. Zhang |
| author_sort | L. Liu |
| collection | DOAJ |
| description | <p>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 nucleation process based on sulfuric acid (SA) and dimethylamine (DMA) in urban environments. However, TFA is widespread all over the world under 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 concentrations 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 in temperature. The enhancement on particle formation rate by TFA and the contributions of the SA–DMA–TFA cluster to the cluster formation pathways can be up to 227-fold and 95 %, respectively, at relatively low temperature, low SA concentration, high TFA concentration, and high DMA concentration, such as in winter, at the relatively high atmospheric boundary layer, or 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.</p> |
| first_indexed | 2024-12-17T06:51:46Z |
| format | Article |
| id | doaj.art-960352f6bf1c4d45bf13524faaab97c2 |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-12-17T06:51:46Z |
| publishDate | 2021-04-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-960352f6bf1c4d45bf13524faaab97c22022-12-21T21:59:34ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242021-04-01216221623010.5194/acp-21-6221-2021Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleationL. Liu0F. Yu1K. Tu2Z. Yang3X. Zhang4Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, ChinaAtmospheric Sciences Research Center, University at Albany, Albany, New York 12203, USAKey Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, ChinaKey Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, ChinaKey Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China<p>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 nucleation process based on sulfuric acid (SA) and dimethylamine (DMA) in urban environments. However, TFA is widespread all over the world under 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 concentrations 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 in temperature. The enhancement on particle formation rate by TFA and the contributions of the SA–DMA–TFA cluster to the cluster formation pathways can be up to 227-fold and 95 %, respectively, at relatively low temperature, low SA concentration, high TFA concentration, and high DMA concentration, such as in winter, at the relatively high atmospheric boundary layer, or 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.</p>https://acp.copernicus.org/articles/21/6221/2021/acp-21-6221-2021.pdf |
| spellingShingle | L. Liu F. Yu K. Tu Z. Yang X. Zhang Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation Atmospheric Chemistry and Physics |
| title | Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation |
| title_full | Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation |
| title_fullStr | Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation |
| title_full_unstemmed | Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation |
| title_short | Influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid–dimethylamine nucleation |
| title_sort | influence of atmospheric conditions on the role of trifluoroacetic acid in atmospheric sulfuric acid dimethylamine nucleation |
| url | https://acp.copernicus.org/articles/21/6221/2021/acp-21-6221-2021.pdf |
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