A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water
<p>While the formation and evolution of nitrate in airborne particles are extensively investigated, little is known about the processing of nitrate in clouds. Here we present a detailed investigation on the in-cloud formation of nitrate, based on the size-resolved mixing state of nitrate in th...
| Main Authors: | , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2022-07-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://acp.copernicus.org/articles/22/9571/2022/acp-22-9571-2022.pdf |
| _version_ | 1818160894997168128 |
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| author | G. Zhang G. Zhang G. Zhang X. Hu X. Hu X. Hu W. Sun W. Sun W. Sun Y. Yang Y. Yang Z. Guo Z. Guo Z. Guo Y. Fu Y. Fu H. Wang S. Zhou L. Li M. Tang M. Tang M. Tang Z. Shi D. Chen X. Bi X. Bi X. Bi X. Wang X. Wang X. Wang |
| author_facet | G. Zhang G. Zhang G. Zhang X. Hu X. Hu X. Hu W. Sun W. Sun W. Sun Y. Yang Y. Yang Z. Guo Z. Guo Z. Guo Y. Fu Y. Fu H. Wang S. Zhou L. Li M. Tang M. Tang M. Tang Z. Shi D. Chen X. Bi X. Bi X. Bi X. Wang X. Wang X. Wang |
| author_sort | G. Zhang |
| collection | DOAJ |
| description | <p>While the formation and evolution of nitrate in airborne particles are extensively investigated, little is known about the processing of nitrate in clouds. Here we present a detailed investigation on the in-cloud formation of nitrate, based on the size-resolved mixing state of nitrate in the individual cloud residual and cloud-free particles obtained by single
particle mass spectrometry, and also the mass concentrations of nitrate in
the cloud water and PM<span class="inline-formula"><sub>2.5</sub></span> at a mountain site (1690 m a.s.l. – above sea level) in southern China. The results show a significant enhancement of nitrate mass fraction and relative intensity of nitrate in the cloud water and the cloud residual particles, respectively, reflecting a critical role of in-cloud processing in the formation of nitrate. We first exclude the gas-phase scavenging of HNO<span class="inline-formula"><sub>3</sub></span> and the facilitated activation of nitrate-containing particles as the major contribution for the enhanced nitrate, according to the size distribution of nitrate in individual particles. Based on regression analysis and theoretical calculations, we then highlight the role of N<span class="inline-formula"><sub>2</sub></span>O<span class="inline-formula"><sub>5</sub></span> hydrolysis in the in-cloud formation of nitrate, even during the daytime, attributed to the diminished light in clouds. Nitrate is highly related (<span class="inline-formula"><i>R</i><sup>2</sup>=</span> <span class="inline-formula">∼</span> 0.6) to the variations in [NO<span class="inline-formula"><sub><i>x</i></sub></span>][O<span class="inline-formula"><sub>3</sub></span>], temperature, and droplet surface area in clouds. Accounting for droplet surface area greatly enhances the predictability of the observed nitrate, compared with using [NO<span class="inline-formula"><sub><i>x</i></sub></span>][O<span class="inline-formula"><sub>3</sub></span>] and temperature. The substantial contribution of N<span class="inline-formula"><sub>2</sub></span>O<span class="inline-formula"><sub>5</sub></span> hydrolysis to nitrate in clouds with diminished light during the daytime can be reproduced by a multiphase chemical box model. Assuming a photolysis rate at 30 % of the default setting, the overall contribution of N<span class="inline-formula"><sub>2</sub></span>O<span class="inline-formula"><sub>5</sub></span> hydrolysis pathway to nitrate formation increases by <span class="inline-formula">∼</span> 20 % in clouds. Given that N<span class="inline-formula"><sub>2</sub></span>O<span class="inline-formula"><sub>5</sub></span> hydrolysis acts as a major sink of NO<span class="inline-formula"><sub><i>x</i></sub></span> in the atmosphere, further model updates would improve our understanding about the processes contributing to nitrate production in cloud and the cycling of odd nitrogen.</p> |
| first_indexed | 2024-12-11T16:09:08Z |
| format | Article |
| id | doaj.art-a812392dc83e447c92bd1eb78b0f4c7b |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-12-11T16:09:08Z |
| publishDate | 2022-07-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-a812392dc83e447c92bd1eb78b0f4c7b2022-12-22T00:59:06ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242022-07-01229571958210.5194/acp-22-9571-2022A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud waterG. Zhang0G. Zhang1G. Zhang2X. Hu3X. Hu4X. Hu5W. Sun6W. Sun7W. Sun8Y. Yang9Y. Yang10Z. Guo11Z. Guo12Z. Guo13Y. Fu14Y. Fu15H. Wang16S. Zhou17L. Li18M. Tang19M. Tang20M. Tang21Z. Shi22D. Chen23X. Bi24X. Bi25X. Bi26X. Wang27X. Wang28X. Wang29State Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaGuangdong-Hong Kong–Macau Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, CAS, Guangzhou 510640, PR ChinaState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, PR ChinaState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, PR ChinaState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, PR ChinaState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaSchool of Atmospheric Sciences, Sun Yat-sen University, Guangzhou 519082, PR ChinaSchool of Atmospheric Sciences, Sun Yat-sen University, Guangzhou 519082, PR ChinaInstitute of Mass Spectrometer and Atmospheric Environment, Jinan University, Guangzhou 510632, PR ChinaState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaGuangdong-Hong Kong–Macau Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, CAS, Guangzhou 510640, PR ChinaSchool of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, UKState Environmental Protection Key Laboratory of Regional Air Quality Monitoring, Guangdong Environmental Monitoring Center, Guangzhou 510308, PR ChinaState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaGuangdong-Hong Kong–Macau Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, CAS, Guangzhou 510640, PR ChinaState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences (CAS), Guangzhou 510640, PR ChinaCenter for Excellence in Deep Earth Science, CAS, Guangzhou 510640, PR ChinaGuangdong-Hong Kong–Macau Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, CAS, Guangzhou 510640, PR China<p>While the formation and evolution of nitrate in airborne particles are extensively investigated, little is known about the processing of nitrate in clouds. Here we present a detailed investigation on the in-cloud formation of nitrate, based on the size-resolved mixing state of nitrate in the individual cloud residual and cloud-free particles obtained by single particle mass spectrometry, and also the mass concentrations of nitrate in the cloud water and PM<span class="inline-formula"><sub>2.5</sub></span> at a mountain site (1690 m a.s.l. – above sea level) in southern China. The results show a significant enhancement of nitrate mass fraction and relative intensity of nitrate in the cloud water and the cloud residual particles, respectively, reflecting a critical role of in-cloud processing in the formation of nitrate. We first exclude the gas-phase scavenging of HNO<span class="inline-formula"><sub>3</sub></span> and the facilitated activation of nitrate-containing particles as the major contribution for the enhanced nitrate, according to the size distribution of nitrate in individual particles. Based on regression analysis and theoretical calculations, we then highlight the role of N<span class="inline-formula"><sub>2</sub></span>O<span class="inline-formula"><sub>5</sub></span> hydrolysis in the in-cloud formation of nitrate, even during the daytime, attributed to the diminished light in clouds. Nitrate is highly related (<span class="inline-formula"><i>R</i><sup>2</sup>=</span> <span class="inline-formula">∼</span> 0.6) to the variations in [NO<span class="inline-formula"><sub><i>x</i></sub></span>][O<span class="inline-formula"><sub>3</sub></span>], temperature, and droplet surface area in clouds. Accounting for droplet surface area greatly enhances the predictability of the observed nitrate, compared with using [NO<span class="inline-formula"><sub><i>x</i></sub></span>][O<span class="inline-formula"><sub>3</sub></span>] and temperature. The substantial contribution of N<span class="inline-formula"><sub>2</sub></span>O<span class="inline-formula"><sub>5</sub></span> hydrolysis to nitrate in clouds with diminished light during the daytime can be reproduced by a multiphase chemical box model. Assuming a photolysis rate at 30 % of the default setting, the overall contribution of N<span class="inline-formula"><sub>2</sub></span>O<span class="inline-formula"><sub>5</sub></span> hydrolysis pathway to nitrate formation increases by <span class="inline-formula">∼</span> 20 % in clouds. Given that N<span class="inline-formula"><sub>2</sub></span>O<span class="inline-formula"><sub>5</sub></span> hydrolysis acts as a major sink of NO<span class="inline-formula"><sub><i>x</i></sub></span> in the atmosphere, further model updates would improve our understanding about the processes contributing to nitrate production in cloud and the cycling of odd nitrogen.</p>https://acp.copernicus.org/articles/22/9571/2022/acp-22-9571-2022.pdf |
| spellingShingle | G. Zhang G. Zhang G. Zhang X. Hu X. Hu X. Hu W. Sun W. Sun W. Sun Y. Yang Y. Yang Z. Guo Z. Guo Z. Guo Y. Fu Y. Fu H. Wang S. Zhou L. Li M. Tang M. Tang M. Tang Z. Shi D. Chen X. Bi X. Bi X. Bi X. Wang X. Wang X. Wang A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water Atmospheric Chemistry and Physics |
| title | A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water |
| title_full | A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water |
| title_fullStr | A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water |
| title_full_unstemmed | A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water |
| title_short | A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water |
| title_sort | comprehensive study about the in cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water |
| url | https://acp.copernicus.org/articles/22/9571/2022/acp-22-9571-2022.pdf |
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