Youtian Zhang , Rongrong Han , Guanru Wu , Xinshuo Wang , Lei Li , Mei Li , Zhen Zhou , Jian Zhen Yu , Yang Zhou
{"title":"改进的单粒子气溶胶质谱仪估算海盐气溶胶中氯消耗的方法","authors":"Youtian Zhang , Rongrong Han , Guanru Wu , Xinshuo Wang , Lei Li , Mei Li , Zhen Zhou , Jian Zhen Yu , Yang Zhou","doi":"10.1016/j.atmosenv.2025.121243","DOIUrl":null,"url":null,"abstract":"<div><div>Chloride-containing aerosols significantly influence tropospheric chemistry and cloud microphysics. Sea salt aerosols (SSAs) are a major source of chlorine-containing aerosols in coastal regions. However, existing methods for estimating chlorine depletion using Single Particle Aerosol Mass Spectrometry (SPAMS) suffer from significant limitations. This study demonstrates that relying solely on [Cl]<sup>-</sup> signal at m/z = −35 and −37 to quantify chlorine content leads to substantial overestimation of chlorine depletion, particularly in fresh SSAs, where additional chlorine is contributed by [Na<sub>2</sub>Cl]<sup>+</sup> and [NaCl<sub>2</sub>]<sup>-</sup> ions. Using SPAMS data collected at a coastal site in Hong Kong during winter, spring and summer, we propose an improved methodology that accounts for all potential chlorine-depleting components. This improved method shows a better correlation with bulk observations, reducing the average estimated chlorine depletion from 98 ± 1 % to 57 ± 3 %, aligning closely with bulk results (49 ± 22 %). The new method significantly improves the refined analysis of chemical processes affecting chlorine depletion by precisely resolving size-dependent biases, organic acid, and NH<sub>3</sub> concentration-dependent dual roles. Seasonal analyses highlight the strong influence of dominant air masses, with winter exhibiting the highest depletion due to air masses originating from industrial inland/coastal regions, while summer shows minimal depletion under clean marine conditions. The improved method establishes a more reliable framework for quantifying chlorine depletion in individual SSAs, advancing mechanistic understanding of coastal chlorine cycling.</div></div>","PeriodicalId":250,"journal":{"name":"Atmospheric Environment","volume":"353 ","pages":"Article 121243"},"PeriodicalIF":4.2000,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Improved method for estimating chlorine depletion in sea salt aerosols using single particle aerosol mass spectrometer\",\"authors\":\"Youtian Zhang , Rongrong Han , Guanru Wu , Xinshuo Wang , Lei Li , Mei Li , Zhen Zhou , Jian Zhen Yu , Yang Zhou\",\"doi\":\"10.1016/j.atmosenv.2025.121243\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Chloride-containing aerosols significantly influence tropospheric chemistry and cloud microphysics. Sea salt aerosols (SSAs) are a major source of chlorine-containing aerosols in coastal regions. However, existing methods for estimating chlorine depletion using Single Particle Aerosol Mass Spectrometry (SPAMS) suffer from significant limitations. This study demonstrates that relying solely on [Cl]<sup>-</sup> signal at m/z = −35 and −37 to quantify chlorine content leads to substantial overestimation of chlorine depletion, particularly in fresh SSAs, where additional chlorine is contributed by [Na<sub>2</sub>Cl]<sup>+</sup> and [NaCl<sub>2</sub>]<sup>-</sup> ions. Using SPAMS data collected at a coastal site in Hong Kong during winter, spring and summer, we propose an improved methodology that accounts for all potential chlorine-depleting components. This improved method shows a better correlation with bulk observations, reducing the average estimated chlorine depletion from 98 ± 1 % to 57 ± 3 %, aligning closely with bulk results (49 ± 22 %). The new method significantly improves the refined analysis of chemical processes affecting chlorine depletion by precisely resolving size-dependent biases, organic acid, and NH<sub>3</sub> concentration-dependent dual roles. Seasonal analyses highlight the strong influence of dominant air masses, with winter exhibiting the highest depletion due to air masses originating from industrial inland/coastal regions, while summer shows minimal depletion under clean marine conditions. The improved method establishes a more reliable framework for quantifying chlorine depletion in individual SSAs, advancing mechanistic understanding of coastal chlorine cycling.</div></div>\",\"PeriodicalId\":250,\"journal\":{\"name\":\"Atmospheric Environment\",\"volume\":\"353 \",\"pages\":\"Article 121243\"},\"PeriodicalIF\":4.2000,\"publicationDate\":\"2025-04-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Atmospheric Environment\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1352231025002183\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Atmospheric Environment","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1352231025002183","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
Improved method for estimating chlorine depletion in sea salt aerosols using single particle aerosol mass spectrometer
Chloride-containing aerosols significantly influence tropospheric chemistry and cloud microphysics. Sea salt aerosols (SSAs) are a major source of chlorine-containing aerosols in coastal regions. However, existing methods for estimating chlorine depletion using Single Particle Aerosol Mass Spectrometry (SPAMS) suffer from significant limitations. This study demonstrates that relying solely on [Cl]- signal at m/z = −35 and −37 to quantify chlorine content leads to substantial overestimation of chlorine depletion, particularly in fresh SSAs, where additional chlorine is contributed by [Na2Cl]+ and [NaCl2]- ions. Using SPAMS data collected at a coastal site in Hong Kong during winter, spring and summer, we propose an improved methodology that accounts for all potential chlorine-depleting components. This improved method shows a better correlation with bulk observations, reducing the average estimated chlorine depletion from 98 ± 1 % to 57 ± 3 %, aligning closely with bulk results (49 ± 22 %). The new method significantly improves the refined analysis of chemical processes affecting chlorine depletion by precisely resolving size-dependent biases, organic acid, and NH3 concentration-dependent dual roles. Seasonal analyses highlight the strong influence of dominant air masses, with winter exhibiting the highest depletion due to air masses originating from industrial inland/coastal regions, while summer shows minimal depletion under clean marine conditions. The improved method establishes a more reliable framework for quantifying chlorine depletion in individual SSAs, advancing mechanistic understanding of coastal chlorine cycling.
期刊介绍:
Atmospheric Environment has an open access mirror journal Atmospheric Environment: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review.
Atmospheric Environment is the international journal for scientists in different disciplines related to atmospheric composition and its impacts. The journal publishes scientific articles with atmospheric relevance of emissions and depositions of gaseous and particulate compounds, chemical processes and physical effects in the atmosphere, as well as impacts of the changing atmospheric composition on human health, air quality, climate change, and ecosystems.