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DOI | 10.5194/acp-21-8809-2021 |
Revisiting the reaction of dicarbonyls in aerosol proxy solutions containing ammonia: The case of butenedial | |
Hensley J.C.; Birdsall A.W.; Valtierra G.; Cox J.L.; Keutsch F.N. | |
发表日期 | 2021 |
ISSN | 1680-7316 |
起始页码 | 8809 |
结束页码 | 8821 |
卷号 | 21期号:11 |
英文摘要 | Reactions in aqueous solutions containing dicarbonyls (especially the -dicarbonyls methylglyoxal, glyoxal, and biacetyl) and reduced nitrogen (NHx ) have been studied extensively. It has been proposed that accretion reactions from dicarbonyls and NHx could be a source of particulate matter and brown carbon in the atmosphere and therefore have direct implications for human health and climate. Other dicarbonyls, such as the 1,4-unsaturated dialdehyde butenedial, are also produced from the atmospheric oxidation of volatile organic compounds, especially aromatics and furans, but their aqueous-phase reactions with NHx have not been characterized. In this work, we determine a pH-dependent mechanism of butenedial reactions in aqueous solutions with NHx that is compared to -dicarbonyls, in particular the dialdehyde glyoxal. Similar to glyoxal, butenedial is strongly hydrated in aqueous solutions. Butenedial reaction with NHx also produces nitrogen-containing rings and leads to accretion reactions that form brown carbon. Despite glyoxal and butenedial both being dialdehydes, butenedial is observed to have three significant differences in its chemical behavior: (1) as previously shown, butenedial does not substantially form acetal oligomers, (2) the butenedial/OH reaction leads to light-absorbing compounds, and (3) the butenedial/NHx reaction is fast and first order in the dialdehyde. Building off of a complementary study on butenedial gas-particle partitioning, we suggest that the behavior of other reactive dialdehydes and dicarbonyls may not always be adequately predicted by dicarbonyls, even though their dominant functionalities are closely related. The carbon skeleton (e.g., its hydrophobicity, length, and bond structure) also governs the fate and climate-relevant properties of dicarbonyls in the atmosphere. If other dicarbonyls behave like butenedial, their reaction with NHx could constitute a regional source of brown carbon to the atmosphere. © 2021 Copernicus GmbH. All rights reserved. |
语种 | 英语 |
scopus关键词 | aerosol; ammonia; aqueous solution; brown carbon; concentration (composition); particulate matter; source apportionment; volatile organic compound |
来源期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/246824 |
作者单位 | School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, United States; Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, United States; Harvard College, Cambridge, MA, United States; Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, United States; Goodyear, Akron, OH, United States |
推荐引用方式 GB/T 7714 | Hensley J.C.,Birdsall A.W.,Valtierra G.,et al. Revisiting the reaction of dicarbonyls in aerosol proxy solutions containing ammonia: The case of butenedial[J],2021,21(11). |
APA | Hensley J.C.,Birdsall A.W.,Valtierra G.,Cox J.L.,&Keutsch F.N..(2021).Revisiting the reaction of dicarbonyls in aerosol proxy solutions containing ammonia: The case of butenedial.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(11). |
MLA | Hensley J.C.,et al."Revisiting the reaction of dicarbonyls in aerosol proxy solutions containing ammonia: The case of butenedial".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.11(2021). |
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