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DOI | 10.5194/acp-22-1467-2022 |
Secondary organic aerosol and organic nitrogen yields from the nitrate radical (NO3) oxidation of alpha-pinene from various RO2 fates | |
Bates, Kelvin H.; Burke, Guy J. P.; Cope, James D.; Nguyen, Tran B. | |
发表日期 | 2022 |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
起始页码 | 1467 |
结束页码 | 1482 |
卷号 | 22期号:2页码:16 |
英文摘要 | The reaction of alpha-pinene with NO3 is an important sink of both alpha-pinene and NO3 at night in regions with mixed biogenic and anthropogenic emissions; however, there is debate on its importance for secondary organic aerosol (SOA) and reactive nitrogen budgets in the atmosphere. Previous experimental studies have generally observed low or zero SOA formation, often due to excessive [NO3] conditions. Here, we characterize the SOA and organic nitrogen formation from alpha-pinene + NO3 as a function of nitrooxy peroxy (nRO(2)) radical fates with HO2, NO, NO3, and RO2 in an atmospheric chamber. We show that SOA yields are not small when the nRO(2) fate distribution in the chamber mimics that in the atmosphere, and the formation of pinene nitrooxy hydroperoxide (PNP) and related organonitrates in the ambient atmosphere can be reproduced. Nearly all SOA from alpha-pinene + NO3 chemistry derives from the nRO(2)+ RO2 pathway, which alone has an SOA mass yield of 56 (+/- 7) %. Molecular composition analysis shows that particulate nitrates are a large (60 %-70 %) portion of the SOA and that dimer formation is the primary mechanism of SOA production from alpha-pinene + NO3 under simulated nighttime conditions. Synergistic dimerization between nRO(2) and RO2 derived from ozonolysis and OH oxidation also contribute to SOA formation and should be considered in models. We report a 58 (+/- 20) % molar yield of PNP from the nRO(2)+ HO2 pathway. Applying these laboratory constraints to model simulations of summertime conditions observed in the southeast United States (where 80 % of alpha-pinene is lost via NO3 oxidation, leading to 20 % nRO(2)+ RO2 and 45 % nRO(2)+ HO2), we estimate yields of 11 % SOA and 7 % particulate nitrate by mass and 26 % PNP by mole from alpha-pinene + NO3 in the ambient atmosphere. These results suggest that alpha-pinene + NO3 significantly contributes to the SOA budget and likely constitutes a major removal pathway of reactive nitrogen from the nighttime boundary layer in mixed biogenic-anthropogenic areas. |
学科领域 | Environmental Sciences; Meteorology & Atmospheric Sciences |
语种 | 英语 |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
WOS记录号 | WOS:000751424400001 |
来源期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/273867 |
作者单位 | University of California System; University of California Davis; Harvard University |
推荐引用方式 GB/T 7714 | Bates, Kelvin H.,Burke, Guy J. P.,Cope, James D.,et al. Secondary organic aerosol and organic nitrogen yields from the nitrate radical (NO3) oxidation of alpha-pinene from various RO2 fates[J],2022,22(2):16. |
APA | Bates, Kelvin H.,Burke, Guy J. P.,Cope, James D.,&Nguyen, Tran B..(2022).Secondary organic aerosol and organic nitrogen yields from the nitrate radical (NO3) oxidation of alpha-pinene from various RO2 fates.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(2),16. |
MLA | Bates, Kelvin H.,et al."Secondary organic aerosol and organic nitrogen yields from the nitrate radical (NO3) oxidation of alpha-pinene from various RO2 fates".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.2(2022):16. |
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