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DOI | 10.5194/acp-22-625-2022 |
Prediction of secondary organic aerosol from the multiphase reaction of gasoline vapor by using volatility-reactivity base lumping | |
Han, Sanghee; Jang, Myoseon | |
发表日期 | 2022 |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
起始页码 | 625 |
结束页码 | 639 |
卷号 | 22期号:1页码:15 |
英文摘要 | Heterogeneous chemistry of oxidized carbons in aerosol phase is known to significantly contribute to secondary organic aerosol (SOA) burdens. The UNIfied Partitioning Aerosol phase Reaction (UNIPAR) model was developed to process the multiphase chemistry of various oxygenated organics into SOA mass predictions in the presence of salted aqueous phase. In this study, the UNIPAR model simulated the SOA formation from gasoline fuel, which is a major contributor to the observed concentration of SOA in urban areas. The oxygenated products, predicted by the explicit mechanism, were lumped according to their volatility and reactivity and linked to stoichiometric coefficients which were dynamically constructed by predetermined mathematical equations at different NOx levels and degrees of gas aging. To improve the model feasibility in regional scales, the UNIPAR model was coupled with the Carbon Bond 6 (CB6r3) mechanism. CB6r3 estimated the hydrocarbon consumption and the concentration of radicals (i.e., RO2 and HO2) to process atmospheric aging of gas products. The organic species concentrations, estimated by stoichiometric coefficient array and the consumption of hydrocarbons, were applied to form gasoline SOA via multiphase partitioning and aerosol-phase reactions. To improve the gasoline SOA potential in ambient air, model parameters were also corrected for gas-wall partitioning (GWP). The simulated gasoline SOA mass was evaluated against observed data obtained in the University of Florida Atmospheric PHotochemical Outdoor Reactor (UF-APHOR) chamber under varying sunlight, NOx levels, aerosol acidity, humidity, temperature, and concentrations of aqueous salts and gasoline vapor. Overall, gasoline SOA was dominantly produced via aerosol-phase reaction, regardless of the seed conditions owing to heterogeneous reactions of reactive multifunctional organic products. Both the measured and simulated gasoline SOA was sensitive to seed conditions showing a significant increase in SOA mass with increasing aerosol acidity and water content. A considerable difference in SOA mass appeared between two inorganic aerosol states (dry aerosol vs. wet aerosol) suggesting a large difference in SOA formation potential between arid (western United States) and humid regions (eastern United States). Additionally, aqueous reactions of organic products increased the sensitivity of gasoline SOA formation to NOx levels as well as temperature. The impact of the chamber wall on SOA formation was generally significant, and it appeared to be higher in the absence of wet salts. Based on the evaluation of UNIPAR against chamber data from 10 aromatic hydrocarbons and gasoline fuel, we conclude that the UNIPAR model with both heterogeneous reactions and the model parameters corrected for GWP can improve the ability to accurately estimate SOA mass in regional scales. |
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:000746464200001 |
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/273627 |
作者单位 | State University System of Florida; University of Florida |
推荐引用方式 GB/T 7714 | Han, Sanghee,Jang, Myoseon. Prediction of secondary organic aerosol from the multiphase reaction of gasoline vapor by using volatility-reactivity base lumping[J],2022,22(1):15. |
APA | Han, Sanghee,&Jang, Myoseon.(2022).Prediction of secondary organic aerosol from the multiphase reaction of gasoline vapor by using volatility-reactivity base lumping.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(1),15. |
MLA | Han, Sanghee,et al."Prediction of secondary organic aerosol from the multiphase reaction of gasoline vapor by using volatility-reactivity base lumping".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.1(2022):15. |
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