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DOI	10.5194/acp-22-11323-2022
	Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical
	Guo, Yindong; Shen, Hongru; Pullinen, Iida; Luo, Hao; Kang, Sungah; Vereecken, Luc; Fuchs, Hendrik; Hallquist, Mattias; Acir, Ismail-Hakki; Tillmann, Ralf; Rohrer, Franz; Wildt, Jurgen; Kiendler-Scharr, Astrid; Wahner, Andreas; Zhao, Defeng; Mentel, Thomas F.
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	11323
结束页码	11346
卷号	22 期号:17 页码:24
英文摘要	Nighttime NO3-initiated oxidation of biogenic volatile organic compounds (BVOCs) such as monoterpenes is important for the atmospheric formation and growth of secondary organic aerosol (SOA), which has significant impact on climate, air quality, and human health. In such SOA formation and growth, highly oxygenated organic molecules (HOM) may be crucial, but their formation pathways and role in aerosol formation have yet to be clarified. Among monoterpenes, limonene is of particular interest for its high emission globally and high SOA yield. In this work, HOM formation in the reaction of limonene with nitrate radical (NO3) was investigated in the SAPHIR chamber (Simulation of Atmospheric PHotochemistry In a large Reaction chamber). About 280 HOM products were identified, grouped into 19 monomer families, 11 dimer families, and 3 trimer families. Both closed-shell products and open-shell peroxy radicals (RO2 center dot) 2 were observed, and many of them have not been reported previously. Monomers and dimers accounted for 47% and 47% of HOM concentrations, respectively, with trimers making up the remaining 6 %. In the most abundant monomer families, C10H15-17NO6-14, carbonyl products outnumbered hydroxyl products, indicating the importance of RO2 center dot termination by unimolecular dissociation. Both RO2 center dot autoxidation and alkoxy-peroxy pathways were found to be important processes leading to HOM. Time-dependent concentration profiles of monomer products containing nitrogen showed mainly second-generation formation patterns. Dimers were likely formed via the accretion reaction of two monomer RO2 center dot , and HOM-trimers via the accretion reaction between monomer RO2 center dot and dimer RO2 center dot. Trimers are suggested to play an important role in new particle formation (NPF) observed in our experiment. A HOM yield of 1.5%(+1.7%)(-0.7%) was estimated considering only first-generation products. SOA mass growth could be reasonably explained by HOM condensation on particles assuming irreversible uptake of ultra-low volatility organic compounds (ULVOCs), extremely low volatility organic compounds (ELVOCs), and low volatility organic compounds (LVOCs). This work provides evidence for the important role of HOM formed via the limonene +NO3 reaction in NPF and growth of SOA particles.
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:000848882400001
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/273460
作者单位	Fudan University; Fudan University; Helmholtz Association; Research Center Julich; Fudan University; University of Gothenburg; Fudan University; University of Eastern Finland; University of Bonn
推荐引用方式 GB/T 7714	Guo, Yindong,Shen, Hongru,Pullinen, Iida,et al. Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical[J],2022,22(17):24.
APA	Guo, Yindong.,Shen, Hongru.,Pullinen, Iida.,Luo, Hao.,Kang, Sungah.,...&Mentel, Thomas F..(2022).Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(17),24.
MLA	Guo, Yindong,et al."Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.17(2022):24.