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DOI	10.5194/acp-22-6001-2022
	Kinetics, SOA yields, and chemical composition of seconaary organic aerosol from beta-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K
	Gao, Linyu; Song, Junwei; Mohr, Claudia; Huang, Wei; Vallon, Magdalena; Jiang, Feng; Leisner, Thomas; Saathoff, Harald
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	6001
结束页码	6020
卷号	22 期号:9 页码:20
英文摘要	beta-caryophyllene (BCP) is one of the most important sesquiterpenes (SQTs) in the atmosphere, with a large potential contribution to secondary organic aerosol (SOA) formation mainly from reactions with ozone (O-3) and nitrate radicals (NO3). In this work, we study the temperature dependence of the kinetics of BCP ozonolysis, SOA yields, and SOA chemical composition in the dark and in the absence and presence of nitrogen oxides including nitrate radicals (NO3). We cover a temperature range of 213-313 K, representative of tropospheric conditions. The oxidized components in both gas and particle phases were characterized on a molecular level by a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols using iodide as the reagent ion (FIGAERO-iodide-CIMS). The batch mode experiments were conducted in the 84.5 m(3) aluminium simulation chamber AIDA at the Karlsruhe Institute of Technology (KIT). In the absence of nitrogen oxides, the temperature-dependent rate coefficient of the endocyclic double bond in BCP reacting with ozone between 243-313 K is negatively correlated with temperature, corresponding to the following Arrhenius equation: k = (1.6 +/- 0.4) x 10(-15) x exp((559 +/- 97)/ T). The SOA yields increase from 16 +/- 5 % to 37 +/- 11 %, with temperatures decreasing from 313 to 243 K at a total organic particle mass of 10 mu g m(-3). The variation in the ozonolysis temperature leads to a substantial impact on the abundance of individual organic molecules. In the absence of nitrogen oxides, monomers C14-15H22-24O3-7 (37.4 %), dimers C28-30H44-48O5-9 (53.7 %), and timers C41_44H62_6609_11 (8.6 %) are abundant in the particle phase at 213 K. At 313 K, we observed more oxidized monomers (mainly C14-15H22-24O6-9, 67.5 %) and dimers (mainly C27-29H42-44O9-11, 27.6 %), including highly oxidized molecules (HOMs; C14H22O7,9C15H22O7,9C15H24O7,9), which can be formed via hydrogen shift mechanisms, but no significant timers. In the presence of nitrogen oxides, the organonitrate fraction increased from 3 % at 213 K to 12 % and 49 % at 243 and 313 K, respectively. Most of the organonitrates were monomers with Cis skeletons and only one nitrate group. More highly oxygenated organonitrates were observed at higher temperatures, with their signal-weighted O : C atomic ratio increasing from 0.41 to 0.51 from 213 to 313 K. New dimeric and timeric organic species without nitrogen atoms (C-20, C-35) were formed in the presence of nitrogen oxides at 298-313 K, indicating potential new reaction pathways. Overall, our results show that increasing temperatures lead to a relatively small decrease in the rate coefficient of the endocyclic double bond in BCP reacting with ozone but to a strong decrease in SOA yields. In contrast, the formation of HOMs and organonitrates increases significantly with temperature.
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:000791462500001
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/273468
作者单位	Helmholtz Association; Karlsruhe Institute of Technology; Helmholtz Association; Karlsruhe Institute of Technology; Stockholm University; University of Helsinki; Ruprecht Karls University Heidelberg
推荐引用方式 GB/T 7714	Gao, Linyu,Song, Junwei,Mohr, Claudia,et al. Kinetics, SOA yields, and chemical composition of seconaary organic aerosol from beta-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K[J],2022,22(9):20.
APA	Gao, Linyu.,Song, Junwei.,Mohr, Claudia.,Huang, Wei.,Vallon, Magdalena.,...&Saathoff, Harald.(2022).Kinetics, SOA yields, and chemical composition of seconaary organic aerosol from beta-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(9),20.
MLA	Gao, Linyu,et al."Kinetics, SOA yields, and chemical composition of seconaary organic aerosol from beta-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.9(2022):20.