气候变化领域集成服务门户(CCPortal): Hydroxyl radical-initiated aging of particulate squalane

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DOI	10.1016/j.atmosenv.2020.117663
	Hydroxyl radical-initiated aging of particulate squalane
	Zhang B.; Hu X.; Yao L.; Wang M.; Yang G.; Lu Y.; Liu Y.; Wang L.
发表日期	2020
ISSN	1352-2310
卷号	237
英文摘要	Heterogeneous aging of organic aerosols can significantly alter their physicochemical properties and thus their impacts on the radiative balance of the earth system. In this study, kinetics and mechanisms of heterogeneous reactions between suspended squalane particles and hydroxyl (OH) radicals were investigated using a self-made photooxidation flow tube and a high-resolution long time-of-flight chemical ionization mass spectrometer equipped with a Filter Inlet for Gases and AEROsols (FIGAERO-HR-LToF-CIMS). In addition to the measurements of the heterogeneous reaction rate constants for squalane and its multi-generation functionalization products whose carbon backbone are retaining, identification and semi-quantification of functionalization and fragmentation products from OH radical-initiated aging of squalane were carried out, which were utilized to develop a plausible reaction scheme. Our results show that the heterogeneous oxidation mechanism for particulate squalane is similar to those for OH radical initiated-oxidation of gaseous alkanes, but intermolecular hydrogen abstraction, in addition to reactions with O2, isomerization, and decomposition, could be an important heterogeneous reaction pathway for alkoxy radicals, leading to the formation of functionalization products of alcohols. The relative abundances of fragmentation products suggest that OH radicals preferably attack the tertiary carbon. The evolution of products indicates that functionalization plays a leading role in the early stage of the reaction and the fragmentation products become more and more important with increased OH exposure. Our study depicts heterogeneous reaction pathways of organic aerosols with OH radicals at the molecular level, and helps to better understand the chemical evolution of complex organic aerosols in the atmosphere. © 2020 Elsevier Ltd
关键词	Fragmentation products Functionalization products Hydroxyl radical Kinetics Reaction pathway Squalane
语种	英语
scopus关键词	Aerosols; Atmospheric movements; Carbon; Free radicals; Ionization of gases; Isomerization; Photooxidation; Physicochemical properties; Rate constants; Chemical evolution; Chemical ionization; Functionalizations; Heterogeneous oxidation; Heterogeneous reactions; Intermolecular hydrogen; Kinetics and mechanism; Relative abundance; Particles (particulate matter); alkane; carbon; hydroxyl radical; oxygen; squalane; unclassified drug; aging; decomposition; fragmentation; heterogeneity; hydrogen; hydroxyl radical; molecular analysis; organic compound; oxidation; physicochemical property; reaction kinetics; suspended load; aerosol; Article; atmosphere; decomposition; fragmentation reaction; gas evolution; isomerization; kinetics; particulate matter; photooxidation; physical chemistry; priority journal; time of flight mass spectrometry
来源期刊	ATMOSPHERIC ENVIRONMENT
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/249057
作者单位	Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University, Shanghai, 200438, China; Collaborative Innovation Center of Climate Change, Nanjing, 210023, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, China
推荐引用方式 GB/T 7714	Zhang B.,Hu X.,Yao L.,et al. Hydroxyl radical-initiated aging of particulate squalane[J],2020,237.
APA	Zhang B..,Hu X..,Yao L..,Wang M..,Yang G..,...&Wang L..(2020).Hydroxyl radical-initiated aging of particulate squalane.ATMOSPHERIC ENVIRONMENT,237.
MLA	Zhang B.,et al."Hydroxyl radical-initiated aging of particulate squalane".ATMOSPHERIC ENVIRONMENT 237(2020).