Role of Water Molecule in the Gas-Phase Formation Process of Nitrated Polycyclic Aromatic Hydrocarbons in the Atmosphere: A Computational Study

CORC > 生态环境研究中心 > 中国科学院生态环境研究中心 > 环境化学与生态毒理学国家重点实验室

	Role of Water Molecule in the Gas-Phase Formation Process of Nitrated Polycyclic Aromatic Hydrocarbons in the Atmosphere: A Computational Study
	Zhang, Qingzhu ; Gao, Rui ; Xu, Fei ; Zhou, Qin ; Jiang, Guibin ; Wang, Tao ; Chen, Jianmin ; Hu, Jingtian ; Jiang, Wei ; Wang, Wenxing
刊名	ENVIRONMENTAL SCIENCE & TECHNOLOGY
	2014
卷号	48 期号:9 页码:5051-5057
ISSN号	0013-936X
中文摘要	Nitro-PAHs are globally worrisome air pollutants because their high direct-acting mutagenicity and carcinogenicity. A mechanistic understanding of their formation is of crucial importance for successful prevention of their atmospheric pollution. Here, the formation of nitro-PAHs arising from the OH-initiated and NO3-initiated atmospheric reactions of PAHs was investigated by using quantum chemical calculations. It is widely assumed that OH or NO3 radicals attack on the C atoms of the aromatic rings in the PAH molecule, followed by the addition of NO2 to the OH-PAH or NO3-PAH adducts at the ortho position and the loss of water or nitric acid to form nitro-PAHs. However, calculations show that the direct loss of water from the OH-NO2-PAH adducts via the unimolecular decomposition is energetically unfavorable. This study reveals for the first time that water molecule plays an important catalytic effect on the loss of water from the OH-NO2-PAH adducts and promotes the formation of nitro-PAHs. In addition, the introduction of water unwraps new formation pathway through the addition of NO2 to the OH-PAH or NO3-PAH adduct at the para position. The individual and overall rate constants for the addition reactions of PAHs with OH and NO3 radicals were deduced by using the Rice-Ramsperger-Kassel-Marcus (RRKM) theory.
WOS记录号	WOS:000335720100050
公开日期	2015-03-24
内容类型	期刊论文
源URL	[http://ir.rcees.ac.cn/handle/311016/9449]
专题	生态环境研究中心_环境化学与生态毒理学国家重点实验室
推荐引用方式 GB/T 7714	Zhang, Qingzhu,Gao, Rui,Xu, Fei,et al. Role of Water Molecule in the Gas-Phase Formation Process of Nitrated Polycyclic Aromatic Hydrocarbons in the Atmosphere: A Computational Study[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2014,48(9):5051-5057.
APA	Zhang, Qingzhu.,Gao, Rui.,Xu, Fei.,Zhou, Qin.,Jiang, Guibin.,...&Wang, Wenxing.(2014).Role of Water Molecule in the Gas-Phase Formation Process of Nitrated Polycyclic Aromatic Hydrocarbons in the Atmosphere: A Computational Study.ENVIRONMENTAL SCIENCE & TECHNOLOGY,48(9),5051-5057.
MLA	Zhang, Qingzhu,et al."Role of Water Molecule in the Gas-Phase Formation Process of Nitrated Polycyclic Aromatic Hydrocarbons in the Atmosphere: A Computational Study".ENVIRONMENTAL SCIENCE & TECHNOLOGY 48.9(2014):5051-5057.