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DOI	10.1016/j.atmosenv.2021.118871
	Barrierless HNO3 formation from the hydrolysis reaction of NO2 with Cl atom in the atmosphere
	Zhao X.; Teng Z.; Wang J.; Ma X.; Sun Y.; Gao R.; Xu F.; Zhang Q.; Wang W.
发表日期	2021
ISSN	1352-2310
英文摘要	Nitric acid (HNO3) is one of the main pollutants in the atmosphere and has an important effect on the air pollution. However, the formation pathways of HNO3 are still poorly understood in the marine boundary layer (MBL). Here, we show evidence of the formation of HNO3 from chlorine (Cl) radical and nitrogen dioxide (NO2), with 1–3 water molecules, as well as on the air-water interface, based on the direct Born-Oppenheimer molecular dynamics (BOMD) simulation. The relative free energy change along the reaction coordinates for the (Cl)(NO2)(H2O)1 (monohydrate) system was calculated using thermodynamic integration, revealing that the monohydrate system exhibited no free energy barrier and was 26.5 kcal mol−1 exergonic. This suggests that the formation of HNO3 from the monohydrate system is thermodynamically favorable. For all the systems studied, the formation of HNO3 was directly observed using BOMD simulations, and only one water molecule participates in the reaction. However, loop structures, which were expected to be ubiquitous on the air-water interface, were not observed. This study identifies the importance of the reactions of Cl atom, NO2, and water molecules in the formation of HNO3 in the MBL region. © 2021
关键词	Ab initio molecular dynamics Chlorine radical Nitric acid Nitrogen dioxide Thermodynamic integration
语种	英语
scopus关键词	Air; Boundary layers; Free energy; Molecular dynamics; Molecules; Nitrogen oxides; Phase interfaces; Reaction kinetics; Ab initio molecular dynamics; Air/Water Interfaces; Born-Oppenheimer molecular dynamics; Chlorine atom; Chlorine radicals; Formation pathways; Hydrolysis reaction; Marine boundary layers; Thermodynamic integration; Water molecule; Nitric acid
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/248775
作者单位	Environment Research Institute, Shandong University, Qingdao, 266237, China; College of Environment and Safety Engineering, Qingdao University of Science & Technology, Qingdao, 266042, China; State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China
推荐引用方式 GB/T 7714	Zhao X.,Teng Z.,Wang J.,et al. Barrierless HNO3 formation from the hydrolysis reaction of NO2 with Cl atom in the atmosphere[J],2021.
APA	Zhao X..,Teng Z..,Wang J..,Ma X..,Sun Y..,...&Wang W..(2021).Barrierless HNO3 formation from the hydrolysis reaction of NO2 with Cl atom in the atmosphere.ATMOSPHERIC ENVIRONMENT.
MLA	Zhao X.,et al."Barrierless HNO3 formation from the hydrolysis reaction of NO2 with Cl atom in the atmosphere".ATMOSPHERIC ENVIRONMENT (2021).