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DOI	10.1016/j.atmosenv.2020.118068
	Theoretical insight into the oxidation mechanism of NO2 and SO2 on TiO2 surface: The role of H2O, NH3 and SO42-
	Wang Z.; Zhang C.; Lv G.; Sun X.
发表日期	2021
ISSN	1352-2310
卷号	246
英文摘要	In this paper, density-functional theory (DFT) was employed to investigate the reaction mechanism of SO2 and NO2 and the important role of intermediate N2O4 formation. In addition, the effect of pure particulate surface (TiO2) and particulate surface containing other atmospheric components (H2O, NH3 and SO42−) on the conversion of SO2 and NO2 to sulfate also was analyzed. The detailed information that intermediate N2O4 acts as the oxidant was demonstrated in this oxidation reaction of SO2 and NO2 (as a rate-determining step). The pure particulate surface (TiO2) has hardly effect on the oxidation process of SO2 and N2O4. Whereas, different amounts of H2O and NH3 molecules as well as SO42−, contained on the particulate surface, can effectively reduce the activation energy of oxidation step. And, the optimal process is that SO2 is oxidized by cis-ONONO2 with the energy barrier of 4.54 kcal/mol when one NH3 molecule and one H2O molecule are contained on the TiO2(101) surface. When more H2O molecules are contained on particulate surface, SO2 tends to form HSO3− first. However, HSO3− is more difficult to be further oxidized by asy-ONONO2 than SO2. This study gains more insight into the contribution of SO2 and NO2 to haze and the potential impact of atmospheric constituents (including H2O/NH3/TiO2 and SO42−/TiO2) on the formation sulfate. © 2020 Elsevier Ltd
关键词	Density functional theory NO2 Particulate surface SO2 Sulfate
语种	英语
scopus关键词	Activation energy; Ammonia; Density functional theory; Molecules; Nitrogen oxides; Oxidation; Oxide minerals; Particles (particulate matter); Sulfur dioxide; Titanium dioxide; Atmospheric components; Atmospheric constituents; Oxidation mechanisms; Oxidation process; Oxidation reactions; Potential impacts; Rate determining step; Reaction mechanism; Reaction intermediates; ammonia; nitrogen dioxide; sulfate; sulfur dioxide; titanium dioxide; water; atmospheric chemistry; chemical alteration; molecular analysis; nitrogen dioxide; oxidation; particulate matter; sulfate; titanium; adsorption; air pollution; computer model; controlled study; density functional theory; dimerization; energy; geometry; hybridization; oxidation; priority journal; surface property; theoretical study
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/248715
作者单位	Environment Research Institute, Shandong University, Qingdao, 266237, China; College of Biological and Environmental Engineering, Binzhou University, Binzhou, 256600, China
推荐引用方式 GB/T 7714	Wang Z.,Zhang C.,Lv G.,et al. Theoretical insight into the oxidation mechanism of NO2 and SO2 on TiO2 surface: The role of H2O, NH3 and SO42-[J],2021,246.
APA	Wang Z.,Zhang C.,Lv G.,&Sun X..(2021).Theoretical insight into the oxidation mechanism of NO2 and SO2 on TiO2 surface: The role of H2O, NH3 and SO42-.ATMOSPHERIC ENVIRONMENT,246.
MLA	Wang Z.,et al."Theoretical insight into the oxidation mechanism of NO2 and SO2 on TiO2 surface: The role of H2O, NH3 and SO42-".ATMOSPHERIC ENVIRONMENT 246(2021).