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DOI	10.1016/j.atmosenv.2021.118392
	Gaseous and heterogeneous reactions on the mechanisms and kinetics of acrolein with ozone
	Wang N.; Sun J.; Wei B.; Mei Q.; An Z.; Wei F.; Li M.; Qiu Z.; Bo X.; Xie J.; Zhan J.; He M.
发表日期	2021
ISSN	1352-2310
卷号	254
英文摘要	In this paper, the gas-phase and heterogeneous reactions of acrolein with ozone were studied comprehensively and deeply. Acrolein is one of the simplest unsaturated aldehydes found widely in the fuel combustion and industrial emissions. Mineral particles produced by frequent sandstorms have important effects on the tropospheric chemistry and the climate change. The content of silica in clay minerals is rich, thus three kinds of clusters (the monomeric model Si(OH)4, the linear model Si3O2(OH)8 and the cyclic hexamer model Si6O6(OH)12) were selected for the heterogeneous study. The reaction rate constant of acrolein with ozone at 298 K and 1 atm was 7.46 × 10−18 cm3 molecule−1 s−1, which was in agreement with the experimental value. SiO2 clusters interacted with acrolein via the hydrogen bonds and had good adsorption properties. The hydrogen bond between the oxygen of aldehyde group on acrolein and the hydrogen of silica surface was stronger and the adsorption energy was greater. The adsorption of silanol groups did not change the ozonation mechanism of acrolein, but had effects on the reaction rate. Among them, three silanol groups acted as positive catalysts. The kinetic data within the temperature range of 216.65–288.15 K corresponding to the height of the troposphere at 0–11 km showed that the rate constant of O3-initiated reaction of acrolein is positively correlated with the temperature. In addition, we also studied the reaction mechanism and kinetic of the Criegee intermediates reacting with atmospheric small molecules and isomerization process in gas-phase and heterogeneous processes. © 2021 Elsevier Ltd
关键词	Acrolein DFT theoretical Calculation Gas-phase reactions Heterogeneous chemistry O3-initiated
语种	英语
scopus关键词	Adsorption; Amides; Climate change; Gases; Herbicides; Hydrogen bonds; Isomerization; Kinetics; Ozone; Ozonization; Phase interfaces; Rate constants; Reaction intermediates; Silica; Gas-phase reactions; Heterogeneous chemistry; Heterogeneous reactions; Mechanism and kinetics; O3-initiated; OH$+-$; Silanol groups; Simple++; Theoretical calculations; Unsaturated aldehydes; Aldehydes; acrolein; aldehyde; hydrogen; oxygen; ozone; silicate; adsorption; aldehyde; chemical reaction; ozone; reaction kinetics; silica; adsorption; air pollution; Article; atmospheric particulate matter; calculation; chemical reaction; combustion; density functional theory; gas; hydrogen bond; isomerization; ozonation; ozonolysis; priority journal; quantum chemistry; rate constant; reaction analysis; thermodynamics; troposphere
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/248452
作者单位	Environment Research Institute, Shandong University, Qingdao, 266237, China; School of Environmental and Materials Engineering, Yantai University, Yantai, 264005, China; Assets and Laboratory Management Office, Shandong University, Qingdao, 266237, China; School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002, China; Key Laboratary for Colloid & Interface Chemistry of Education Ministry, Department of Chemistry, Shandong University, Jinan, 250100, China
推荐引用方式 GB/T 7714	Wang N.,Sun J.,Wei B.,et al. Gaseous and heterogeneous reactions on the mechanisms and kinetics of acrolein with ozone[J],2021,254.
APA	Wang N..,Sun J..,Wei B..,Mei Q..,An Z..,...&He M..(2021).Gaseous and heterogeneous reactions on the mechanisms and kinetics of acrolein with ozone.ATMOSPHERIC ENVIRONMENT,254.
MLA	Wang N.,et al."Gaseous and heterogeneous reactions on the mechanisms and kinetics of acrolein with ozone".ATMOSPHERIC ENVIRONMENT 254(2021).