气候变化领域集成服务门户(CCPortal): Trifluoroacetaldehyde aminolysis catalyzed by a single water molecule: An important sink pathway for trifluoroacetaldehyde and a potential pathway for secondary organic aerosol growth

CCPortal

DOI	10.1016/j.atmosenv.2021.118242
	Trifluoroacetaldehyde aminolysis catalyzed by a single water molecule: An important sink pathway for trifluoroacetaldehyde and a potential pathway for secondary organic aerosol growth
	Dong Z.-G.; Xu F.; Mitchell E.; Long B.
发表日期	2021
ISSN	1352-2310
卷号	249
英文摘要	High-level ab initio calculations and variational transition state theory with small curvature tunneling have been used to study the aminolysis of trifluoroacetaldehyde catalyzed by a single water molecule. The results of energetic studies indicate that the energy barrier of the trifluoroacetaldehyde aminolysis reaction decreases along ammonia, methylamine, and dimethylamine. A single water molecule can significantly reduce the reaction energy barrier of trifluoroacetaldehyde aminolysis. In particular, the reaction involving dimethylamine has the lowest reaction energy barrier and the energy barrier is decreased to be −9.69 kcal/mol in the CF3CHO + (CH3)2NH + H2O reaction relative to CF3CHO, (CH3)2NH, and H2O separated reactants. Kinetic calculation shows that the rate coefficient of CF3CHO + (CH3)2NH⋯H2O ranges from 7.78 × 10−13 to 4.45 × 10−16 cm3⋅molecules−1⋅s−1 at 190–350 K. Here, we find an important CF3CHO elimination pathway, which can compete with the reaction of CF3CHO + OH when the OH concentration is 104 molecules⋅cm−3 and the dimethylamine concentration is higher than 109 molecules⋅cm−3 in the temperature range between 240 and 330 K. In addition, once (CH3)2NCH(OH)CF3 is formed by the reaction of CF3CHO + (CH3)2NH + H2O, it will further promote the growth of secondary organic aerosols. © 2021 Elsevier Ltd
关键词	Aminolysis Reaction kinetics Reaction mechanisms Trifluoroacetaldehyde
语种	英语
scopus关键词	Aerosols; Amination; Ammonia; Calculations; Catalysis; Electronic states; Energy barriers; Aminolysis reaction; High-level ab initio calculations; Kinetic calculations; Reaction energy barriers; Secondary organic aerosols; Small-curvature tunneling; Trifluoroacetaldehyde; Variational transition state theory; Molecules; acetaldehyde; ammonia; dimethylamine; methylamine; water; aerosol; catalysis; catalyst; chemical compound; chemical reaction; concentration (composition); molecular analysis; reaction kinetics; aminolysis; Article; catalysis; chemical reaction kinetics; concentration (parameter); controlled study; energy; growth; priority journal; reduction (chemistry); secondary organic aerosol; temperature
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/248552
作者单位	School of Materials Science and Engineering, Guizhou Minzu University, Guiyang, 550025, China; Department of Chemistry, Bridgewater College, BridgewaterVA 22812, United States; Special and Key Laboratory for Development and Utilization of Guizhou Superior Bio-based Materials (Wood,Bamboo,Tea,etc.), Guiyang, 550025, China
推荐引用方式 GB/T 7714	Dong Z.-G.,Xu F.,Mitchell E.,et al. Trifluoroacetaldehyde aminolysis catalyzed by a single water molecule: An important sink pathway for trifluoroacetaldehyde and a potential pathway for secondary organic aerosol growth[J],2021,249.
APA	Dong Z.-G.,Xu F.,Mitchell E.,&Long B..(2021).Trifluoroacetaldehyde aminolysis catalyzed by a single water molecule: An important sink pathway for trifluoroacetaldehyde and a potential pathway for secondary organic aerosol growth.ATMOSPHERIC ENVIRONMENT,249.
MLA	Dong Z.-G.,et al."Trifluoroacetaldehyde aminolysis catalyzed by a single water molecule: An important sink pathway for trifluoroacetaldehyde and a potential pathway for secondary organic aerosol growth".ATMOSPHERIC ENVIRONMENT 249(2021).