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DOI	10.1016/j.atmosenv.2019.117161
	Formation mechanism of methanesulfonic acid and ammonia clusters: A kinetics simulation study
	Chen D.; Li D.; Wang C.; Liu F.; Wang W.
发表日期	2020
ISSN	1352-2310
卷号	222
英文摘要	The formation mechanism of methanesulfonic acid (MSA) and ammonia (NH3) clusters is investigated using density functional theory (DFT) and Atmospheric Cluster Dynamic Code (ACDC) in different conditions. The results suggest that hydrogen bonding and electrostatic interactions induced by proton transfer could provide the primary driving force that forms these clusters. NH3 can effectively promote the formation of MSA-based clusters at pptv levels, but high concentrations of precursors ([MSA] ≥ 2 × 107 molecules cm−3 and [NH3] ≥ 1 ppbv) is necessary for effective formation. The formation of the initial (MSA)2 dimer is a rate-determining step of cluster growth. The formation rate is proportional to the monomer concentration and inversely proportional to the temperature in the troposphere. Hydration has a great influence on the evaporation rate, formation rate, and nucleation mechanism of the MSA-NH3 system. The relative evaporation rate of all clusters is significantly affected by humidity, especially for the (MSA)(NH3) dimer. The evaporation rate of the (MSA)(NH3) dimer can be reduced by approximately a factor of 10−5 at a relative humidity (RH) ≥ 40%. The formation rate increases significantly with RH and reached up to a factor of 105 at RH = 100%. The formation of the initial (MSA)(NH3) dimer is the rate-determining step, which indicates that the nucleation mechanism is fundamentally different from anhydrous cases. In addition, the results showed that the formation of MSA-NH3 molecular clusters is relatively weak under typical atmospheric conditions. In addition to the high concentration of precursors and atmospheric humidity, the formation of MSA-based ternary clusters through the participation of other species such as SA that may be more important in promoting effective nucleation of MSA-NH3 system in the coastal atmosphere. © 2019 Elsevier Ltd
关键词	Evaporation rate Formation rate Growth pathway Hydration Methanesulfonic acid
语种	英语
scopus关键词	Atmospheric humidity; Crystallization; Density functional theory; Dimers; Evaporation; Hydration; Hydrogen bonds; Nucleation; Organic acids; Atmospheric conditions; Evaporation rate; Formation rates; Kinetics simulations; Methane sulfonic acid; Monomer concentration; Nucleation mechanism; Rate determining step; Ammonia; ammonia; dimer; mesylic acid; monomer; ammonia; chemical bonding; chemical compound; chemical reaction; concentration (composition); evaporation; formation mechanism; reaction kinetics; relative humidity; simulation; temperature effect; troposphere; density functional theory; evaporation; humidity; hydration; hydrogen bond; kinetics; priority journal; proton transport; simulation; static electricity; temperature; 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/249444
作者单位	Key Laboratory for Macromolecular Science of Shaanxi Province, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, Shaanxi 710119, China
推荐引用方式 GB/T 7714	Chen D.,Li D.,Wang C.,et al. Formation mechanism of methanesulfonic acid and ammonia clusters: A kinetics simulation study[J],2020,222.
APA	Chen D.,Li D.,Wang C.,Liu F.,&Wang W..(2020).Formation mechanism of methanesulfonic acid and ammonia clusters: A kinetics simulation study.ATMOSPHERIC ENVIRONMENT,222.
MLA	Chen D.,et al."Formation mechanism of methanesulfonic acid and ammonia clusters: A kinetics simulation study".ATMOSPHERIC ENVIRONMENT 222(2020).