气候变化领域集成服务门户(CCPortal): Role of base strength; cluster structure and charge in sulfuric-acid-driven particle formation

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DOI	10.5194/acp-19-9753-2019
	Role of base strength; cluster structure and charge in sulfuric-acid-driven particle formation
	Myllys N.; Kubečka J.; Besel V.; Alfaouri D.; Olenius T.; Norman Smith J.; Passananti M.
发表日期	2019
ISSN	16807316
起始页码	9753
结束页码	9768
卷号	19 期号:15
英文摘要	In atmospheric sulfuric-acid-driven particle formation, bases are able to stabilize the initial molecular clusters and thus enhance particle formation. The enhancing potential of a stabilizing base is affected by different factors, such as the basicity and abundance. Here we use weak (ammonia), medium strong (dimethylamine) and very strong (guanidine) bases as representative atmospheric base compounds, and we systematically investigate their ability to stabilize sulfuric acid clusters. Using quantum chemistry, we study proton transfer as well as intermolecular interactions and symmetry in clusters, of which the former is directly related to the base strength and the latter to the structural effects. Based on the theoretical cluster stabilities and cluster population kinetics modeling, we provide molecular-level mechanisms of cluster growth and show that in electrically neutral particle formation, guanidine can dominate formation events even at relatively low concentrations. However, when ions are involved, charge effects can also stabilize small clusters for weaker bases. In this case the atmospheric abundance of the bases becomes more important, and thus ammonia is likely to play a key role. The theoretical findings are validated by cluster distribution experiments, as well as comparisons to previously reported particle formation rates, showing a good agreement. © Author(s) 2019.
语种	英语
scopus关键词	ammonia; cluster analysis; particulate matter; reaction kinetics; sulfuric acid; symmetry; theoretical study
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/144235
作者单位	Department of Chemistry, University of California, Irvine, CA, United States; Institute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, Finland; Department of Environmental Science, Analytical Chemistry and Bolin Centre for Climate Research, Stockholm University, Stockholm, Sweden; Dipartimento di Chimica, Universitá di Torino, Turin, Italy
推荐引用方式 GB/T 7714	Myllys N.,Kubečka J.,Besel V.,et al. Role of base strength; cluster structure and charge in sulfuric-acid-driven particle formation[J],2019,19(15).
APA	Myllys N..,Kubečka J..,Besel V..,Alfaouri D..,Olenius T..,...&Passananti M..(2019).Role of base strength; cluster structure and charge in sulfuric-acid-driven particle formation.Atmospheric Chemistry and Physics,19(15).
MLA	Myllys N.,et al."Role of base strength; cluster structure and charge in sulfuric-acid-driven particle formation".Atmospheric Chemistry and Physics 19.15(2019).