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DOI	10.1073/pnas.1915459116
	Unexpected quenching effect on new particle formation from the atmospheric reaction of methanol with SO3
	Liu L.; Zhong J.; Vehkamäki H.; Kurtén T.; Du L.; Zhang X.; Francisco J.S.; Zeng X.C.
发表日期	2019
ISSN	0027-8424
起始页码	24966
结束页码	24971
卷号	116 期号:50
英文摘要	Despite the high abundance in the atmosphere, alcohols in general and methanol in particular are believed to play a small role in atmospheric new particle formation (NPF) largely due to the weak binding abilities of alcohols with the major nucleation precursors, e.g., sulfuric acid (SA) and dimethylamine (DMA). Herein, we identify a catalytic reaction that was previously overlooked, namely, the reaction between methanol and SO3, catalyzed by SA, DMA, or water. We found that alcohols can have unexpected quenching effects on the NPF process, particularly in dry and highly polluted regions with high concentrations of alcohols. Specifically, the catalytic reaction between methanol and SO3 can convert methanol into a less-volatile species––methyl hydrogen sulfate (MHS). The latter was initially thought to be a good nucleation agent for NPF. However, our simulation results suggest that the formation of MHS consumes an appreciable amount of atmospheric SO3, disfavoring further reactions of SO3 with H2O. Indeed, we found that MHS formation can cause a reduction of SA concentration up to 87%, whereas the nucleation ability of MHS toward new particles is not as good as that of SA. Hence, a high abundance of methanol in the atmosphere can lower the particle nucleation rate by as much as two orders of magnitude. Such a quenching effect suggests that the recently identified catalytic reactions between alcohols and SO3 need to be considered in atmospheric modeling in order to predict SA concentration from SO2, while also account for their potentially negative effect on NPF. © 2019 National Academy of Sciences. All rights reserved.
英文关键词	Alcohols; Atmospheric aerosol; Catalytic reactions; Nucleation precursors; SO3
语种	英语
scopus关键词	alcohol; dimethylamine; methanol; sulfur derivative; sulfur trioxide; sulfuric acid; unclassified drug; Article; atmosphere; catalysis; chemical reaction; controlled study; evaporation; hydrogen bond; molecular dynamics; priority journal; quorum sensing; simulation; thermodynamics
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/160329
作者单位	Liu, L., Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081, China, Department of Chemistry, University of Nebraska–Lincoln, Lincoln, NE 68588, United States; Zhong, J., Department of Chemistry, University of Nebraska–Lincoln, Lincoln, NE 68588, United States, Department of Earth and Environmental Sciences, University of Pennsylvania, Philadelphia, PA 19104, United States, Department of Chemistry, University of Pennsylvania, Philadelphia, PA 19104, United States; Vehkamäki, H., Faculty of Science, Institute for Atmospheric and Earth System Research/Physics, University of Helsinki, Helsinki, FI-00014, Finland; Kurtén, T., Department of Chemistry, University of Helsinki, Helsinki, FI-00014, Finland; Du, L., Environment Research Institute, Shandong University, Qingdao, 266237, China; Zhang, X., Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical En...
推荐引用方式 GB/T 7714	Liu L.,Zhong J.,Vehkamäki H.,et al. Unexpected quenching effect on new particle formation from the atmospheric reaction of methanol with SO3[J],2019,116(50).
APA	Liu L..,Zhong J..,Vehkamäki H..,Kurtén T..,Du L..,...&Zeng X.C..(2019).Unexpected quenching effect on new particle formation from the atmospheric reaction of methanol with SO3.Proceedings of the National Academy of Sciences of the United States of America,116(50).
MLA	Liu L.,et al."Unexpected quenching effect on new particle formation from the atmospheric reaction of methanol with SO3".Proceedings of the National Academy of Sciences of the United States of America 116.50(2019).