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DOI	10.1016/j.atmosenv.2021.118615
	On-line study of the influence of seed particle acidity on ozonation reaction of pyrene
	Zhu S.; Qi X.; Zhu C.; Ji Y.; Lou S.; Xu L.; Dong J.; Cheng P.
发表日期	2021
ISSN	1352-2310
卷号	262
英文摘要	Acid-catalyzed heterogeneous reaction can lead to potentially multifold increase in secondary organic aerosol (SOA) generation, which may have a greater impact on climate forcing effects. In this study, single particle aerosol mass spectrometry (SPAMS) and scanning mobility particle sizer (SMPS) were applied to perform an online study of the chemical and physical characteristics of the pyrene-coated inorganic seed particle ozonation in a smog chamber to examine the influence of seed acidity on pyrene-SOA formation. Acidic seed particles are made of ammonium sulfate, ammonium bisulfate and sulfuric acid in different proportions. Fs, the inorganic seed composition number, is defined as a ratio of the molar concentration of SO42− to the total molar concentration of SO42− and NH4+ in this study. Suspended pyrene-coated acidic seed particles were generated by the vaporization-condensation method. Homogeneous and heterogeneous reaction products were identified and assigned. The results show that the seed particle acidity can enhance the mass yield, as well as the chemical diversity of pyrene-SOAs, and also dramatically increase the formation of new smaller particles. Kinetic analysis revealed that the first-order reaction rate constant (K) of acidic seed particles was much higher than that of neutral seed particles, with K values for Fs = 0.77 being 1.47 times that of Fs = 0.50 and 2.58 times that of Fs = 0.33. A mechanism for pyrene-SOA formation was also proposed based on real-time monitoring. For neutral seeds, the pyrene ozonation preferred ‘atom attack’ and mainly formed 1-hydroxypyrene; while for acidic seeds, the pyrene ozonation preferred ‘bond attack’ and formed a Criegee intermediate, followed by broken C–O and C–C bonds, thereby resulting in a variety of semi- and low-volatile products. This study presents a rapid analytical method for the combined use of smog chamber, SPAMS, and SMPS to immediately characterize the effect of seed particle acidity on the formation of polycyclic aromatic hydrocarbon SOA, which may deepen our understanding of new particle formation and particle growth in the atmosphere. Therefore, the present study provides a new insight for an in-depth understanding of haze pollution in China. © 2021 Elsevier Ltd
关键词	Acid-catalyzed reaction Heterogeneous reaction Pyrene Smog chamber SPAMS
语种	英语
scopus关键词	Aerosols; Catalysis; Ozonization; Pyrene; Rate constants; Sulfur compounds; Acid-catalyzed reactions; Aerosol mass spectrometry; Heterogeneous reactions; Organic aerosol; Organic aerosol formation; Scanning mobility particle sizer; Seed particle; Single particle aerosol mass spectrometry; Single-particle; Smog chambers; Mass spectrometry; 1 hydroxypyrene; ammonium bisulfate; ammonium sulfate; ozone; pyrene; sulfuric acid; unclassified drug; acidity; aerosol; aromatic hydrocarbon; climate forcing; hydrocarbon; PAH; pyrene; seed; sulfuric acid; acidity; aerosol; Article; catalysis; chemical reaction kinetics; coated particle; cycloaddition; hydration; ionization; kinetics; mass spectrometry; ozonation; ozonolysis; particle size; polymerization; rate constant; reaction analysis; reaction time; secondary organic aerosol; single particle aerosol mass spectrometry; China
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/248297
作者单位	School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, China; State Environmental Protection Key Laboratory of the Formation and Prevention of Urban Air Pollution Complex, Shanghai Academy of Environmental Science, Shanghai, 200233, China
推荐引用方式 GB/T 7714	Zhu S.,Qi X.,Zhu C.,et al. On-line study of the influence of seed particle acidity on ozonation reaction of pyrene[J],2021,262.
APA	Zhu S..,Qi X..,Zhu C..,Ji Y..,Lou S..,...&Cheng P..(2021).On-line study of the influence of seed particle acidity on ozonation reaction of pyrene.ATMOSPHERIC ENVIRONMENT,262.
MLA	Zhu S.,et al."On-line study of the influence of seed particle acidity on ozonation reaction of pyrene".ATMOSPHERIC ENVIRONMENT 262(2021).