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DOI	10.5194/acp-20-515-2020
	Multi-generation OH oxidation as a source for highly oxygenated organic molecules from aromatics
	Garmash O.; Rissanen M.P.; Pullinen I.; Schmitt S.; Kausiala O.; Tillmann R.; Zhao D.; Percival C.; Bannan T.J.; Priestley M.; Hallquist A.M.; Kleist E.; Kiendler-Scharr A.; Hallquist M.; Berndt T.; McFiggans G.; Wildt J.; Mentel T.F.; Ehn M.
发表日期	2020
ISSN	1680-7316
起始页码	515
结束页码	537
卷号	20 期号:1
英文摘要	Recent studies have recognised highly oxygenated organic molecules (HOMs) in the atmosphere as important in the formation of secondary organic aerosol (SOA). A large number of studies have focused on HOM formation from oxidation of biogenically emitted monoterpenes. However, HOM formation from anthropogenic vapours has so far received much less attention. Previous studies have identified the importance of aromatic volatile organic compounds (VOCs) for SOA formation. In this study, we investigated several aromatic compounds, benzene (C6H6), toluene (C7H8), and naphthalene (C10H8), for their potential to form HOMs upon reaction with hydroxyl radicals (OH). We performed flow tube experiments with all three VOCs and focused in detail on benzene HOM formation in the Julich Plant Atmosphere Chamber (JPAC). In JPAC, we also investigated the response of HOMs to NOx and seed aerosol. Using a nitrate-based chemical ionisation mass spectrometer (CI-APi-TOF), we observed the formation of HOMs in the flow reactor oxidation of benzene from the first OH attack. However, in the oxidation of toluene and naphthalene, which were injected at lower concentrations, multigeneration OH oxidation seemed to impact the HOM composition. We tested this in more detail for the benzene system in the JPAC, which allowed for studying longer residence times. The results showed that the apparent molar benzene HOM yield under our experimental conditions varied from 4.1% to 14.0 %, with a strong dependence on the OH concentration, indicating that the majority of observed HOMs formed through multiple OH-oxidation steps. The composition of the identified HOMs in the mass spectrum also supported this hypothesis. By injecting only phenol into the chamber, we found that phenol oxidation cannot be solely responsible for the observed HOMs in benzene experiments. When NOx was added to the chamber, HOM composition changed and many oxygenated nitrogen-containing products were observed in CI-APi-TOF. Upon seed aerosol injection, the HOM loss rate was higher than predicted by irreversible condensation, suggesting that some undetected oxygenated intermediates also condensed onto seed aerosol, which is in line with the hypothesis that some of the HOMs were formed in multi-generation OH oxidation. Based on our results, we conclude that HOM yield and composition in aromatic systems strongly depend on OH and VOC concentration and more studies are needed to fully understand this effect on the formation of HOMs and, consequently, SOA. We also suggest that the dependence of HOM yield on chamber conditions may explain part of the variability in SOA yields reported in the literature and strongly advise monitoring HOMs in future SOA studies. © Author(s) 2020.
语种	英语
scopus关键词	aerosol; aromatic hydrocarbon; concentration (composition); condensation; monoterpene; nitrate; organic matter; oxidation; ozone; volatile organic compound
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/248046
作者单位	Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland; Aerosol Physics Laboratory, Physics Unit, Faculty of Engineering and Natural Sciences, Tampere University, Tampere, Finland; Institut für Energie- und Klimaforschung, IEK-8: Troposphäre, Forschungszentrum Jülich GmbH, Jülich, Germany; Department of Earth and Environmental Sciences, School of Natural Sciences, University of Manchester, Manchester, United Kingdom; Atmospheric Science, Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden; IVL Swedish Environmental Research Institute, Gothenburg, Sweden; Institut für Bio- und Geowissenschaften, IBG-2: Pflanzenwissenschaften, Forschungszentrum Jülich GmbH, Jülich, Germany; Leibniz-Institut für Troposphärenforschung (TROPOS), Leipzig, 04318, Germany; Department of Applied Physics, University of Eastern Finland, Kuopio, Finland; TSI GmbH, Aachen, Germany; Kärsa Oy, Helsinki, Finland; Department of Atmo...
推荐引用方式 GB/T 7714	Garmash O.,Rissanen M.P.,Pullinen I.,et al. Multi-generation OH oxidation as a source for highly oxygenated organic molecules from aromatics[J],2020,20(1).
APA	Garmash O..,Rissanen M.P..,Pullinen I..,Schmitt S..,Kausiala O..,...&Ehn M..(2020).Multi-generation OH oxidation as a source for highly oxygenated organic molecules from aromatics.ATMOSPHERIC CHEMISTRY AND PHYSICS,20(1).
MLA	Garmash O.,et al."Multi-generation OH oxidation as a source for highly oxygenated organic molecules from aromatics".ATMOSPHERIC CHEMISTRY AND PHYSICS 20.1(2020).