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DOI	10.5194/acp-21-10439-2021
	Aqueous-phase reactive species formed by fine particulate matter from remote forests and polluted urban air
	Tong H.; Liu F.; Filippi A.; Wilson J.; Arangio A.M.; Zhang Y.; Yue S.; Lelieveld S.; Shen F.; Keskinen H.-M.K.; Li J.; Chen H.; Zhang T.; Hoffmann T.; Fu P.; Brune W.H.; Petäjä T.; Kulmala M.; Yao M.; Berkemeier T.; Shiraiwa M.; Pöschl U.
发表日期	2021
ISSN	1680-7316
起始页码	10439
结束页码	10455
卷号	21 期号:13
英文摘要	In the aqueous phase, fine particulate matter can form reactive species (RS) that influence the aging, properties, and health effects of atmospheric aerosols. In this study, we explore the RS yields of aerosol samples from a remote forest (Hyytiälä, Finland) and polluted urban locations (Mainz, Germany; Beijing, China), and we relate the RS yields to different chemical constituents and reaction mechanisms. Ultra-high-resolution mass spectrometry was used to characterize organic aerosol composition, electron paramagnetic resonance (EPR) spectroscopy with a spin-trapping technique was applied to determine the concentrations of OH, O2-, and carbon-or oxygen-centered organic radicals, and a fluorometric assay was used to quantify H2O2. The aqueous H2O2-forming potential per mass unit of ambient PM2.5 (particle diameter 2.5 μm) was roughly the same for all investigated samples, whereas the mass-specific yields of radicals were lower for sampling sites with higher concentrations of PM2.5. The abundances of water-soluble transition metals and aromatics in ambient PM2.5 were positively correlated with the relative fraction of OH and negatively correlated with the relative fraction of carbon-centered radicals. In contrast, highly oxygenated organic molecules (HOM) were positively correlated with the relative fraction of carbon-centered radicals and negatively correlated with the relative fraction of OH. Moreover, we found that the relative fractions of different types of radicals formed by ambient PM2.5 were comparable to surrogate mixtures comprising transition metal ions, organic hydroperoxide, H2O2, and humic or fulvic acids. The interplay of transition metal ions (e.g., iron and copper ions), highly oxidized organic molecules (e.g., hydroperoxides), and complexing or scavenging agents (e.g., humic or fulvic acids) leads to nonlinear concentration dependencies in aqueous-phase RS production. A strong dependence on chemical composition was also observed for the aqueous-phase radical yields of laboratory-generated secondary organic aerosols (SOA) from precursor mixtures of naphthalene and β-pinene. Our findings show how the composition of PM2.5 can influence the amount and nature of aqueous-phase RS, which may explain differences in the chemical reactivity and health effects of particulate matter in clean and polluted air. © 2021 Haijie Tong et al.
语种	英语
scopus关键词	aerosol; atmospheric pollution; chemical composition; particulate matter; radical; urban atmosphere; Beijing [Beijing (ADS)]; Beijing [China]; China; Finland; Germany; Hyytiala; Mainz; Pirkanmaa; Rhineland-Palatinate
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/246741
作者单位	Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz, 55128, Germany; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332, United States; École Polytechnique Fédérale de Lausanne, Lausanne, 1015, Switzerland; Institute of Inorganic and Analytical Chemistry, Johannes Gutenberg University, Mainz, 55128, Germany; State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China; College of Earth and Planetary Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China; Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin, 300072, China; School of Space and Environment, Beihang University, Beijing, 100191, China; Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, Helsinki, 00014, Finland; Hyytiälä Forestr...
推荐引用方式 GB/T 7714	Tong H.,Liu F.,Filippi A.,et al. Aqueous-phase reactive species formed by fine particulate matter from remote forests and polluted urban air[J],2021,21(13).
APA	Tong H..,Liu F..,Filippi A..,Wilson J..,Arangio A.M..,...&Pöschl U..(2021).Aqueous-phase reactive species formed by fine particulate matter from remote forests and polluted urban air.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(13).
MLA	Tong H.,et al."Aqueous-phase reactive species formed by fine particulate matter from remote forests and polluted urban air".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.13(2021).