title: Reactions of Atmospheric Particulate Stabilized Criegee Intermediates Lead to High-Molecular-Weight Aerosol Components.
abstract: Aging of organic aerosol particles is one of the most poorly understood topics in atmospheric aerosol research. Here, we used an aerosol flow tube together with an iodide-adduct high-resolution time-of-flight chemical-ionization mass spectrometer equipped with a Filter Inlet for Gases and AEROsols (FIGAERO-HRToF-CIMS) to investigate heterogeneous ozonolysis of oleic acid (OL), developing a comprehensive oxidation mechanism with observed products. In addition to the well-known first-generation C9 products including nonanal, nonanoic acid, azelaic acid, and 9-oxononanoic acid, the iodide-adduct chemical ionization permitted unambiguous determination of a large number of high-molecular-weight particulate products up to 670 Da with minimum amounts of fragmentation. These high-molecular-weight products are characterized by a fairly uniform carbon oxidation state but stepwise addition of a carbon backbone moiety, and hence continuous decrease in the volatility. Our results demonstrate that heterogeneous oxidation of organic aerosols has a significant effect on the physiochemical properties of organic aerosols and that reactions of particulate SCIs from ozonolysis of an unsaturated particulate species represent a previously underappreciated mechanism that lead to formation of high-molecular-weight particulate products that are stable under typical atmospheric conditions.
authors.affiliation: Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University , Shanghai 200433, China.
authors.forename: MingYi
authors.initials: M
authors.lastname: Wang
authors.affiliation: Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University , Shanghai 200433, China.
authors.forename: Lei
authors.initials: L
authors.lastname: Yao
authors.affiliation: Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Nanjing University of Information Science & Technology , Nanjing 210044, China.
authors.forename: Jun
authors.initials: J
authors.lastname: Zheng
authors.affiliation: Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University , Shanghai 200433, China.
authors.forename: XinKe
authors.initials: X
authors.lastname: Wang
authors.affiliation: Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University , Shanghai 200433, China.
authors.forename: JianMin
authors.initials: J
authors.lastname: Chen
authors.affiliation: Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University , Shanghai 200433, China.
authors.forename: Xin
authors.initials: X
authors.lastname: Yang
authors.affiliation: Aerodyne Research, Billerica, Massachusetts 01821, United States.
authors.forename: Douglas R
authors.initials: DR
authors.lastname: Worsnop
authors.affiliation: Center for Atmospheric Particle Studies, Carnegie Mellon University , 5000 Forbes Avenue, Pittsburgh, Pennsylvania 15213, United States.
authors.forename: Neil M
authors.initials: NM
authors.lastname: Donahue
authors.affiliation: Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University , Shanghai 200433, China.
authors.forename: Lin
authors.initials: L
authors.lastname: Wang
mesh_terms: D000336:Aerosols / Q000737:chemistry*; D005740:Gases / Q000737:chemistry; D019301:Oleic Acid / Q000737:chemistry; D010084:Oxidation-Reduction; D010316:Particle Size
chemical_list: D000336:Aerosols; D005740:Gases; D019301:Oleic Acid