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Gas- and particle-phase products from the photooxidation of acenaphthene and acenaphthylene by OH radicals
AbstractThis work is focused on the gas-phase oxidation of acenaphthylene and acenaphthene by OH radicals and associated secondary organic aerosol (SOA) formation under low and high-NOx conditions. Experiments were carried out in an atmospheric simulation chamber using a proton transfer reaction time-of-flight-mass spectrometer (PTR-TOF-MS) and an aerosol time-of-flight-mass spectrometer (ATOFMS) to chemically characterize the gas- and particle-phase products, respectively. Due to the structures of these two aromatic compounds, the proposed chemical mechanisms exhibit some differences. In the case of acenaphthene, H-atom abstraction from the saturated cyclopenta-fused ring was found to be competitive with the OH-addition to the aromatic rings. During the photooxidation of acenaphthene using nitrous acid (HONO), aromatic ring-opening products such as indanone and indanone carbaldehyde, generated through OH addition to the aromatic ring, were formed in higher yields compared to low-NOx conditions. In the case of acenaphthylene, OH addition to the unsaturated cyclopenta-fused ring was strongly favored. Hence, ring-retaining species such as acenaphthenone and acenaphthenequinone, were identified as the main reaction products in both gas- and particle-phases, especially under high-NOx conditions. Subsequent SOA formation was observed in all experiments and SOA yields were determined under low/high-NOx conditions to be 0.61/0.46 and 0.68/0.55 from the OH-initiated oxidation of acenaphthylene and acenaphthene, respectively.
HighlightsIdentification of competitive pathways for the OH-initiated oxidation of Acenaphthene.Formation of ring-opening products favored from the OH oxidation of Acenaphthylene.Impact of NOx on product distributions and SOA formation have been observed.Proposition of identified secondary chemistry in the extended mechanisms.SOA yields in the range 46–68% have been measured.
Gas- and particle-phase products from the photooxidation of acenaphthene and acenaphthylene by OH radicals
AbstractThis work is focused on the gas-phase oxidation of acenaphthylene and acenaphthene by OH radicals and associated secondary organic aerosol (SOA) formation under low and high-NOx conditions. Experiments were carried out in an atmospheric simulation chamber using a proton transfer reaction time-of-flight-mass spectrometer (PTR-TOF-MS) and an aerosol time-of-flight-mass spectrometer (ATOFMS) to chemically characterize the gas- and particle-phase products, respectively. Due to the structures of these two aromatic compounds, the proposed chemical mechanisms exhibit some differences. In the case of acenaphthene, H-atom abstraction from the saturated cyclopenta-fused ring was found to be competitive with the OH-addition to the aromatic rings. During the photooxidation of acenaphthene using nitrous acid (HONO), aromatic ring-opening products such as indanone and indanone carbaldehyde, generated through OH addition to the aromatic ring, were formed in higher yields compared to low-NOx conditions. In the case of acenaphthylene, OH addition to the unsaturated cyclopenta-fused ring was strongly favored. Hence, ring-retaining species such as acenaphthenone and acenaphthenequinone, were identified as the main reaction products in both gas- and particle-phases, especially under high-NOx conditions. Subsequent SOA formation was observed in all experiments and SOA yields were determined under low/high-NOx conditions to be 0.61/0.46 and 0.68/0.55 from the OH-initiated oxidation of acenaphthylene and acenaphthene, respectively.
HighlightsIdentification of competitive pathways for the OH-initiated oxidation of Acenaphthene.Formation of ring-opening products favored from the OH oxidation of Acenaphthylene.Impact of NOx on product distributions and SOA formation have been observed.Proposition of identified secondary chemistry in the extended mechanisms.SOA yields in the range 46–68% have been measured.
Gas- and particle-phase products from the photooxidation of acenaphthene and acenaphthylene by OH radicals
Riva, Matthieu (author) / Healy, Robert M. (author) / Flaud, Pierre-Marie (author) / Perraudin, Emilie (author) / Wenger, John C. (author) / Villenave, Eric (author)
Atmospheric Environment ; 151 ; 34-44
2016-11-28
11 pages
Article (Journal)
Electronic Resource
English
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