Particle-phase processing of α-pinene NO3 secondary organic aerosol in the dark
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Published:2022-10-13
Issue:19
Volume:22
Page:13167-13182
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Bell David M., Wu Cheng, Bertrand Amelie, Graham Emelie, Schoonbaert Janne, Giannoukos Stamatios, Baltensperger UrsORCID, Prevot Andre S. H., Riipinen Ilona, El Haddad Imad, Mohr ClaudiaORCID
Abstract
Abstract. The NO3 radical represents a significant nighttime oxidant which is present downstream of polluted environments. Existing studies have
investigated the formation of secondary organic aerosol (SOA) from NO3
radicals, focusing on the yields, general composition, and hydrolysis of
organonitrates; however, there is limited knowledge about how the
composition of NO3-derived SOA evolves as a result of particle-phase
reactions. Here, SOA was formed from the reaction of α-pinene with
NO3 radicals generated from N2O5, and the resulting SOA was aged
in the dark. The initial composition of NO3-derived α-pinene
SOA was slightly dependent upon the concentration of N2O5 injected
(excess of NO3 or excess of α-pinene) but was largely
dominated by dimer dinitrates (C20H32N2O8−13). Oxidation reactions (e.g., C20H32N2O8→
C20H32N2O9→ C20H32N2O10) accounted for 60 %–70 % of the particle-phase reactions
observed. Fragmentation reactions and dimer degradation pathways made up the
remainder of the particle-phase processes occurring. The exact oxidant is
not known, although suggestions are offered (e.g., N2O5, organic
peroxides, or peroxynitrates). Hydrolysis of –ONO2 functional groups was not an important loss term during dark aging under the relative humidity
conditions of our experiments (58 %–62 %), and changes in the bulk
organonitrate composition were likely driven by evaporation of highly
nitrogenated molecules. Overall, 25 %–30 % of the particle-phase composition
changes as a function of particle-phase reactions during dark aging,
representing an important atmospheric aging pathway.
Funder
Horizon 2020 Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung Knut och Alice Wallenbergs Stiftelse
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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