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    Evaluation of a detailed model of secondary organic aerosol formation from α-pinene against dark ozonolysis experiments

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    Ceulemans(2010).pdf (366.9Kb)
    Authors
    Ceulemans, K.
    Compernolle, S.
    Peeters, J.
    Müller, J.-F.
    Show allShow less
    Discipline
    Earth and related Environmental sciences
    Subject
    Detailed models
    Gas phase oxidation
    Gas-phase reactions
    High temperature
    Low-yield
    Non-volatile compounds
    Nonideality
    Order of magnitude
    Organic products
    Ozonolysis
    Prediction methods
    Relative humidities
    Secondary organic aerosols
    Stabilised Criegee intermediates
    Temperature dependence
    Terpenes
    UNIFAC method
    Vapour pressures
    Worst case
    Yield measurement
    Atmospheric aerosols
    Atmospheric humidity
    Experiments
    Lipids
    Olefins
    Oligomers
    Phase interfaces
    Reaction intermediates
    Volatile organic compounds
    Ozone
    oligomer
    pinene
    aerosol formation
    atmospheric modeling
    experimental study
    gas phase reaction
    high temperature
    monoterpene
    oxidation
    ozone
    polymer
    vapor pressure
    article
    gas
    high temperature
    humidity
    magnitude estimation method
    ozonolysis
    priority journal
    secondary organic aerosol
    simulation
    temperature dependence
    thermodynamics
    vapor pressure
    Audience
    Scientific
    Date
    2010
    Metadata
    Show full item record
    Description
    BOREAM, a detailed model for the gas-phase oxidation of α-pinene and its subsequent formation of Secondary Organic Aerosol (SOA), is tested against a large set of SOA yield measurements obtained in dark ozonolysis experiments. For the majority of experiments, modelled SOA yields are found to agree with measured yields to within a factor 2. However, the comparisons point to a general underestimation of modelled SOA yields at high temperatures (above 30 °C), reaching an order of magnitude or more in the worst cases, whereas modelled SOA yields are often overestimated at lower temperature (by a factor of about 2). Comparisons of results obtained using four different vapour pressure prediction methods indicate a strong sensitivity to the choice of the method, although the overestimated temperature dependence of the yields is found in all cases. Accounting for non-ideality of the aerosol mixture (based on an adapted UNIFAC method) has significant effects, especially at low yields. Our simulations show that the formation of oligomers through the gas-phase reactions of Stabilised Criegee Intermediates (SCI) with other molecular organic products could increase the SOA yield significantly only at very low relative humidity (below 1%). Further tests show that the agreement between model and measurements is improved when the ozonolysis mechanism includes additional production of non-volatile compounds.
    Citation
    Ceulemans, K.; Compernolle, S.; Peeters, J.; Müller, J.-F. (2010). Evaluation of a detailed model of secondary organic aerosol formation from α-pinene against dark ozonolysis experiments. , Atmospheric Environment, Vol. 44, Issue 40, 5434-5442, DOI: 10.1016/j.atmosenv.2010.05.001.
    Identifiers
    uri: https://orfeo.belnet.be/handle/internal/3210
    doi: http://dx.doi.org/10.1016/j.atmosenv.2010.05.001
    scopus: 2-s2.0-77950609365
    Type
    Article
    Peer-Review
    Yes
    Language
    eng
    Links
    NewsHelpdeskBELSPO OA Policy

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