Evaluation of a detailed model of secondary organic aerosol formation from α-pinene against dark ozonolysis experiments
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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
2010Metadata
Show full item recordDescription
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
scopus: 2-s2.0-77950609365
Type
Article
Peer-Review
Yes
Language
eng