Comprehensive modelling study of ozonolysis of oleic acid aerosol based on real-time, online measurements of aerosol composition

P. J. Gallimore, P. T. Griffiths, F. D. Pope, Jonathan Reid, M. Kalberer

Research output: Contribution to journalArticle (Academic Journal)peer-review

12 Citations (Scopus)
401 Downloads (Pure)

Abstract

The chemical composition of organic aerosols profoundly influences their atmospheric properties, but a detailed understanding of heterogeneous and in-particle reactivity is lacking. We present here a combined experimental and modelling study of the ozonolysis of oleic acid particles. An online mass spectrometry (MS) method, Extractive Electrospray Ionization (EESI), is used to follow the composition of the aerosol at a molecular level in real time; relative changes in the concentrations of both reactants and products are determined during aerosol aging. The results show evidence for multiple non first order reactions involving stabilized Criegee intermediates, including the formation of secondary ozonides and other oligomers. Offline Liquid Chromatography (LC) MS is used to confirm the online MS assignment of the monomeric and dimeric products. We explain the observed EESI-MS chemical composition changes, and chemical and physical data from previous studies, using a process-based aerosol chemistry simulation, the Pretty Good Aerosol Model (PG-AM). In particular, we extend previous studies of reactant loss by demonstrating success in reproducing the time dependence of product formation and the evolving particle size. This advance requires a comprehensive chemical scheme coupled to the partitioning of semivolatile products; relevant reaction and evaporation parameters have been refined using our new measurements in combination with PG-AM.
Original languageEnglish
Pages (from-to)4364-4377
Number of pages14
JournalJournal of Geophysical Research: Atmospheres
Volume122
Issue number8
Early online date18 Apr 2017
DOIs
Publication statusPublished - 27 Apr 2017

Keywords

  • aerosol
  • SOA
  • mass spectrometry
  • EESI-MS
  • process model
  • PG-AM

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