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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Volume 17, issue 16 | Copyright
Atmos. Chem. Phys., 17, 9853-9868, 2017
https://doi.org/10.5194/acp-17-9853-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 22 Aug 2017

Research article | 22 Aug 2017

Multiphase composition changes and reactive oxygen species formation during limonene oxidation in the new Cambridge Atmospheric Simulation Chamber (CASC)

Peter J. Gallimore1, Brendan M. Mahon1, Francis P. H. Wragg1, Stephen J. Fuller1, Chiara Giorio1,a, Ivan Kourtchev1,b, and Markus Kalberer1 Peter J. Gallimore et al.
  • 1Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK
  • anow at: Aix Marseille Univ, CNRS, LCE Marseille, France
  • bnow at: Department of Chemistry, University College Cork, College Road, Cork, Ireland

Abstract. The chemical composition of organic aerosols influences their impacts on human health and the climate system. Aerosol formation from gas-to-particle conversion and in-particle reaction was studied for the oxidation of limonene in a new facility, the Cambridge Atmospheric Simulation Chamber (CASC). Health-relevant oxidising organic species produced during secondary organic aerosol (SOA) formation were quantified in real time using an Online Particle-bound Reactive Oxygen Species Instrument (OPROSI). Two categories of reactive oxygen species (ROS) were identified based on time series analysis: a short-lived component produced during precursor ozonolysis with a lifetime of the order of minutes, and a stable component that was long-lived on the experiment timescale (∼4h). Individual organic species were monitored continuously over this time using Extractive Electrospray Ionisation (EESI) Mass Spectrometry (MS) for the particle phase and Proton Transfer Reaction (PTR) MS for the gas phase. Many first-generation oxidation products are unsaturated, and we observed multiphase aging via further ozonolysis reactions. Volatile products such as C9H14O (limonaketone) and C10H16O2 (limonaldehyde) were observed in the gas phase early in the experiment, before reacting again with ozone. Loss of C10H16O4 (7-hydroxy limononic acid) from the particle phase was surprisingly slow. A combination of reduced C = C reactivity and viscous particle formation (relative to other SOA systems) may explain this, and both scenarios were tested in the Pretty Good Aerosol Model (PG-AM). A range of characterisation measurements were also carried out to benchmark the chamber against existing facilities. This work demonstrates the utility of CASC, particularly for understanding the reactivity and health-relevant properties of organic aerosols using novel, highly time-resolved techniques.

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Limonene is emitted in substantial quantities by plants, and also has indoor sources from air fresheners and cleaning products. We studied particle formation from the oxidation of limonene and found substantial quantities of oxidising components which are thought to be associated with the negative health effects of particulates. State-of-the-art measurements of the products of limonene–ozone chemistry were also presented.
Limonene is emitted in substantial quantities by plants, and also has indoor sources from air...
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