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

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dc.contributor.authorGallimore, P. J.
dc.contributor.authorMahon, B. M.
dc.contributor.authorWragg, F. P. H.
dc.contributor.authorFuller, S. J.
dc.contributor.authorGiorio, Chiara
dc.contributor.authorKourtchev, Ivan
dc.contributor.funderEuropean Research Councilen
dc.contributor.funderNatural Environment Research Councilen
dc.contributor.funderVelux Fondenen
dc.contributor.funderSeventh Framework Programmeen
dc.date.accessioned2017-09-12T14:58:16Z
dc.date.available2017-09-12T14:58:16Z
dc.date.issued2017-08-22
dc.description.abstractThe 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 (∼ 4 h). 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.en
dc.description.sponsorshipNatural Environment Research Council, UK (grant NE/H52449X/1); Velux Fonden (Velux foundation project number 593).en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationGallimore, P. J., Mahon, B. M., Wragg, F. P. H., Fuller, S. J., Giorio, C., Kourtchev, I. and Kalberer, M. (2017) 'Multiphase composition changes and reactive oxygen species formation during limonene oxidation in the new Cambridge Atmospheric Simulation Chamber (CASC)', Atmospheric Chemistry and Physics, 17(16), pp. 9853-9868. doi: 10.5194/acp-17-9853-2017en
dc.identifier.doi10.5194/acp-17-9853-2017
dc.identifier.endpage9868en
dc.identifier.issn1680-7316
dc.identifier.issn1680-7324
dc.identifier.issued16en
dc.identifier.journaltitleAtmospheric Chemistry and Physicsen
dc.identifier.startpage9853en
dc.identifier.urihttps://hdl.handle.net/10468/4692
dc.identifier.volume17en
dc.language.isoenen
dc.publisherCopernicus Publicationsen
dc.relation.projectinfo:eu-repo/grantAgreement/EC/FP7::SP2::ERC/279405/EU/Composition and Sources of Atmospheric Organic Aerosol and their Negative Health Effects/CORANEen
dc.rights© Authors 2017. This work is distributed under the Creative Commons Attribution 3.0 License.en
dc.rights.urihttp://creativecommons.org/licenses/by/3.0/en
dc.subjectOrganic aerosolsen
dc.subjectMass Spectrometryen
dc.subjectCambridge Atmospheric Simulation Chamber (CASC)en
dc.titleMultiphase composition changes and reactive oxygen species formation during limonene oxidation in the new Cambridge Atmospheric Simulation Chamber (CASC)en
dc.typeArticle (peer-reviewed)en
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