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.author Gallimore, P. J.
dc.contributor.author Mahon, B. M.
dc.contributor.author Wragg, F. P. H.
dc.contributor.author Fuller, S. J.
dc.contributor.author Giorio, Chiara
dc.contributor.author Kourtchev, Ivan
dc.date.accessioned 2017-09-12T14:58:16Z
dc.date.available 2017-09-12T14:58:16Z
dc.date.issued 2017-08-22
dc.identifier.citation Gallimore, 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-17-9853-2017 en
dc.identifier.volume 17 en
dc.identifier.issued 16 en
dc.identifier.startpage 9853 en
dc.identifier.endpage 9868 en
dc.identifier.issn 1680-7316
dc.identifier.issn 1680-7324
dc.identifier.uri http://hdl.handle.net/10468/4692
dc.identifier.doi 10.5194/acp-17-9853-2017
dc.description.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 (∼ 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.sponsorship Natural Environment Research Council, UK (grant NE/H52449X/1); Velux Fonden (Velux foundation project number 593). en
dc.format.mimetype application/pdf en
dc.language.iso en en
dc.publisher Copernicus Publications en
dc.rights © Authors 2017. This work is distributed under the Creative Commons Attribution 3.0 License. en
dc.rights.uri http://creativecommons.org/licenses/by/3.0/ en
dc.subject Organic aerosols en
dc.subject Mass Spectrometry en
dc.subject Cambridge Atmospheric Simulation Chamber (CASC) en
dc.title Multiphase composition changes and reactive oxygen species formation during limonene oxidation in the new Cambridge Atmospheric Simulation Chamber (CASC) en
dc.type Article (peer-reviewed) en
dc.internal.authorcontactother Ivan Kourtchev, Chemistry, University College Cork, Cork, Ireland. +353-21-490-3000 Email: I.Kourtchev@ucc.ie en
dc.internal.availability Full text available en
dc.description.version Published Version en
dc.contributor.funder European Research Council en
dc.contributor.funder Natural Environment Research Council en
dc.contributor.funder Velux Fonden en
dc.contributor.funder Seventh Framework Programme en
dc.description.status Peer reviewed en
dc.identifier.journaltitle Atmospheric Chemistry and Physics en
dc.internal.copyrightchecked !!CORA!! en
dc.internal.IRISemailaddress i.kourtchev@ucc.ie en
dc.relation.project info:eu-repo/grantAgreement/EC/FP7::SP2::ERC/279405/EU/Composition and Sources of Atmospheric Organic Aerosol and their Negative Health Effects/CORANE en


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© Authors 2017. This work is distributed under the Creative Commons Attribution 3.0 License. Except where otherwise noted, this item's license is described as © Authors 2017. This work is distributed under the Creative Commons Attribution 3.0 License.
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