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DOI | 10.5194/acp-17-9853-2017 |
Multiphase composition changes and reactive oxygen species formation during limonene oxidation in the new Cambridge Atmospheric Simulation Chamber (CASC) | |
Gallimore, Peter J.1; Mahon, Brendan M.1; Wragg, Francis P. H.1; Fuller, Stephen J.1; Giorio, Chiara1,2; Kourtchev, Ivan1,3; Kalberer, Markus1 | |
2017-08-22 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2017 |
卷号 | 17期号:16 |
文章类型 | Article |
语种 | 英语 |
国家 | England; France; Ireland |
英文摘要 | 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 Particlebound 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 longlived on the experiment timescale (similar to 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. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000408098800004 |
WOS关键词 | SECONDARY ORGANIC AEROSOL ; PARTICLE-PHASE ; RATE CONSTANTS ; AIR-POLLUTION ; ALPHA-PINENE ; BETA-PINENE ; GAS UPTAKE ; OZONOLYSIS ; CHEMISTRY ; OZONE |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/30928 |
专题 | 地球科学 |
作者单位 | 1.Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England; 2.Aix Marseille Univ, CNRS, LCE Marseille, Marseille, France; 3.Univ Coll Cork, Dept Chem, Coll Rd, Cork, Ireland |
推荐引用方式 GB/T 7714 | Gallimore, Peter J.,Mahon, Brendan M.,Wragg, Francis P. H.,et al. Multiphase composition changes and reactive oxygen species formation during limonene oxidation in the new Cambridge Atmospheric Simulation Chamber (CASC)[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2017,17(16). |
APA | Gallimore, Peter J..,Mahon, Brendan M..,Wragg, Francis P. H..,Fuller, Stephen J..,Giorio, Chiara.,...&Kalberer, Markus.(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). |
MLA | Gallimore, Peter J.,et al."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(2017). |
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