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  Heterogeneous Ozonolysis of Squalene: Gas-Phase Products Depend on Water Vapor Concentration

Arata, C., Heine, N., Wang, N., Misztal, P. K., Wargocki, P., Beko, G., et al. (2019). Heterogeneous Ozonolysis of Squalene: Gas-Phase Products Depend on Water Vapor Concentration. Environmental Science & Technology, 53(24), 14441-14448. doi:10.1021/acs.est.9b05957.

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Arata, Caleb1, Autor
Heine, Nadja1, Autor
Wang, Nijing2, Autor           
Misztal, Pawel K.1, Autor
Wargocki, Pawel1, Autor
Beko, Gabriel1, Autor
Williams, Jonathan2, Autor           
Nazaroff, William W.1, Autor
Wilson, Kevin R.1, Autor
Goldstein, Allen H.1, Autor
Affiliations:
1external, ou_persistent22              
2Atmospheric Chemistry, Max Planck Institute for Chemistry, Max Planck Society, ou_1826285              

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 Zusammenfassung: Previous work examining the condensed-phase products of squalene particle ozonolysis found that an increase in water vapor concentration led to lower concentrations of secondary ozonides, increased concentrations of carbonyls, and smaller particle diameter, suggesting that water changes the fate of the Criegee intermediate. To determine if this volume loss corresponds to an increase in gas-phase products, we measured gas-phase volatile organic compound (VOC) concentrations via proton-transfer-reaction time-of-flight mass spectrometry. Studies were conducted in a flow-tube reactor at atmospherically relevant ozone (O3) exposure levels (5-30 ppb h) with pure squalene particles. An increase in water vapor concentration led to strong enhancement of gas-phase oxidation products at all tested O3 exposures. An increase in water vapor from near zero to 70% relative humidity (RH) at high O3 exposure increased the total mass concentration of gas-phase VOCs by a factor of 3. The observed fraction of carbon in the gas-phase correlates with the fraction of particle volume lost. Experiments involving O3 oxidation of shirts soiled with skin oil confirms that the RH dependence of gas-phase reaction product generation occurs similarly on surfaces containing skin oil under realistic conditions. Similar behavior is expected for O3 reactions with other surface-bound organics containing unsaturated carbon bonds.

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 Datum: 2019
 Publikationsstatus: Erschienen
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 Identifikatoren: ISI: 000503910500039
DOI: 10.1021/acs.est.9b05957
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Titel: Environmental Science & Technology
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Easton, PA : American Chemical Society
Seiten: - Band / Heft: 53 (24) Artikelnummer: - Start- / Endseite: 14441 - 14448 Identifikator: ISSN: 0013-936X
CoNE: https://pure.mpg.de/cone/journals/resource/954921342157