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Experimental study of the formation of organosulfates from $\alpha$-Pinene oxidation. 2. Time evolution and effect of particle acidity

dc.rights.licenseopenen_US
hal.structure.identifierEnvironnements et Paléoenvironnements OCéaniques [EPOC]
dc.contributor.authorDUPORTE, Geoffroy
hal.structure.identifierEnvironnements et Paléoenvironnements OCéaniques [EPOC]
dc.contributor.authorFLAUD, Pierre Marie
ORCID: 0000-0002-2331-5641
IDREF: 102543291
hal.structure.identifierEnvironnements et Paléoenvironnements OCéaniques [EPOC]
dc.contributor.authorKAMMER, Julien
hal.structure.identifierEnvironnements et Paléoenvironnements OCéaniques [EPOC]
dc.contributor.authorGENESTE, Emmanuel
hal.structure.identifierEnvironnements et Paléoenvironnements OCéaniques [EPOC]
dc.contributor.authorAUGAGNEUR, Sylvie
hal.structure.identifierLaboratoire Interuniversitaire des Systèmes Atmosphériques [LISA (UMR_7583)]
dc.contributor.authorPANGUI, E.
hal.structure.identifierLaboratoire Interuniversitaire des Systèmes Atmosphériques [LISA (UMR_7583)]
dc.contributor.authorLAMKADDAM, H.
hal.structure.identifierLaboratoire Interuniversitaire des Systèmes Atmosphériques [LISA (UMR_7583)]
dc.contributor.authorGRATIEN, A.
hal.structure.identifierLaboratoire Interuniversitaire des Systèmes Atmosphériques [LISA (UMR_7583)]
dc.contributor.authorDOUSSIN, J.-F.
hal.structure.identifierEnvironnements et Paléoenvironnements OCéaniques [EPOC]
dc.contributor.authorBUDZINSKI, Hélène
hal.structure.identifierEnvironnements et Paléoenvironnements OCéaniques [EPOC]
dc.contributor.authorVILLENAVE, Eric
hal.structure.identifierEnvironnements et Paléoenvironnements OCéaniques [EPOC]
dc.contributor.authorPERRAUDIN, Emilie
dc.date.accessioned2024-03-20T14:04:59Z
dc.date.available2024-03-20T14:04:59Z
dc.date.issued2020
dc.identifier.issn1089-5639en_US
dc.identifier.urihttps://oskar-bordeaux.fr/handle/20.500.12278/188885
dc.description.abstractEnThe present work is an extensive laboratory study of organosulfate (OS) formation from the reaction of α-pinene oxidation products or proxies with acidified ammonium sulfate aerosols in three different acidity conditions (NH$_4$)$_2$SO$_4$ 0.06 M; (NH$_4$)$_2$SO$_4$/H$_2$SO$_4$ 0.06 M/0.005 M; (NH$_4$)$_2$SO$_4$/H$_2$SO$_4$ 0.03 M/0.05 M). The kinetics of the reactions of $\alpha$-pinene, $\alpha$-pinene oxide, isopinocampheol, pinanediol, and myrtenal with ammonium sulfate particles were studied using a quasi-static reactor. The reaction of $\alpha$-pinene oxide with the highly acidic ammonium sulfate particles was determined to be 7, 10, 21, and 24 times faster than for isopinocampheol, $\alpha$-pinene, pinanedial, and myrtenal, respectively, for an OS precursor concentration of 1 ppm and after 1 h reaction time. The effective rate coefficients for OS formation from $\alpha$-pinene oxide were determined to be 2 orders of magnitude higher in highly acidic conditions than for the two other acidity conditions. For $\alpha$-pinene oxide reactions with highly acidic ammonium sulfate particles, OS formation was observed to increase linearly with (i) the time of reaction up to 400 min ($r^2$= > 0.95) and (ii) α-pinene oxide gas-phase concentration. However, OS formation from $\alpha$-pinene oxide reactions with slightly acidic or pure ammonium sulfate particles was limited, with a plateau ([OS]max = 0.62 ± 0.03 $\mu$g) reached after around 15–20 min. Organosulfate dimers (m/z 401 and m/z 481) were detected not only with highly acidic particles but also with slightly acidic and pure ammonium sulfate particles, indicating that oligomerization processes do not require strong acidity conditions. Dehydration products of organosulfates ($m/z$ 231 and $m/z$ 383) were observed only under highly acidic conditions, indicating the key role of H$_2$SO$_4$ on the dehydration of organosulfates and the formation of olefins in the atmosphere. Finally, this kinetic study was completed with simulation chamber experiments in which the mass concentration of organosulfates was shown to depend on the available sulfate amount present in the particle phase ($r^2$ = 0.96). In conclusion, this relative comparison between five organosulfate precursors shows that epoxide was the most efficient reactant to form organosulfates via heterogeneous gas–particle reactions and illustrates how gas–particle reactions may play an important role in OS formation and hence in the atmospheric fate of organic carbon. The kinetic data presented in this work provide strong support to organosulfate formation mechanisms proposed in part 1 ( J. Phys. Chem. A 2016, 120, 7909−7923).
dc.description.sponsorshipImpact de la chimie des biradicaux organiques atmosphériques sur la genèse d'aérosols - ANR-13-BS06-0002en_US
dc.language.isoENen_US
dc.subject.enOxides
dc.subject.enAnions
dc.subject.enAerosols
dc.subject.enAcidity
dc.subject.enVolatile organic compounds
dc.title.enExperimental study of the formation of organosulfates from $\alpha$-Pinene oxidation. 2. Time evolution and effect of particle acidity
dc.typeArticle de revueen_US
dc.identifier.doi10.1021/acs.jpca.9b07156en_US
dc.subject.halPlanète et Univers [physics]/Océan, Atmosphèreen_US
dc.subject.halPlanète et Univers [physics]/Interfaces continentales, environnementen_US
dc.description.sponsorshipEuropeIntegration of European Simulation Chambers for Investigating Atmospheric Processes - Part 2en_US
bordeaux.journalJournal of Physical Chemistry Aen_US
bordeaux.page409-421en_US
bordeaux.volume124en_US
bordeaux.hal.laboratoriesEPOC : Environnements et Paléoenvironnements Océaniques et Continentaux - UMR 5805en_US
bordeaux.issue2en_US
bordeaux.institutionUniversité de Bordeauxen_US
bordeaux.institutionCNRSen_US
bordeaux.teamLPTCen_US
bordeaux.peerReviewedouien_US
bordeaux.inpressnonen_US
bordeaux.import.sourcehal
hal.identifierhal-02967567
hal.version1
hal.popularnonen_US
hal.audienceInternationaleen_US
hal.exportfalse
workflow.import.sourcehal
dc.rights.ccPas de Licence CCen_US
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