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Etude de la formation d'aérosols organiques secondaires par spectométrie de masse lors de l'ozonolyse de composés organiques volatils insatures

Abstract : The understanding of secondary organic aerosols (SOA) is still incomplete, especially from the ozonolysis of unsaturated volatile organic compounds (VOC). The measurement of low volatility compounds involved in SOA formation is a challenge that the scientific community attempts to address. One of the objectives of this thesis work was the installation and use of a system for sampling and measuring the chemical composition of the aerosol by chemical ionization mass spectrometry (FIGAERO-CI-ToF-MS). This instrument has been used in the ozonolysis of unsaturated VOCs in the atmospheric simulation chamber HELIOS and the conditions for the formation of carboxylic acids and organosulfur compounds has been evaluated. The specific formation pathways of organosulfates (OS) have in addition been studied by injecting acidified seed particles. This study confirmed the low efficiency of the esterification of hydroxyl groups. Conversely, OS formation by epoxide ring opening is more efficient and increases with more acidic pH. In addition, the increase in relative humidity has a positive impact on the generation of carboxylic acids in the particulate phase.A second objective was the characterization of a system coupled to a proton transfer mass spectrometer (CHARON-PTR-ToF-MS) for collecting aerosols and measuring its chemical composition. The measurement of the fragmentation of 26 pure compounds in particulate phase allowed the development of a corrective procedure taking into account fragmentation process. This procedure was applied to the measurement of SOA generated by the ozonolysis of biogenic VOCs in an aerosol flow reactor. The volatility of the aerosol has been estimated using a thermodenuder installed downstream of the reactor. Taking into account fragmentation has greatly improved the agreement between the measured and the calculated volatility by several parametric equations.
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Joris Leglise. Etude de la formation d'aérosols organiques secondaires par spectométrie de masse lors de l'ozonolyse de composés organiques volatils insatures. Autre. Université d'Orléans, 2019. Français. ⟨NNT : 2019ORLE3013⟩. ⟨tel-03101668⟩

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