000845400 001__ 845400
000845400 005__ 20240712101039.0
000845400 0247_ $$2Handle$$a2128/18473
000845400 0247_ $$2URN$$aurn:nbn:de:0001-2018050951
000845400 0247_ $$2ISSN$$a1866-1793
000845400 020__ $$a978-3-95806-314-3
000845400 037__ $$aFZJ-2018-02671
000845400 041__ $$aEnglish
000845400 1001_ $$0P:(DE-Juel1)165645$$aGkatzelis, Georgios$$b0$$eCorresponding author$$gmale$$ufzj
000845400 245__ $$aGas-to-Particle Partitioning of Major Oxidation Products from Monoterpenes and Real Plant Emissions$$f- 2018-05-09
000845400 260__ $$aJülich$$bForschungszentrum Jülich GmbH Zentralbibliothek, Verlag$$c2018
000845400 300__ $$axii, 128 S.
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000845400 4900_ $$aSchriften des Forschungszentrums Jülich Reihe Energie & Umwelt / Energy & Environment$$v417
000845400 502__ $$aUniversität Köln, Diss., 2017$$bDissertation$$cUniversität Köln$$d2017
000845400 520__ $$aSecondary organic aerosol (SOA), formed through the oxidation of volatile organic compounds (VOCs) in the atmosphere, play a key role in climate change and air quality. Due to thousands of individual compounds involved in SOA formation, the chemical characterization of organic aerosols (OA) remains a huge analytical challenge. Defining the fundamental parameters that distribute these organic molecules between the gas and particle phases is essential, as atmospheric lifetime and their impacts change drastically depending on their phase state. In this work, an instrument called aerosol collection module (ACM) was redeveloped and automated to allow a better characterization of SOA originating from the oxidation of biogenic precursors. An inter-comparison of the ACM to different aerosol chemical characterization techniques was performed with a focus on the partitioning of major biogenic oxidation products between the gas- and particle-phase. In particular, the ACM, the collection thermal desorption unit (TD) and the chemical analysis of aerosol on-line (CHARON) are different aerosol sampling inlets utilizing a Proton-Transfer-Reaction Timeof- Flight Mass Spectrometer (PTR-ToF-MS). These techniques were deployed at the atmosphere simulation chamber SAPHIR to study SOA formation and aging from different monoterpenes (β-pinene, limonene) and real plant emissions ($\textit{Pinus sylvestris L.}$). The capabilities of the PTR-based techniques were compared among each other and to results from an Aerodyne Aerosol Mass Spectrometer (AMS) and a Scanning Mobility Particle Sizer (SMPS). Gas-to-particle partitioning values were determined based on the saturation mass concentration (C*) of individual ions by performing simultaneous measurement of their signal in the gas- and particle-phase. Despite significant differences in the aerosol collection and desorption methods of the PTR based techniques, the determined chemical composition was comparable, i.e. the same major contributing ions were found by all instruments for the different chemical systems studied. These ions could be attributed to known products expected from the oxidation of the examined monoterpenes. Averaged over all experiments, the total aerosol mass recovery compared to an SMPS was 80 ± 10%, 51 ± 5% and 27 ± 3% for CHARON, ACM and TD, respectively. Comparison to the oxygen to carbon ratios (O:C) obtained by AMS showed that all PTR based techniques observed lower O:C ratios indicating a loss of molecular oxygen either during aerosol sampling or detection. Differences in total mass recovery and O:C between the three instruments was found to result predominately from differences in the electric field strength (V cm$^{-1}$) to buffer gas density (molecules cm$^{-3}$) (E/N) ratio in the drifttube reaction ionization chambers of the PTR-ToF-MS instruments and from dissimilarities in the collection/desorption of aerosols. A method to identify and exclude ions affected by thermal dissociation during desorption and ionic dissociation in the ionization chamber of the PTRMS was developed and tested. Determined species were mapped onto the two dimensional volatility basis set (2D-VBS) and results showed a decrease of the C* with increasing oxidation state. For compounds measured [...]
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