Dissertation / PhD Thesis

FZJ-2016-02335

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Temperature Dependence of Carbon Kinetic Isotope Effect for Oxidation Reaction of Ethane by Hydroxyl Radicals Under Atmospherically Relevant Conditions: Experimental and Theoretical Studies

Piansawan, T. (Corresponding author)FZJ*

2016
Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag Jülich

Please use a persistent id in citations: http://hdl.handle.net/2128/12363

Abstract: Ethane is the second most abundant hydrocarbon in the atmosphere, after methane, impacting on air quality, human health and climate. A quantification of its effects requires accurate knowledge of sources, processes along transport, and sinks. Carbon stable isotopic ratio investigations, complementarily to concentration measurements, were demonstrated to give more insight in source apportionment and atmospheric processing of organic compounds. Yet, apportionment of atmospheric ethane sources, processing and sinks by using the $^{13}$C isotopic composition ($\delta^{13}$C) requires accurate knowledge of the stable carbon kinetic isotope effect (KIE) of its atmospheric degradation through oxidation by hydroxyl(OH) radicals. Moreover, the interpretation of tropospheric ambient data should account for the temperature dependence of KIE, since the tropospheric temperatures can vary extremely, over the range of 180-320 K. In this work, the KIE temperature dependence for the oxidation of ethane by OH radicals in the tropospherically relevant temperature range was comprehensively investigated by experimental measurements and theoretical calculations. A framework to apply the observed KIE for interpreting ambient observations is presented. Experiments to determine the KIE temperature dependence of ethane oxidation by OH radicals were carried out with natural isotope abundances in the reactant, at ambient pressure, and in a temperature range of 243 to 303 K. Propane was used as a reference compound to verify the ethane chemistry [...]

Note: Bergische Universität Wuppertal, Diss., 2016

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Contributing Institute(s):

1. Troposphäre (IEK-8)

Research Program(s):

1. 243 - Tropospheric trace substances and their transformation processes (POF3-243) (POF3-243)
2. HITEC - Helmholtz Interdisciplinary Doctoral Training in Energy and Climate Research (HITEC) (HITEC-20170406) (HITEC-20170406)

Appears in the scientific report 2016

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