Study of the Low Temperature Oxidation of Propane
Identifieur interne : 000A80 ( Hal/Corpus ); précédent : 000A79; suivant : 000A81Study of the Low Temperature Oxidation of Propane
Auteurs : Maximilien Cord ; Benoit Husson ; Juan Carlos Lizardo Huerta ; Olivier Herbinet ; Pierre-Alexandre Glaude ; René Fournet ; Baptiste Sirjean ; Frédérique Battin-Leclerc ; Manuel Ruiz-Lopez ; Zhandong Wang ; Mingfeng Xie ; Zhanjun Cheng ; Fei QiSource :
- Journal of Physical Chemistry A [ 1089-5639 ] ; 2012-11-26.
English descriptors
- mix :
Abstract
The low-temperature oxidation of propane was investigated using a jet-stirred reactor at atmospheric pressure and two methods of analysis: gas chromatography and synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) with direct sampling through a molecular jet. The second method allowed the identification of products, such as molecules with hydroperoxy functions, which are not stable enough to be detected by gas chromatography. Mole fractions of the reactants and reaction products were measured as a function of the temperature (530-730 K), with a particular attention to reaction products involved in the low temperature oxidation, such as cyclic ethers, aldehydes, alcohols, ketones, and hydroperoxides. A new model has been obtained from an automatically generated one, which was used as a starting point, with a large number of re-estimated thermochemical and kinetic data. The kinetic data of the most sensitive reactions, i.e., isomerizations of alkylperoxy radicals and the subsequent decompositions, have been calculated at the CBS-QB3 level of theory. The model allows a satisfactory prediction of the experimental data. A flow rate analysis has allowed highlighting the important reaction channels.
Url:
DOI: 10.1021/jp309821z
Links to Exploration step
Hal:hal-00771603Le document en format XML
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<idno type="DOI">10.1021/jp309821z</idno>
<series><title level="j">Journal of Physical Chemistry A</title>
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<imprint><date type="datePub">2012-11-26</date>
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<profileDesc><textClass><keywords scheme="mix" xml:lang="en"><term>SVUV-PIMS</term>
<term>combustion</term>
<term>detailed kinetic model</term>
<term>ketohydroperoxide</term>
<term>low-temperature</term>
<term>oxidation</term>
<term>propane</term>
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<front><div type="abstract" xml:lang="en">The low-temperature oxidation of propane was investigated using a jet-stirred reactor at atmospheric pressure and two methods of analysis: gas chromatography and synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) with direct sampling through a molecular jet. The second method allowed the identification of products, such as molecules with hydroperoxy functions, which are not stable enough to be detected by gas chromatography. Mole fractions of the reactants and reaction products were measured as a function of the temperature (530-730 K), with a particular attention to reaction products involved in the low temperature oxidation, such as cyclic ethers, aldehydes, alcohols, ketones, and hydroperoxides. A new model has been obtained from an automatically generated one, which was used as a starting point, with a large number of re-estimated thermochemical and kinetic data. The kinetic data of the most sensitive reactions, i.e., isomerizations of alkylperoxy radicals and the subsequent decompositions, have been calculated at the CBS-QB3 level of theory. The model allows a satisfactory prediction of the experimental data. A flow rate analysis has allowed highlighting the important reaction channels.</div>
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<hal api="V3"><titleStmt><title xml:lang="en">Study of the Low Temperature Oxidation of Propane</title>
<author role="aut"><persName><forename type="first">Maximilien</forename>
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<author role="aut"><persName><forename type="first">Benoit</forename>
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<author role="aut"><persName><forename type="first">Juan Carlos</forename>
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<author role="aut"><persName><forename type="first">René</forename>
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<email>Rene.Fournet@ensic.inpl-nancy.fr</email>
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<author role="aut"><persName><forename type="first">Baptiste</forename>
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<author role="aut"><persName><forename type="first">Frédérique</forename>
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<author role="aut"><persName><forename type="first">Manuel</forename>
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<author role="aut"><persName><forename type="first">Mingfeng</forename>
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<author role="aut"><persName><forename type="first">Zhanjun</forename>
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<idno type="halauthor">802581</idno>
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<author role="aut"><persName><forename type="first">Fei</forename>
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<editor role="depositor"><persName><forename>Olivier</forename>
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<email>olivier.herbinet@univ-lorraine.fr</email>
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<funder ref="#projeurop-13713"></funder>
<funder>This work was supported by European Commission ("Clean ICE" ERC Advanced Research Grant) and by the COST Action CM0901. This work was granted access to the HPC resources of CINES under the allocation c2012086686 made by GENCI (Grand Equipement National de Calcul Intensif).</funder>
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<editionStmt><edition n="v1" type="current"><date type="whenSubmitted">2013-01-09 09:04:58</date>
<date type="whenModified">2016-05-10 16:53:49</date>
<date type="whenReleased">2013-01-09 10:25:34</date>
<date type="whenProduced">2012-11-26</date>
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<idno type="doi">10.1021/jp309821z</idno>
</biblStruct>
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<profileDesc><langUsage><language ident="en">English</language>
</langUsage>
<textClass><keywords scheme="author"><term xml:lang="en">propane</term>
<term xml:lang="en">oxidation</term>
<term xml:lang="en">combustion</term>
<term xml:lang="en">low-temperature</term>
<term xml:lang="en">ketohydroperoxide</term>
<term xml:lang="en">SVUV-PIMS</term>
<term xml:lang="en">synchrotron</term>
<term xml:lang="en">detailed kinetic model</term>
</keywords>
<classCode scheme="halDomain" n="chim.theo">Chemical Sciences/Theoretical and/or physical chemistry</classCode>
<classCode scheme="halTypology" n="ART">Journal articles</classCode>
</textClass>
<abstract xml:lang="en">The low-temperature oxidation of propane was investigated using a jet-stirred reactor at atmospheric pressure and two methods of analysis: gas chromatography and synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) with direct sampling through a molecular jet. The second method allowed the identification of products, such as molecules with hydroperoxy functions, which are not stable enough to be detected by gas chromatography. Mole fractions of the reactants and reaction products were measured as a function of the temperature (530-730 K), with a particular attention to reaction products involved in the low temperature oxidation, such as cyclic ethers, aldehydes, alcohols, ketones, and hydroperoxides. A new model has been obtained from an automatically generated one, which was used as a starting point, with a large number of re-estimated thermochemical and kinetic data. The kinetic data of the most sensitive reactions, i.e., isomerizations of alkylperoxy radicals and the subsequent decompositions, have been calculated at the CBS-QB3 level of theory. The model allows a satisfactory prediction of the experimental data. A flow rate analysis has allowed highlighting the important reaction channels.</abstract>
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