Study of the Low Temperature Oxidation of Propane

详细信息    查看全文

• 作者：Maximilien Cord ; Benoit Husson ; Juan Carlos Lizardo Huerta ; Olivier Herbinet ; Pierre-Alexandre Glaude ; Ren茅 Fournet ; Baptiste Sirjean ; Fr茅d茅rique Battin-Leclerc ; Manuel Ruiz-Lopez ; Zhandong Wang ; Mingfeng Xie ; Zhanjun Cheng ; Fei Qi
• 刊名：The Journal of Physical Chemistry A
• 出版年：2012
• 出版时间：December 20, 2012
• 年：2012
• 卷：116
• 期：50
• 页码：12214-12228
• 全文大小：885K
• 年卷期：v.116,no.50(December 20, 2012)
• ISSN：1520-5215

文摘

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鈥?30 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.