Detailed product analysis during the low temperature oxidation of n-butane

Olivier Herbinet (1) , Frédérique Battin-Leclerc (1) , Sarah Bax (1) , Hervé Le Gall (1) , Pierre Alexandre Glaude (1) , René Fournet (1) , Zhongyue Zhou (2) , Liulin Deng (2) , Huijun Guo (2) , Mingfeng Xie (2) , Fei Qi (2)

1 LRGP - Laboratoire Réactions et Génie des Procédés
2 National Synchrotron Radiation Laboratory

The products obtained from the low-temperature oxidation of n-butane in a jet-stirred reactor (JSR) have been analysed using two methods: gas chromatography analysis of the outlet gas and reflectron time-of-flight mass spectrometry. The mass spectrometer was combined with tunable synchrotron vacuum ultraviolet photoionization and coupled with a JSR via a molecular-beam sampling system. Experiments were performed under quasi-atmospheric pressure, for temperatures between 550 and 800 K, at a mean residence time of 6 s and with a stoichiometric n-butane/oxygen/argon mixture (composition = 4/26/70 in mol%). 36 reaction products have been quantified, including in addition to the usual oxidation products, acetic acid, hydrogen peroxide, C1, C2 and C4 alkylhydroperoxides and C4 ketohydroperoxides. Evidence of the possible formation of products (dihydrofuranes, furanones) derived from cyclic ethers has also been found. The performance of a detailed kinetic model of the literature has been assessed with the simulation of the formation of this extended range of species. These simulations have also allowed the analysis of possible pathways for the formation of some obtained products.

Domaines: Chimie-Physique [physics.chem-ph]

Olivier Herbinet, Frédérique Battin-Leclerc, Sarah Bax, Hervé Le Gall, Pierre Alexandre Glaude, et al.. Detailed product analysis during the low temperature oxidation of n-butane. Physical Chemistry Chemical Physics, 2011, 13, pp. 296-308. ⟨10.1039/C0CP00539H⟩. ⟨hal-00602156⟩