Jump to main content
Jump to site search

Issue 45, 2013
Previous Article Next Article

Experimental and modeling study of the oxidation of n-butane in a jet stirred reactor using cw-CRDS measurements

Author affiliations

Abstract

The gas-phase oxidation of n-butane has been studied in an atmospheric jet-stirred reactor (JSR) at temperatures up to 950 K. For the first time, continuous wave cavity ring-down spectroscopy (cw-CRDS) in the near-infrared has been used, together with gas chromatography (GC), to analyze the products formed during its oxidation. In addition to the quantification of formaldehyde and water, which is always difficult by GC, cw-CRDS allowed as well the quantification of hydrogen peroxide (H2O2). A comparison of the obtained mole fraction temperature profiles with simulations using a detailed gas-phase mechanism shows a good agreement at temperatures below 750 K, but an overestimation of the overall reactivity above this temperature. Also, a strong overestimation was found for the H2O2 mole fraction at higher temperatures. In order to improve the agreement between model and experimental results, two modifications have been implemented to the model: (a) the rate constant for the decomposition of H2O2 (+M) ↔ 2OH (+M) has been updated to the value recently proposed by Troe (Combust. Flame, 2011, 158, 594–601) and (b) a temperature dependent heterogeneous destruction of H2O2 on the hot reactor walls with assumed rate parameters has been added. The improvement (a) slows down the overall reactivity at higher temperatures, but has a negligible impact on the maximal H2O2 mole fraction. Improvement (b) has also a small impact on the overall reactivity at higher temperatures, but a large effect on the maximal H2O2 mole fraction. Both modifications lead to an improved agreement between model and experiment for the oxidation of n-butane in a JSR at temperatures above 750 K.

Graphical abstract: Experimental and modeling study of the oxidation of n-butane in a jet stirred reactor using cw-CRDS measurements

Back to tab navigation

Supplementary files

Publication details

The article was received on 06 Aug 2013, accepted on 13 Sep 2013 and first published on 17 Sep 2013


Article type: Paper
DOI: 10.1039/C3CP53335B
Phys. Chem. Chem. Phys., 2013,15, 19686-19698

  •   Request permissions

    Experimental and modeling study of the oxidation of n-butane in a jet stirred reactor using cw-CRDS measurements

    C. Bahrini, P. Morajkar, C. Schoemaecker, O. Frottier, O. Herbinet, P. Glaude, F. Battin-Leclerc and C. Fittschen, Phys. Chem. Chem. Phys., 2013, 15, 19686
    DOI: 10.1039/C3CP53335B

Search articles by author

Spotlight

Advertisements