Laure Pillier

Quantitative Measurements of HO2 and Other Products of n-Butane Oxidation (H2O2, H2O, CH2O, and C2H4) at Elevated Temperatures by Direct Coupling of a Jet-Stirred Reactor with Sampling Nozzle and Cavity Ring-Down Spectroscopy (cw-CRDS)

For the first time quantitative measurements of the hydroperoxyl radical (HO2) in a jet-stirred reactor were performed thanks to a new experimental setup involving fast sampling and near-infrared cavity ring-down spectroscopy at low pressure. The experiments were performed at atmospheric pressure and over a range of temperatures (550-900 K) with n-butane, the simplest hydrocarbon fuel exhibiting cool flame oxidation chemistry which represents a key process for the auto-ignition in internal combustion engines. The same technique was also used to measure H2O2, H2O, CH2O, and C2H4 under the same conditions. This new setup brings new scientific horizons for characterizing complex reactive systems at elevated temperatures. Measuring HO2 formation from hydrocarbon oxidation is extremely important in determining the propensity of a fuel to follow chain-termination pathways from R + O2 compared to chain branching (leading to OH), helping to constrain and better validate detailed chemical kinetics models.

NO reburning study based on species quantification obtained by coupling LIF and cavity ring-down spectroscopy

NO reburning is studied in a low pressure (15 hPa) premixed flame of CH4-O2 seeded with 1.8% of NO. Measurements were carried out by using cavity ring-down spectroscopy (CRDS) and laser induced fluorescence (LIF) techniques. The temperature profile was obtained by OH-LIF thermometry in the A-X (0-0) band. The OH profile was determined by LIF and calibrated by single pass absorption. The NO concentration profile was obtained by LIF in the A-X (0-0) band and corrected for Boltzmann fraction and quantum yield variations. The absolute concentration profile was determined in the burned gases by CRDS allowing a direct experimental determination of the NO reburning amount. Finally CH and CN mole fraction profiles were obtained by CRDS by exciting rotational transitions in the B-X (0-0) bands of CH and CN around 387 nm. We found a peak mole fraction of 29 ppm for CH and 3.3 ppm for CN. This last result is in contrast with a previous study of W. Juchmann, H. Latzel, D. L. Shin, G. Peiter, T. Dreier, H. R. Volpp, J. Wolfrum, R. P. Lindstedt and K. M. Leung, XXVIIth Symposium (International) on Combustion, The Combustion Institute, Pittsburgh, 1998, p. 469, performed in a similar flame, which reported much lower levels of CN. In that study the absolute concentration of CN was indirectly obtained by LIF calibrated by Rayleigh scattering. In a second part, experimental species profiles are compared with predictions of the GRI 3.0 mechanism. Comparison between experimental and predicted profiles shows a good agreement particularly for CN and NO species. A qualitative analysis of NO reburning is then performed.

Premixed CH4/O2-enriched air combustion: Identification of thermal, chemical and aerodynamic effects

This work contributes to the evaluation of a new innovative process focused on the reduction of the cost of a post-combustion capture of CO2 in a Carbon Capture and Storage system (CCS). The process based on the separation of dried fumes composed mainly by CO2 and N2 by using membranes, which should lead to a lower energetic separation cost than amines. But the membranes become efficient if the upstream CO2 concentration is higher than 30% at their entrance that requires enriching the oxidizer flow by O2. To maintain the exhaust temperature compatible with materials thermal resistance, the reactants are diluted by a recirculation of a part of the flue gases (like N2/O2/CO2). But, the chemical kinetic, the energetic efficiencies, the radiation transfer, the transport and thermal properties of the flow can be affected by CO2. The objective of this work will be to identify the behaviour of the combustion of premixed CH4/O2-enriched air, both diluted in N2 and CO2 and to determine the combustion parameters. This allows to recover the CH4/air conditions in terms of CO2 concentration in reactants, O2 excess, dilution rate, temperature of the reactants, etc. Experiments are performed on the laminar premixed flame using counterflow burner. To characterize the combustion behaviour, the flammability limits are determined and flame thickness and position are measured from PLIF-OH diagnostic. Further, CHEMKIN simulations are performed to check the validity of the GRI3.0 chemical kinetic mechanism for premixed CH4/air synthetic combustion and identify the leading phenomena.