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Ignition in Convective-Diffusive Systems

Journal article published in 2 by Chung K. Law
This paper was not found in any repository; the policy of its publisher is unknown or unclear.
This paper was not found in any repository; the policy of its publisher is unknown or unclear.

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Abstract

The main goal of this work is understanding the controlling mechanisms and responses of forced ignition in an environment where chemistry and transport phenomena are intimately coupled. To analyze systematically this interaction the well-characterized counterflow configuration is selected whereupon a cold fuel jet impinges on a heated air jet, and ignites as the air temperature is raised gradually. In this configuration the ignition response is studied experimentally and numerically with extensive variations of the fuel dilution, flow strain rate, and ambient pressure, for hydrogen and Csb1{-}Csb4 paraffins. Experimentally, the temperatures are measured by thermocouple and Raman spectroscopy, while flow strain rates are determined through laser Doppler velocimetry. The experimental envelope comprises pressures of 0.1-8.0 atm, fuel concentrations from 0 to 100%, and strain rates between 50 and 700 ssp{-1}. Computations are performed using various detailed kinetic and transport models, whose adequacy is assessed by comparison with the experimental results. Through computational simulations, the controlling ignition mechanisms are isolated and analyzed. Simplified kinetic models are derived and evaluated, by using sensitivity/flux analyses and the Computational Singular Perturbation (CSP) method. The investigation demonstrates that the coupling chemistry-transport can produce unexpected responses, even for the arguably simplest Hsb2-air kinetic system. Here, up to three stable steady-states are identified experimentally for identical boundary conditions, corresponding to the distinct regimes of frozen flow, mild oxidation, and flaming combustion, respectively. These states can be accessed in a dual-staged ignition sequence, with radical runaway followed by thermokinetic ignition. The pattern, however, depends on the imposed parameters. Specifically, three ignition limits are found when pressure is varied; the first two are characterized by radical runaway only, whereas the third is thermokinetic in character, and may involve dual-staged ignition. The similarity with homogeneous pressure-temperature explosion limits is attributed to the dominance of similar chemistry. When this involves fast kinetics only the transport effects are minimal, such as occurs within the second limit. Conversely, the other two limits are transport-sensitive because of the relatively slower dominant chemistry. The homogeneous-heterogeneous analogy persists when studying the hydrocarbons. For example, increasing pressure uniformly facilitates ignition in both systems. The transport of heat and chemical species out of the reaction zone, however, requires higher temperatures for nonpremixed ignition. Furthermore, nonpremixed ignition is affected by preferential diffusion of light species such as Hsb2. As a result, the addition of relatively small amounts of hydrogen to the fuel jet dramatically reduces the ignition temperature for low ignitability fuels, such as methane. Finally, the presence of diffusive-convective losses results in a selection of the most efficient chemical branching modes. For hydrocarbons, this selection typically implies the dominance of high temperature kinetics, although the Csb4 alkanes show possible transition to a low-to-intermediate temperature branching mode in the limit of elevated pressures. Further research is suggested in this area, as well as in other related directions.