Thermal-pyrolysis induced over-driven flame and its potential role in the negative-temperature dependence of iso-octane flame speed at elevated temperatures

Abstract

Recently, high-temperature flame speed measurement up to 900 K has been successfully realized at Stanford University using a conventional shock tube, assisted by laser ignition and chemiluminescence image systems. For a near stoichiometric iso-octane/O2/N2/He mixture at atmospheric pressure, their results show that while flame speed increases with increasing unburnt temperature in the low and high-temperature range, it decreases with increasing unburnt temperature in the intermediate temperature regime (750–800 K). The measurement time for the flame initiation and propagation is orders of magnitude shorter than the first-stage ignition delay time, implying that the unburnt mixture upstream of the flame is largely chemically frozen. Therefore, such non-monotonic behavior in the flame speed is unlikely to be induced by autoignition chemistry. To understand this interesting phenomenon, 1-D transient simulation of spherical flame initiation and propagation with different ignition energy has been performed and compared with the experiment data. It is shown that for the relatively low ignition energy 7.5 mJ, an over-driven flame regime characterized by flame speeds and stretch rates well above the steady-state values occurs in the intermediate temperature range. The chemical structure of an over-driven flame involves substantial fuel thermal decomposition in the preheat zone, followed by C1-C4 oxidation in the reaction zone. It is found that the non-monotonicity in the observed flame speed is strongly correlated with the occurrence of over-driven flames in simulations. These results demonstrate a new flame structure which can potentially explain the observed non-monotonic flame speed for iso-octane at high temperatures. Higher ignition energy or smaller ignition kernel is suggested in future experiments to mitigate such over-driven effects.