Combustion and Flame 136 (2004) 371–376 www.elsevier.com/locate/jnlabr/cnf Measurement of propagation speeds in adiabatic flat and cellular premixed flames of C2H6 + O2 + CO2 A.A. Konnov ∗ and I.V. Dyakov Department of Mechanical Engineering, Vrije Universiteit Brussel, 1050 Brussels, Belgium Received 7 July 2003; received in revised form 14 November 2003; accepted 18 November 2003 Abstract Adiabatic burning velocities of premixed flat flames and propagation speeds of adiabatic cellular flames of mixtures of ethane + oxygen + carbon dioxide are reported. The oxygen content O2 /(O2 + CO2 ) in the artificial air was varied from 26 to 35%. Nonstretched flames were stabilized on a perforated plate burner at 1 atm. A heat flux method was used to determine burning velocities under conditions when the net heat loss of the flame is zero. Under specific experimental conditions the flames become cellular; this leads to significant modification of the flame propagation speed. Measurements in cellular flames are presented and compared with those for laminar flat flames and also with qualitative predictions of a theoretical model. The onset of cellularity was observed throughout the stoichiometric range of the mixtures studied. Cellularity disappears when the flames become only slightly subadiabatic. 2003 The Combustion Institute. Published by Elsevier Inc. All rights reserved. 1. Introduction Premixed planar flames stabilized on flat burners have often been used for experimental investigations of flame structure, since they resemble steady onedimensional adiabatic free flames propagating in the doubly infinite domain. In the laboratory, however, a planar flame is stabilized through losing heat to the surface of the burner, where fresh mixture is introduced. Then the flame becomes adiabatic only in the limiting case of zero heat loss to the burner when the flame turns unstable. The method proposed by Botha and Spalding [1] for the determination of the laminar burning velocity by linear extrapolation of the burning velocities to zero heat loss is based on this consideration. A limitation of this method manifested itself by the onset of cellular instability when the heat losses approached zero [1,2]. Botha and Spalding [1] described the appearance of these cells and noted that * Corresponding author. E-mail address: [email protected] (A.A. Konnov). the cellular flames propagate much faster than the corresponding laminar flat flames of the same composition. Using essentially the same technique, the cellular flame structures have been studied by Vantelon et al. [3] and by Gorman et al. [4–8]. The flames in all these studies were nonadiabatic. Major attention has been paid to classification and to quantification of the cellular patterns. These scarce experiments [1,3–8] have received significant attention from the combustion modeling community and have been frequently discussed [9–12]. It is important to note that cellular instability appears throughout the stoichiometric range of propane-air flames stabilized on a flat flame burner [1], contrary to the predictions of diffusivethermal [13–16] models or ones of preferential diffusion [10,17–20]. The onset of cellularity in these flames has been explained by hydrodynamic influences within the flame holder [12]. The importance of the coupling of diffusion and hydrodynamics has been emphasized by Markstein [9], and significant progress in the analytical investigation of the coupling problem has been achieved since then [21,22]. 0010-2180/$ – see front matter 2003 The Combustion Institute. Published by Elsevier Inc. All rights reserved. doi:10.1016/j.combustflame.2003.11.005 372 A.A. Konnov, I.V. Dyakov / Combustion and Flame 136 (2004) 371–376 A new method of adiabatic flame stabilization on a flat burner was introduced by de Goey et al. [23]. This method is based on balancing the heat loss required for flame stabilization with the convective heat flux from the burner surface to the flame front. It was demonstrated that the heat flux method is suitable for determining the adiabatic flame temperature and burning velocity [24–26]. Experimental measurements of the adiabatic burning velocity for laminar flat flames of methane + oxygen + carbon dioxide were reported recently [27]. It was noted that under specific experimental conditions these flames became cellular, leading to significant modification of the flame’s propagation speed [28]. The goal of the present work therefore was to extend these studies and to measure adiabatic propagation speeds of premixed flat and cellular flames of ethane + oxygen + carbon dioxide, stabilized using the heat flux method. In the following, an experimental installation is described. Then the experimental measurements in cellular flames are presented and compared with those for laminar flat flames and also with qualitative predictions of a theoretical model [12]. 2. Experimental details The experimental setup for stabilizing an adiabatic flame using the heat flux method has been described elsewhere [26,29]; however, the most relevant details are repeated below. The scheme of the burner is shown in Fig. 1. It consisted of the burner head mounted on a plenum chamber. The 2-mm-thick burner plate perforated with small holes was attached to the burner outlet. The burner mouth had a diameter of 30 mm and a heating jacked supplied with thermostated water to keep the temperature of the burner plate constant. Recent measurements of the burning velocity in mixtures of ethane + oxygen + nitrogen [30] were performed with the heating jacket at 353 K. However, at this temperature flames of ethane + oxygen + carbon dioxide were unstable with a clear cellular instability. Increasing the temperature of the burner plate suppressed this instability; lowering the temperature of the burner plate extended the range of equivalence ratios over which the cellularity was observed. In the present experiments this temperature was fixed at 368, 353, or 338 K, as described below. The plenum chamber had a separate cooling system supplied with water at a temperature of 298 K to control the initial temperature of a mixture. The heating jacket kept the edges of the burner plate at a certain temperature higher than the initial gas temperature, thus warming up the unburned gases flowing through. If the flame was stabilized under subadiabatic conditions, the gas velocity Fig. 1. The perforated plate burner. was lower than the adiabatic flame burning velocity and the sum of the heat loss and heat gain was higher than zero. Then the center of the burner plate was hotter than the heating jacket. If the unburned gas velocity was higher than the adiabatic burning velocity (superadiabatic conditions), the net heat flux was lower than zero, and the center of the burner plate was cooler than the heating jacket. By changing the flow rate of the gas mixture, an appropriate value of the gas velocity could be found to nullify the net heat flux. In this case the radial temperature distribution in the burner plate was uniform and equal to the temperature of the heating jacket. Experimentally the series of thermocouples attached to the burner plate allowed the temperature distribution in it to be measured. The flow rate at which the net heat flux was zero was shown to be an adiabatic flame burning velocity [24]. A schematic illustration of the principle of flame stabilization using the heat flux method is shown in Fig. 2. It displays an adiabatic flame temperature profile and position of the flame front, which in the present work was flat or wrinkled. The reference plane in this case is the burner surface, which was heated to some fixed temperature, as noted above. The physical properties of the flat flame were identical to those of the flat freely propagating adiabatic flame [23]. Variation of the burner plate’s temperature led to a tiny change in the position of the flame front. An increase of this temperature from 338 to 368 K shifted the flame by only 0.05 mm along the calculated adiabatic flame temperature profile (see Fig. 2). This physical principle of flame stabilization resembles the computational principle of the adiabatic flame stabilization in the infinite domain employed in the Premix code [31]. By fixing the temperature at one point in the flame-fixed coordinate system (keyword A.A. Konnov, I.V. Dyakov / Combustion and Flame 136 (2004) 371–376 Fig. 2. Schematic illustration of the principle of the flame stabilization using the heat flux method. Solid line, adiabatic temperature profile; vertical dashed line, arbitrary position of the burner plate; hatched area, flame front. TFIX), the program calculated the flame’s burning velocity as an eigenvalue. When the flame was wrinkled, the concave and convex regions of it were stabilized at different distances from the burner plate; also the heat fluxes from these regions were different and the local temperature profiles were generally different, because preferential diffusion changed the local composition. In this case the radial temperature distribution in the burner plate was locally nonuniform, but was approximated by a parabolic fit [32], and by changing the flow rate of the gas mixture, an appropriate value of the gas velocity was found to make the average radial temperature distribution in the burner plate uniform and to nullify the net heat flux. The cellular flame was, therefore, adiabatic since the net heat loss from the flame to the burner is zero. The corresponding flow rate of the gas mixture in the following is referred to as the propagation speed of an adiabatic cellular flame. One should note that the propagation speed of an adiabatic cellular flame is not a characteristic of the mixture, unlike the adiabatic burning velocity of a flat flame. It has been realized and discussed long ago (e.g., [9,13,14, 18]) that due to changes of the local temperature and mixture composition, the concave and convex regions of the wrinkled flame have different local burning velocities. In the present experiments the number of cells varied from 15 to 65; thus, the propagation speed of a cellular flame was an averaged value over the ensemble of cells. The stabilized flames employing the heat flux method resembled steady one-dimensional adiabaticfree flames inasmuch as the heat flux from the flame to the burner was zero. However, due to the finite size 373 of a flame, the influence of ambient conditions was not negligible. The development and testing of the installation used in the present study, together with an analysis of errors in apparent burning velocities, have been described earlier [26]. The overall accuracy of a measured burning velocity was estimated to be better than ±0.8 cm/s (double standard deviation with 95% confidence level) over the whole range of velocities from about 10 to 40 cm/s. The relative accuracy of the equivalence ratio was ±0.54%. To achieve this accuracy, the installation was calibrated before each experimental run [26]. The uncertainties on a long-term basis were found to be somewhat higher (±1% for equivalence ratio and ±1 cm/s for burning velocities in rich and lean mixtures) [32]. The experimental measurements of the adiabatic burning velocity for methane + oxygen + nitrogen and for ethane + oxygen + nitrogen were found to be in very good agreement with the literature [26,30]. The pure gases were used as delivered by the supplier. The stated purity of ethane, oxygen, and carbon dioxide was 99.995% or better. 3. Modeling details A detailed C/H/N/O reaction mechanism for the combustion of small hydrocarbons was used for the adiabatic flame modeling [33]. The current version of the mechanism (Release 0.5) consisted of 1200 reactions of 127 species. This mechanism has been validated with experimental measurements for the oxidation, ignition, and flame structure of hydrogen, carbon monoxide, formaldehyde, methanol, methane, ethane, propane, and some of their mixtures. The CHEMKIN-II collection of codes [31,34,35], including transport properties [36] from Sandia National Laboratories, was used. Multicomponent diffusion and thermal diffusion options were taken into account. Adaptive mesh parameters were GRAD = 0.1 and CURV = 0.5. 4. Results and discussion As noted above, the burner plate’s temperature defined the appearance of a flame. In mixtures of CH4 + O2 + CO2 [28] it was observed that when the temperature was fixed at 368 K, the flame stabilized closer to the surface, making the flame perfectly flat for any dilution ratio D = O2 /(O2 + CO2 ). In the present work measurements were performed in mixtures of C2 H6 + O2 + CO2 with the dilution ratio D equal to 0.26, 0.29, 0.3155, and 0.35. At higher dilution ratios (0.3155 and 0.35) the flames were corrugated, even with the burner plate at its 374 A.A. Konnov, I.V. Dyakov / Combustion and Flame 136 (2004) 371–376 Fig. 3. Adiabatic burning velocities in C2 H6 + O2 + CO2 flames with different dilution ratios (D) at standard temperature (298 K) and pressure. Symbols, experiment; lines, modeling. Solid line, D = 35%; dashed line, D = 31.55%; dash-dot line and crosses, D = 29%; dash-dot-dot line and squares, D = 26%. hottest (368 K). Only at lower dilution ratios (0.26 and 0.29) could the adiabatic burning velocity in a laminar flat flame be determined. The measurements and calculated adiabatic burning velocities in flames of C2 H6 + O2 + CO2 with different dilution ratios are shown in Fig. 3. The overall agreement between the experiment and the modeling is very good over the whole range of equivalence ratios for D equal to 0.26 and 0.29. The deviations of the calculations from the experiments exceeded the evaluated uncertainty of the heat flux method (±0.8 cm/s) only in the richest, highly diluted mixtures. Taking into account the good performance of the detailed reaction mechanism shown in diluted mixtures and also in C2 H6 + O2 + N2 (Ar) flames [30], one can assume that the calculated adiabatic burning velocities in flames of C2 H6 + O2 + CO2 with D = 0.3155 and 0.35 (solid and dashed lines in Fig. 3) are accurate. These calculated burning velocities are compared with the propagation speeds of adiabatic cellular flames in the following. All the experimental measurements in flames having dilution ratios of 0.35 and 0.3155 are summarized in Figs. 4 and 5, respectively. First, the calculated laminar adiabatic burning velocities shown in Fig. 3 are repeated as lines for comparison. Also shown are the propagation speeds of the adiabatic cellular flames with the burner plate at 338 or 353 K. These burning velocities are systematically higher than in laminar flat flames; the difference is more pronounced at lower temperatures of stabilization. To observe a transition between the cellular and flat flames, similar Fig. 4. Burning velocities in C2 H6 + O2 + CO2 flames with dilution ratio D = 35% at standard temperature (298 K) and pressure. Line, laminar adiabatic burning velocity (cf. Fig. 3); solid diamonds and solid squares, propagation speeds of the adiabatic cellular flames at the burner plate temperature of 338 and 353 K, respectively; open diamonds and open squares, propagation speeds of the subadiabatic flat flames at the burner plate temperature of 338 and 353 K, respectively. Fig. 5. Burning velocities in C2 H6 + O2 + CO2 flames with dilution ratio D = 31.55% at standard temperature (298 K) and pressure. Line, laminar adiabatic burning velocity (cf. Fig. 3); solid diamonds and solid squares, propagation speeds of the adiabatic cellular flames at the burner plate temperature of 338 and 353 K, respectively; open diamonds and open squares, propagation speeds of the subadiabatic flat flames at the burner plate temperature of 338 and 353 K, respectively. A.A. Konnov, I.V. Dyakov / Combustion and Flame 136 (2004) 371–376 to that found by Botha and Spalding [1], the velocity of the fresh gas mixture was gradually reduced until the moment when the flame was flattened out. These velocities are denoted in Figs. 4 and 5 as the propagation speeds of the subadiabatic flat flames, also at the burner plate temperature of 338 and 353 K. In agreement with earlier experiments [1] and with theoretical predictions [12], the onset of cellularity was observed throughout the stoichiometric range. In addition, the cellularity disappeared when a flame became only slightly subadiabatic. The perforated plate flame holder therefore served to stabilize a flat flame when the flame approached it due to a reduction in the velocity of the fresh mixture or due to an increase of the burner plate’s temperature. In the last case the flame was still adiabatic, since the net heat loss of the flame was zero. The theoretical model [12] showed that for hypodermic-type flame holders, where transverse velocities are not allowed, the instability is removed for subadiabatic conditions. The perforated plate burner used in the present study can be considered as an intermediate case between the porousplug and the hypodermic-type flame holders. Therefore any comparison of theory with an experiment can only be qualitative. Similar to observations in mixtures of CH4 + O2 + CO2 [28], the propagation speeds of adiabatic cellular flames shown in Figs. 4 and 5 depend on the burner plate’s temperature. One can expect that in the limit of the burner plate’s temperature approaching the temperature of the initial mixture (298 K), the structure and the propagation speeds would approach those of the “free” or quasistabilized flames, extensively studied in vertical wide tubes [9]. Unfortunately, due to the limitations of the heat flux method, these flames cannot be stabilized on a flat flame burner, and direct comparison with the numerous studies of the quasi-stabilized flames is impossible. Visual observations of the flames were performed to compare their cellular structure with that in mixtures of CH4 + O2 + CO2 [28]. It was noted that the appearance of the cells varies with equivalence ratio, dilution by CO2 , and the temperature of the burner plate. In rich mixtures with an equivalence ratio 1.7–1.8, the flame broke down to form a number of individual cells. These cells had the shape of a hemisphere convex toward the fresh mixture and were separated by nonluminous relatively wide zones. Similar cells have been observed in lean flames of methane [28]. When the mixture composition was changed toward the stoichiometric one or when the temperature of the burner plate was increased, the cells joined to form a continuous corrugated flame front. The cells in lean mixtures were usually asymmetric and possessed different sizes. In many cases, especially in very lean or very rich mixtures, the cells 375 in the center of the flame and on the edges differed in size dramatically. The variation of the appearance of ethane flames with equivalence ratio inversely mirrored that of methane flames. This is not surprising, since the diffusion coefficients of methane and ethane are respectively higher and lower than that of oxygen. One can assume therefore that the cells observed in rich mixtures of ethane and in lean mixtures of methane were formed mostly due to the diffusivethermal instability. In the opposite case of lean ethane and rich methane flames, the mechanism of instability was probably mostly hydrodynamic in nature. The cellular structure of the flames was obviously sensitive to any nonuniformity in the flow and to the local mixture composition. Entrainment of the ambient air caused dilution of the burnt gases in very lean mixtures, while in very rich mixtures it caused oxidation of the combustion products [29]. These nonidealities led to disparities in the cell size in the center and on the edges of the burner. Sometimes jumping changes of the cellularity picture were observed. 5. Conclusions This work extends that performed with mixtures of CH4 + O2 + CO2 [28]. For the first time adiabatic burning velocities of premixed flat flames are reported, together with propagation speeds of adiabatic cellular flames of ethane + oxygen + carbon dioxide. The propagation speeds of cellular flames with the burner plate at 338 and 353 K were systematically higher than those in laminar flat flames. The difference is more pronounced at lower temperatures of stabilization. In agreement with earlier experiments [1] and with theoretical predictions [12], the onset of cellularity was observed throughout the stoichiometric range. In addition, the cellularity disappeared when a flame became only slightly subadiabatic. The perforated plate flame holder therefore served as a flat flame stabilizer when the flame approached it, due to a reduction of the velocity of the fresh mixture or due to an increase of the burner plate’s temperature. 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