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1.
An experimental and numerical investigation of counterflow prevaporized partially premixed n-heptane flames is reported. The major objective is to provide well-resolved experimental data regarding the detailed structure and emission characteristics of these flames, including profiles of C1-C6, and aromatic species (benzene and toluene) that play an important role in soot formation. n-Heptane is considered a surrogate for liquid hydrocarbon fuels used in many propulsion and power generation systems. A counterflow geometry is employed, since it provides a nearly one-dimensional flat flame that facilitates both detailed measurements and simulations using comprehensive chemistry and transport models. The measurements are compared with predictions using a detailed n-heptane oxidation mechanism that includes the chemistry of NOx and PAH formation. The reaction mechanism was synergistically improved using pathway analysis and measured benzene profiles and then used to characterize the effects of partial premixing and strain rate on the flame structure and the production of NOx and soot precursors. Measurements and predictions exhibit excellent agreement for temperature and major species profiles (N2, O2, n-C7H16, CO2, CO, H2), and reasonably good agreement for intermediate (CH4, C2H4, C2H2, C3Hx) and higher hydrocarbon species (C4H8, C4H6, C4H4, C4H2, C5H10, C6H12) and aromatic species (toluene and benzene). Both the measurements and predictions also indicate the existence of two partially premixed regimes; a double flame regime for ?<5.0, characterized by spatially separated rich premixed and nonpremixed reaction zones, and a merged flame regime for ?>5.0. The NOx and soot precursor emissions exhibit strong dependence on partial premixing and strain rate in the first regime and relatively weak dependence in the second regime. At higher levels of partial premixing, NOx emission is increased due to increased residence time and higher peak temperature. In contrast, the emissions of acetylene and PAH species are reduced by partial premixing because their peak locations move away from the stagnation plane, resulting in lower residence time, and the increased amount of oxygen in the system drives the reactions to the oxidation pathways. The effects of partial premixing and strain rate on the production of PAH species become progressively stronger as the number of aromatic rings increases.  相似文献   

2.
We investigate the effects of hydrogen addition on Fenimore NO formation in fuel-rich, low-pressure burner-stabilized CH4/O2/N2 flames. Towards this end, axial profiles of temperature and mole fractions of CH and NO are measured using laser-induced fluorescence (LIF). The experiments are performed at equivalent ratios of 1.3 and 1.5, using 0.25 mole fraction of hydrogen in the fuel, while varying the mass flux through the burner. The results are compared with those reported previously for burner-stabilized CH4/O2/N2 flames. The increased burning velocity caused by hydrogen addition is seen to result in a lower flame temperature as compared to methane flame stabilized at the same mass flux. This increase in burner stabilization upon hydrogen addition results in significantly lower CH mole fractions at φ = 1.3, but appears to have little effect on the CH profile at φ = 1.5. In addition, the results show that not only the maximum flame temperature is reduced upon hydrogen addition, but the local gas temperature in the region of the CH profile is lowered as well. The measured NO mole fractions are seen to decrease substantially for both equivalence ratios. Analysis of the factors responsible for Fenimore NO formation shows the reduction in temperature in the flame front to be the major factor in the decrease in NO mole fraction, with a significant contribution from the decrease in CH mole fraction at φ = 1.3. At φ = 1.5, the results suggest that the lower flame temperature upon hydrogen addition further retards the conversion of residual fixed-nitrogen species to NO under these rich conditions as compared to the equivalent methane flames.  相似文献   

3.
Velocities of reactive and non‐reactive flows, where NO2 molecules were seeded, were measured by a NO‐based Laser Induced Fluorescence (LIF) method. NO2 dilute gases were injected from a round tube with an inner diameter of 2 cm and its flow rate was 10 liters/minute or 20 liters/minute. Experiments were performed for 4 conditions—non‐reactive flows of NO2 dilute gases at two flow rates, an unburnt gas flow of the premixed flame with NO2 addition, and an unburnt gas flow of the diffusion flame with NO2 addition. NO molecules were produced in flows by planar emissions of 355 nm laser rays from an Nd:YAG laser system, and NO‐LIF images were taken in a pre‐determined delay. An ICCD camera, a dye laser excited by an excimer laser, and Nd:YAG laser were strictly synchronized by a pulse generator. NO‐LIF signals, which were emitted by photochemically produced NO from NO2, were strong enough to measure the NO displacements in the case of non‐reactive flows, while with only a few ppm concentrations of NO2 added it was possible to measure the velocity in detail. Although fluctuations of NO trajectories were observed at the flow rate of 20 liters/minute, instantaneous velocities were measured accurately. In the case of the unburnt gas of the diffusion flame, NO‐LIF signals were also strong, and profiles of NO produced by NO2 photodissociation were clearly measured. Profiles of NO produced by NO2 photodissociation in the unburnt gas of the premixed flame were also clearly measured, even in the vicinity of the reaction zone. It can be seen that velocities were measured correctly in the unburnt regions of the premixed and the diffusion flames. With this method, it was possible to measure velocities of both steady and unsteady flows. © 2004 Wiley Periodicals, Inc. Heat Trans Asian Res, 34(1): 40–52, 2005; Published online in Wiley InterScience ( www.interscience.wiley.com ). DOI 10.1002/htj.20038  相似文献   

4.
The impact of dimethyl methylphosphonate (DMMP) was studied in a premixed methane/oxygen/N2-Ar flame in a flat flame burner slightly under atmospheric pressure at two different equivalence ratios: rich and slightly lean. CH4, CO, CO2, CH2O, CH3OH, C2H6, C2H4, and C2H2 profiles were obtained with a Fourier Transform Infrared (FTIR) spectrometer. Gas samples, analyzed in the FTIR, were extracted from the reaction zone using a quartz microprobe with choked flow at its orifice. Temperature profiles were obtained by measuring the probe flow rate through the choked orifice. Flame calculations were performed with two existing detailed chemical kinetic mechanisms for organophosphorus combustion. DMMP addition caused all profiles except that of CH3OH to move further away from the burner surface, which can be interpreted as a consequence of a reduction in the adiabatic flame speed. Experimentally, the magnitude of the shift was 50% greater for the near-stoichiometric flame than for the rich flame. Experimental CH3OH profiles were four to seven times higher in the doped flames than in the undoped ones. The magnitude of this effect is not predicted in the calculations, suggesting a need for further mechanism development. Otherwise, the two mechanisms are reasonably successful in predicting the effects of DMMP on the flame.  相似文献   

5.
In the present work, the effects of blending dimethyl ether (DME) and hydrogen (H2) with methane (CH4) have been numerically studied in the context of counterflow diffusion flames. In order to do so, a reaction mechanism consisting of 974 reaction steps among 146 species with updated thermodynamic and transport properties has been developed. This mechanism has been validated against the experimental data on laminar burning velocity, ignition delay time and species profiles in counterflow diffusion flames. The present study suggests that the heat release pattern of the CH4 counter flow diffusion flame shows major changes when DME and H2 are present in the fuel stream. Furthermore, the results show that the presence of low volume fractions of DME in CH4 increases the formation of benzene (C6H6) in the flame. This fact can be negated by the presence of H2 together with CH4 and DME in the fuel stream. Moreover, the present study suggests that H2 mitigates the C6H6 formation in the CH4 diffusion flame with greater effectiveness compared to DME. Contrary to the popular belief, the main reason behind such efficacy of H2 has been found to be physical rather than chemical. On the other hand, the NO production routes are primarily dominated by the Zeldovich mechanism in the flames involving CH4, DME and H2 blends. In this regard, the present analysis suggests that the simultaneous presence of DME and H2 in CH4 effectively prevents the formation of NO in the flame.  相似文献   

6.
Species concentration measurements specifically those associated with nitrogen oxides (NOx) can act as important validation targets for developing kinetic models to predict NOx emissions under syngas combustion accurately. In the present study, premixed combustion of syngas/air mixtures, with equivalence ratio (Φ) from 0.5 to 1.0 and H2/CO ratio from 0.25 to 1.0 was conducted in a McKenna burner operating at atmospheric pressure. Temperature and NOx concentrations were measured in the post-combustion zone. For a given H2/CO ratio, increasing the equivalence ratio from lean to stoichiometric resulted in an increase in NO and decrease in NO2 concentration near the flame. Increasing the H2/CO ratio led to a decrease in the temperature as well as the NO concentration near the flame. Based on the axial profiles above the burner, NO concentration increases right above the flame while NO2 concentration decreases through NO2-NO conversion reactions according to the path flux analysis. In addition, the present experiments were operated in the laminar region where multidimensional transport effects play significant roles. In order to account for the radial and axial diffusive and convective coupling to chemical kinetics in laminar flow, a multidimensional model was developed to simulate the post-combustion species and temperature distribution. The measurements were compared against both multidimensional computational fluid dynamics (CFD) simulations and one-dimensional burner-stabilized flame simulations. The multidimensional model predictions resulted in a better agreement with the measurements, clearly highlighting the effect of multidimensional transport.  相似文献   

7.
OH radical profiles were measured in the near-deposition-surface region in low-pressure, stagnation-flow diamond-forming flames using laser-induced fluorescence (LIF). The objective of these measurements was to explore the chemistry of the diamond chemical-vapor deposition (CVD) process by resolving the OH profile near the deposition substrate. Detailed OH LIF measurements were performed in stagnation-flow diamond-forming C2H2/O2 flames with equivalence ratios of 1.80, 2.10, and 2.32. The flame with an equivalence ratio of 1.80 exhibited no diamond film growth, while the flame with an equivalence ratio of 2.32 exhibited significant diamond film growth. The LIF measurements were performed in the linear LIF regime and the laser frequency was scanned across the spectral profile of the P1(3) line in the (1,0) band of the A2Σ+-X2Π electronic transition at each spatial location. In earlier H2 CARS measurements, the temperature gradients near the deposition substrate were resolved and good agreement between the measured temperature profiles and the numerical modeling results was demonstrated. The measured LIF profiles were corrected for electronic quenching and the variation of the Boltzmann fraction with temperature. Major species profiles were calculated using the results of the numerical flame code. The laser beam spatial profile was accounted for by convolving the theoretical OH profiles from the numerical model with the measured laser beam profile. The experimental OH profiles for all three cases are compared with theoretical results calculated using a stagnation-flame model that includes the diamond-formation surface chemistry. The measured OH concentrations near the deposition surface are substantially lower than theoretical results from a flame model that does not include the surface chemistry, but somewhat higher than for the model that does include the diamond-formation surface chemistry, especially for the flames with equivalence ratios of 1.80 and 2.10. The measured OH profile for the flame with an equivalence ratio of 2.32 is in good agreement with the profile calculated using a theoretical model with diamond-formation surface chemistry.  相似文献   

8.
The effects of hydrogen addition on NO formation in fuel-rich, burner-stabilized methane, ethane and propane flames are reported. Profiles of temperature and NO mole fraction were obtained using spontaneous Raman scattering and laser-induced fluorescence (LIF), respectively. Experiments were performed at equivalent ratio of 1.3, with 0 and 0.2 mole fraction of hydrogen in the fuel; and the mass flux through the burner was varied for each mixture. The addition of hydrogen only modestly affects the flame temperature and NO mole fraction. For the vast majority of the flames studied, the temperature and NO decrease by less than 40 K and 20% (relative), respectively, upon hydrogen addition. The decrease in NO fraction is more distinct in methane and propane flames, and more modest for ethane. The comparison of the experimental data obtained for a given fuel in near-adiabatic CnH2n+2/H2/O2/N2 and burner-stabilized CnH2n+2/Air flames shows that the NO mole fraction at a given mass flux is practically independent of the composition of the oxidizer. Comparison of the experimental profiles with the predictions of one-dimensional flame calculations with detailed chemical mechanisms indicates that the decrease in the Fenimore NO formation with hydrogen addition arises from the concomitant decrease in CH fraction. Analysis of the computational results suggests that the reaction NCN + H → CH + N2 returns a considerable fraction of NCN back to N2.  相似文献   

9.
Numerical study with detailed chemistry has been conducted to investigate the effect of CO2 addition on flame structure and NOx formation in CH4–air counterflow diffusion flame. Radiation effect is found to be dominant especially at low strain rates. The addition of CO2 makes radiation effect more remarkable even at high‐strain rates. It is, as a result, seen that flame structure is determined by the competition between the radiation and strain rate effects. The important role of CO2 addition is addressed to thermal and chemical reaction effects, which can be precisely specified through the introduction of an imaginary species. Thermal effect contributes to the changes in flame structure and NO formation mainly, but the effect of chemical reaction cannot be neglected. It is noted that flame structure is changed considerably due to the addition of CO2, in such a manner, that the path of methane oxidation prefers to take CH4→CH3→C2H6→C2H5 instead of CH4→CH3→CH2→CH. Copyright © 2001 John Wiley & Sons, Ltd.  相似文献   

10.
To better understand the chemistry involved in the combustion of components of diesel fuel, the structure of a laminar lean premixed methane flame doped with n-butylbenzene has been investigated. The inlet gases contained 7.1% (molar) methane, 36.8% oxygen, and 0.96% n-butylbenzene corresponding to an equivalence ratio of 0.74 and a ratio C10H14/CH4 of 13.5%. The flame has been stabilized on a burner at a pressure of 6.7 kPa using argon as diluent, with a gas velocity at the burner of 49.2 cm/s at 333 K. Quantified species included the usual methane C0-C2 combustion products, but also 16 C3-C5 hydrocarbons, and 7 C1-C3 oxygenated compounds, as well as 20 aromatic products. A new mechanism for the oxidation of n-butylbenzene is proposed whose predictions are in satisfactory agreement with measured species profiles in flames and flow reactor experiments. The main reaction pathways of consumption of n-butylbenzene have been derived from flow rate analyses.  相似文献   

11.
This article sheds light on the combustion characteristics of dimethyl ether and its mixtures with methane/hydrogen under flameless conditions at different equivalence ratios. It was found that combustion of 100% dimethyl ether in flameless conditions minimises the NO formation, keeping it less than 10 ppm with no CO or unburned hydrocarbons. Progressive addition of methane was found to reduce the NO, reaching up to zero value at 50% methane in molar fraction along with a marginal CO2 reduction. However, large amounts of CO were found for higher methane levels, greater than 60% CH4 in molar fraction. Reactive structures based on OH1 chemiluminescence revealed that adding methane results in increased ignition delay times and, consequently, a more distributed reaction zone characterised by reduced temperature gradients. No visible flame was observed for pure dimethyl ether as well as dimethyl ether/methane mixtures. Furthermore, a more intense and narrower reaction zone, characterised by the presence of a visible flame, was formed upon hydrogen addition. Adding hydrogen by 50% in molar fraction did not cause a noticeable rise in NO levels; however, CO2 was lowered by about 18%. Further addition of hydrogen resulted in increased peak temperatures of about 1700 K and higher NO emissions of about 50 ppm. Additionally, a skeletal Chemical Reactor Network was built and simulated with the commercial software CHEMKIN Pro to investigate the effect of the different mixtures and operating conditions on NO formation from a chemical point of view. N2O pathway was observed to be the root source of NO emissions for pure DME and DME/CH4 mixtures, however; the thermal pathway became gradually more important as hydrogen concentration was increased in the mixture.  相似文献   

12.
The present study has been motivated by the need to understand and predict fuel-nitrogen conversion in the combustion of biomass-derived fuels. Within that broader context, an earlier related publication (Lucassen et al., Proc. Combust. Inst. 32 (2009) 1269–1276) has investigated morpholine (C4H9NO, 1-oxa-4-aza-cyclohexane) as a model oxygen- and nitrogen-containing biofuel, and species identification was presented for a slightly fuel-rich Φ = 1.3 (C/O = 0.41) laminar premixed morpholine-oxygen-argon flame at 40 mbar. To attempt a more detailed insight into the flame structure and combustion mechanism, the present contribution has now combined photoionization (PI) and electron ionization (EI) molecular-beam mass spectrometry (MBMS) to determine absolute mole-fraction profiles of numerous major and intermediate species with up to 6 heavy atoms. In general, PI-MBMS and EI-MBMS results were found in good agreement. The results reveal formation of a number of intermediates that may contribute to harmful emissions, including aldehydes and several nitrogen-containing compounds in percent-level concentrations. Both NH3 and HCN pathways are seen to contribute to NO formation.To identify reaction pathways for this detailed experimental analysis, development of a flame model was started, considering a combustion mechanism for cyclohexane and analogous fuel-breakdown reactions for morpholine by addition of necessary thermodynamic, transport and kinetic parameters. The present model captures relevant features of the morpholine flame quite well, including HCN, N2, and NO, and it can serve as a nucleus for further development of detailed combustion models for fuel-nitrogen conversion from model biofuel compounds.  相似文献   

13.
Ammonia, made up of 17.8% hydrogen, has attracted a lot of attention in combustion community due to its zero carbon emission as a fuel in gas turbines. However, ammonia combustion still faces some challenges including the weak combustion and sharp NOx emissions which discourage its application. It was demonstrated that the combustion intensity of ammonia/air flame can be enhanced through adding active fuels like methane and hydrogen, while the NOx emission issue will emerge in the meantime. This study investigates regulation effect of methane and hydrogen on the emission characteristics of ammonia/air flame in a gas turbine combustor. The instantaneous OH profile and global emissions at the combustion chamber outlet are measured with Planar Laser Induced Fluorescence (PLIF) technique and the Fourier Transform Infrared (FTIR), respectively. The flames are also simulated by large eddy simulation to further reveal physical and chemical processes of the emissions formation. Results show that for NH3/air flames, the emissions behavior of the gas turbine combustor is similar to the calculated one-dimensional flames. Moreover, the NOx emissions and the unburned NH3 can be simultaneously controlled to a proper value at the equivalence ratio (φ) of approximate 1.1. The variation of NO and NO2 with φ for NH3/H2/air flames and NH3/CH4/air flames at blending ratio (Zf) of 0.1 are similar to the NH3/air flames, with the peak moving towards rich condition. This indicates that the NH3/air flame can be regulated through adding a small amount of active fuels without increasing the NOx emission level. However, when Zf = 0.3, we observe a clear large NOx emission and CO for NH3/CH4/air flames, indicating H2 is a better choice on the emission control. The LES results show that NO and OH radicals exhibit a general positive correlation. And the temperature plays a secondary role in promoting NOx formation comparing with CH4/air flame.  相似文献   

14.
The stoichiometric methane–hydrogen–air freely propagated laminar premixed flames at normal temperature and pressure were calculated by using PREMIX code of CHEMKIN II program with GRI-Mech 3.0 mechanism. The mole fraction profiles and the rate of production of the dominant reactions contributing to the major species and some selected intermediate species in the flames of methane–hydrogen–air were obtained. The rate of production analysis was conducted and the effect of hydrogen addition on the reactions of methane–air mixtures combustion was analyzed by the dominant elementary reactions for specific species. The results showed that the mole fractions of major species CH4, CO and CO2 were decreased while their normalized values were increased as hydrogen is added. The rate of production of the dominant reactions contributing to CH4, CO and CO2 shows a remarkable increase as hydrogen is added. The role of H2 in the flame will change from an intermediate species to a reactant when hydrogen fraction in the blends exceeds 20%. The enhancement of combustion with hydrogen addition can be ascribed to the significant increase of H, O and OH in the flame as hydrogen is presented. The decrease of the mole fractions of CH2O and CH3CHO with hydrogen addition suggests a potential in the reduction of aldehydes emissions of methane combustion as hydrogen is added. The methane oxidation reaction pathways will move toward the lower carbon reaction pathways when hydrogen is available and this has the potential in reducing the soot formation. Chemical kinetics effect of hydrogen addition has a little influence on NO formation for methane combustion with hydrogen addition.  相似文献   

15.
A numerical study has been conducted to clearly grasp the impact of chemical effects caused by added CO2 and of flame location on flame structure and NO emission behaviour. Flame location affects the major source reaction of CO formation, CO2+H→CO+OH and the H‐removal reaction, CH4+H→CH3+H2. It is, as a result, seen that the reduction of maximum flame temperature due to chemical effects for fuel‐side dilution is mainly caused by the competition of the principal chain branching reaction with the reaction, CH4+H→CH3+H2, while that for fuel‐side dilution is attributed to the competition of the principal chain branching reaction with the reaction, CO2+H→CO+OH. The importance of the NNH mechanism for NO production, where the reaction pathway is NNH→NH→HNO, is recognized. In C‐related reactions most of NO is the direct outcome of (R171) and the contribution of (R171) becomes more and more important with increasing amount of added CO2 as much as the reaction step (R171) competes with the key reaction of thermal mechanism, (R237), for N atom. This indicates a possibility that NO emission in hydrogen flames diluted with CO2 shows less dependent behaviour upon flame temperature. Copyright © 2004 John Wiley & Sons, Ltd.  相似文献   

16.
The effect of hydrocarbon addition on tip opening of lean and stoichiometric hydrogen-air flames is studied computationally by performing two-dimensional numerical simulations. The numerical study reveals that the flame tip of the H2-air burner stabilized flame is open at lean and stoichiometric mixture conditions. The flame tip closes upon hydrocarbon addition. The tip closing is mainly affected by preferential diffusion of the multi-component mixture and the stretch effects. In the addition of light hydrocarbon (CH4), the tip closing starts at a higher percentage of hydrocarbon addition in H2-air flames. Whereas, upon the addition of heavy hydrocarbons such as propane and butane in H2-air flames, tip closing starts with a lesser amount of hydrocarbon addition. Temperature, OH mole fraction and heat release rate have been investigated, focusing on the flame structure at the tip. The tip opening regime diagram for H2–CH4-air, H2–C3H8-air and H2–C4H10-air mixtures are presented.  相似文献   

17.
18.
The effect of CO2/N2/CH4 dilution on NO formation in laminar coflow H2/CO syngas diffusion flames was experimentally and numerically investigated. The results reveal that the NO emission index increases with H2/CO mole ratio. In all cases, CO2/N2/CH4 dilution can reduce the peak temperature of syngas flame and have the ability to reduce peak flame temperature is decreased in the following order: CO2>N2>CH4. CO2/N2 dilution reduces the NO formation in syngas flame while CH4 dilution promotes the NO formation. Besides, the dilution of CO2/N2/CH4 can reduce the peak mole fraction of OH and its variations with H2/CO mole ratio and dilution ratio show the same trend as the peak flame temperature variations. The height of the flame with CO2 and N2 dilution increases with dilution ratio. The flame with CH4 dilution becomes higher and wider with the increase of dilution ratio.  相似文献   

19.
In this work, extensive chemical kinetic modeling is performed to analyze the combustion and emissions characteristics of premixed NH3/CH4–O2/N2/H2O2 mixtures at different replacement percentages of air with hydrogen peroxide (H2O2). This work is comprehensively discusses the ignition delay time, flame speed, heat release rate, and NOx & CO emissions of premixed NH3/CH4–O2/N2/H2O2 mixtures. Important intermediate crucial radicals such as OH, HO2, HCO, and HNO effect on the above-mentioned parameters is also discussed in detail. Furthermore, correlations were obtained for the laminar flame speed, NO, and CO emissions with important radicals such as OH, HO2, HCO, and HNO. The replacement of air with H2O2 increases flame speed and decreases the ignition delay time of the mixture significantly. Also, increases the CO and NOx concentration in the products. The CO and NOx emissions can be controlled by regulating the H2O2 concentration and equivalence ratios. Air replacement with H2O2 enhances the reactions rate and concentration of intermediate radicals such as O/H, HO2, and HCO in the mixture. These intermediate radicals closely govern the combustion chemistry of the NH3/CH4– O2/N2/H2O2 mixture. A linear correlation is observed between the flame speed and peak mole fraction of OH + HO2 radicals, and 2nd degree polynomial correlation is observed for the peak mole fraction of NO and CO with HNO + OH and HCO + OH radicals, respectively.  相似文献   

20.
An edge flame was established in a counterflow field with a stretch rate gradient using twin rectangular burners which were misaligned by a few degrees. The stretch rate gradient was quantitatively defined as a function of the angle between the two burners and the distance from the edge of the burner, and thus the effect of stretch rate gradient on the behavior of the edge flame was investigated. The local chemical reaction rate at the edge of a CH4/air flame was stronger than that at other parts of the flame. On the other hand, the reaction rate at the edge of a C3H8/air flame was weaker than that of other parts of the flame. The curvature of the flame edge of the CH4/air flame was much larger than that of the C3H8/air flame. These results are thought to be due to the effect of the Lewis number. The ratios of the local stretch rate at the flame edge to the extinction stretch rate for planar twin flames with the same composition as the edge flame were 0.5 to 0.7 for the CH4/air flame and 0.6 to 0.8 for the C3H8/air flame. These values were midway between those in the numerical simulation by Daou and Linan and those in the experiment by Liu and Ronney. Moreover, it was shown that an increase in the stretch rate gradient resulted in a lower local stretch rate at the flame edge. Behavior of the edge flames did not depend on the Lewis number of the mixture.  相似文献   

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