Premixed turbulent flame front structure investigation by Rayleigh scattering in the thin reaction zone regime

Premixed turbulent flames of methane–air and propane–air stabilized on a bunsen type burner were studied using planar Rayleigh scattering and particle image velocimetry. The fuel–air equivalence ratio range was from lean 0.6 to stoichiometric for methane flames, and from 0.7 to stoichiometric for propane flames. The non-dimensional turbulence rms velocity, u′/S_L, covered a range from 3 to 24, corresponding to conditions of corrugated flamelets and thin reaction zones regimes. Flame front thickness increased slightly with increasing non-dimensional turbulence rms velocity in both methane and propane flames, although the flame thickening was more prominent in propane flames. The probability density function of curvature showed a Gaussian-like distribution at all turbulence intensities in both methane and propane flames, at all sections of the flame.The value of the term Dκ, the product of molecular diffusivity evaluated at reaction zone conditions and the flame front curvature, has been shown to be smaller than the magnitude of the laminar burning velocity. This finding questions the validity of extending the level set formulation, developed for corrugated flames region, into the thin reaction zone regime by increasing the local flame propagation by adding the term Dκ to laminar burning velocity.     

Characterization of the effects of pressure and hydrogen concentration on laminar burning velocities of methane–hydrogen–air mixtures

The aim of the present work was to characterize both the effects of pressure and of hydrogen addition on methane/air premixed laminar flames. The experimental setup consists of a spherical combustion chamber coupled to a classical shadowgraphy system. Flame pictures are recorded by a high speed camera. Global equivalence ratios were varied from 0.7 to 1.2 for the initial pressure range from 0.1 to 0.5 MPa. The mole fraction of hydrogen in the methane + hydrogen mixture was varied from 0 to 0.2. Experimental results were compared to calculations using a detailed chemical kinetic scheme (GRIMECH 3.0). First, the results for atmospheric laminar CH₄/air flames were compared to the literature. Very good agreements were obtained both for laminar burning velocities and for burned gas Markstein length. Then, increasing the hydrogen content in the mixture was found to be responsible for an increase in the laminar burning velocity and for a reduction of the flame dependence on stretch. Transport effects, through the reduction of the fuel Lewis number, play a role in reducing the sensitivity of the fundamental flame velocity to the stretch. Finally, when the pressure was increased, the laminar burning velocity decreased for all mixtures. The pressure domain was limited to 0.5 MPa due to the onset of instabilities at pressures above this value.     

Measurements of burning velocities of dimethyl ether and air premixed flames at elevated pressures

Laminar burning velocities of dimethyl ether (DME) and air premixed flames at elevated pressures up to 10 atm were measured by using a newly developed pressure-release type spherical bomb. The measurement system was validated using laminar burning velocities of methane–air flames. A comparison with the previous experimental data shows an excellent agreement and demonstrates the accuracy and reliability of the present experimental system. The measured flame speeds of DME–air flames were compared with the previous experimental data and the predictions using the full and reduced mechanisms. At atmospheric pressure, the measured laminar burning velocities of DME–air flames are in reasonable agreement with the previous data from spherical bomb method, but are much lower than both predictions and the experimental data of the PIV based counterflow flame measurements. The laminar burning velocities of DME–air flames at 2, 6, and 10 atm were also measured. It was found that flame speed decreases considerably with the increase of pressure. Moreover, the measured flame speeds are also lower than the predictions at high pressures. In addition, experiments showed that at high pressures the rich DME–air flames are strongly affected by the hydrodynamic and thermal-diffusive instabilities. Markstein lengths and the overall reaction order at different equivalence ratios were extracted from the flame speed data at elevated pressures. Sensitivity analysis showed that reactions involving methyl and formyl radicals play an important role in DME–air flame propagation and suggested that systematic modification of the reactions rates associated with methyl and formyl formations are necessary to reduce the discrepancies between predictions and measurements.     

Measurement of unstable burning velocities of iso-octane–air mixtures at high pressure and the derivation of laminar burning velocities

A new technique is reported for measuring burning velocities at high pressures in the final stages of two inwardly propagating flame kernels in an explosion bomb. The flames were initiated at diametrically opposite spark electrodes, close to the wall, in quiescent mixtures. Measurements of pressure and flame kernel propagation speeds by high-speed photography showed the burning velocities to be elevated above the corresponding laminar burning velocities as a result of the developing flame instabilities. The enhancement increased with increase in pressure and decreased with increase in Markstein number. When the Markstein number was negative, instabilities could be appreciable, as could the enhancement. For the iso-octane–air mixtures investigated, where the mixtures had well-characterised Markstein numbers or critical Peclet numbers at the relevant pressures and temperatures, it was possible to explain the enhancement quantitatively by the spherical explosion flame instability theory of Bechtold and Matalon, provided the critical Peclet number was that observed experimentally, and allowance was made for the changing pressure. With this theoretical procedure, it was possible to derive values of laminar burning velocity from the measured values of burning velocity over a wide range of equivalence ratios, pressures, and temperatures. The values became less reliable at the higher temperatures and pressures as the data on Markstein and critical Peclet numbers became less certain. It was found that with iso-octane as the fuel the laminar burning velocity decreased during isentropic compression.     

Formation and destruction of nitric oxide in methane flames doped with NO at atmospheric pressure

A study of formation and destruction of NO in adiabatic laminar premixed flames of CH₄ + O₂ mixtures diluted with N₂ or Ar (with various dilution ratios) in a range of equivalence ratios at atmospheric pressure is presented. Nitric oxide was seeded into the flames using mixtures of diluent gas + 100 ppm of NO. The heat flux method was employed to measure adiabatic burning velocities of these flames. Nitric oxide concentrations in the post-flame zone at 10, 15 and 20 mm above the burner surface were measured using probe sampling. Burning velocities and NO concentrations simulated using a previously developed chemical kinetic mechanism were compared with the experimental results. The conversion ratio of NO seeded into the flames was determined. The kinetic mechanism accurately predicts burning velocities over the range of equivalence ratios and NO conversion in the rich flames. Significant discrepancies between measured and calculated NO conversion in the lean and near-stoichiometric flames were observed and discussed.     

Localised forced ignition of globally stoichiometric stratified mixtures: A numerical investigation

Localised forced ignition of globally stoichiometric stratified mixtures (i.e. < φ > =1.0) has been analysed here based on direct numerical simulations for different initial values of velocity and equivalence ratio fluctuations (i.e. u′ and φ′), and the Taylor micro-scale l_φ of equivalence ratio φ variation. The localised ignition is accounted for by a source term in the energy transport equation which deposits energy over a stipulated time interval. It has been found that combustion takes place predominantly under premixed mode in the case of successful ignition. The initial values of φ′ and l_φ have been found to have significant effects on the extent of burning of stratified mixtures following localised ignition. It has been found that an increase in u′(φ′) has adverse effects on the burned gas mass, whereas the effects of l_φ on the extent of burning are non-monotonic and dependent on φ′. Detailed physical explanations have been provided for the observed u′, φ′ and l_φ dependences on the extent of burning in stratified mixtures.     

Coaxial turbulent jet flames: Scaling relations for measured stoichiometric mixing lengths

Previous studies have quantified the fuel–air mixing processes within jet flames having a central fuel jet surrounded by an oxidizer coflow, where the mixing primarily occurs in the far field. The present work instead quantifies mixing within coaxial jet flames having a central jet of oxygen and a surrounding finite thickness coflow of hydrogen. These flames are relatively short and the primary mixing occurs in the near field. The stoichiometric mixing length (L_S) was measured, which is the distance along the centerline at which the stoichiometric condition occurs. Values of L_S were measured for a wide range of velocity ratios for both reacting and nonreacting cases using Planar Laser Induced Fluorescence (PLIF). Acetone PLIF was utilized for nonreacting cases, while OH PLIF was used for reacting. In nonreacting cases the use of a nondimensional momentum flux ratio collapses the nonreacting coaxial jet values of L_S to a single curve, which confirms previous theory. It also was found that the reacting and nonreacting coaxial jet data collapses approximately to a single curve, if one uses both the nondimensional momentum flux ratio and an effective outer flow gas density which is predicted by the analysis of Tacina and Dahm.     

Problems of predicting turbulent burning rates

Different approaches to the modelling of turbulent combustion first are reviewed briefly. A unified, stretched flamelet approach then is presented. With Reynolds stress modelling and a generalized probability density function (PDF) of strain rate, it enables a source term, in the form of a probability of burning function, P_b, to be expressed as a function of Markstein numbers and the Karlovitz stretch factor. When P_b is combined with some turbulent flame fractal considerations, an expression is obtained for the turbulent burning velocity. When it is combined with the profile of the unstretched laminar flame volumetric heat release rate plotted against the reaction progress variable and the PDF of the latter, an expression is obtained for the mean volumetric turbulent heat release rate. Through these relationships experimental values of turbulent burning velocity might be used to evaluate P_b and hence the CFD source term, the mean volumetric heat release rate.

Different theoretical expressions for the turbulent burning velocity, including the present one, are compared with experimental measurements. The differences between these are discussed and this is followed by a review of CFD applications of these flamelet concepts to premixed and non-premixed combustion. The various assumptions made in the course of the analyses are scrutinized in the light of recent direct numerical simulations of turbulent flames and the applications to the flames of laser diagnostics. Remaining problem areas include a sufficiently general combination of strain rate and flame curvature PDFs to give a single PDF of flame stretch rate, the nature of flame quenching under positive and negative stretch rates, flame responses to changing stretch rates and the effects of flame instabilities.     

Global reduced mechanisms for methane and hydrogen combustion with nitric oxide formation constructed with CSP data

Reduced mechanisms for methane-air and hydrogen-air combustion including NO formation have been constructed with the computational singular perturbation (CSP) method using the fully automated algorithm described by Massias et al. The analysis was performed on solutions of unstrained adiabatic premixed flames with detailed chemical kinetics described by GRI 2.11 for methane and a 71-reaction mechanism for hydrogen including NO _x formation. A 10-step reduced mechanism for methane has been constructed which reproduces accurately laminar burning velocities, flame temperatures and mass fraction distributions of major species for the whole flammability range. Many steady-state species are also predicted satisfactorily. This mechanism is an improvement over the seven-step set of Massias et al, especially for rich flames, because the use of HCNO, HCN and C₂H₂ as major species results in a better calculation of prompt NO. The present 10-step mechanism may thus also be applicable to diffusion flames. A five-step mechanism for lean and hydrogen-rich combustion has also been constructed based on a detailed mechanism including thermal NO. This mechanism is accurate for a wide range of the equivalence ratio and for pressures as high as 40 bar. For both fuels, the CSP algorithm automatically pointed to the same steady-state species as those identified by laborious analysis or intuition in the literature and the global reactions were similar to well established previous methane-reduced mechanisms. This implies that the method is very well suited for the study of complex mechanisms for heavy hydrocarbon combustion.M This article features supplementary data files available from the supplemental page in the online journal.     

Laser-induced fluorescence determination of flame temperatures in comparison with CARS measurements

Temperature profiles in several premixed low pressure H₂/O₂/N₂ flames and in an atmospheric pressure CH₄/air flame were determined by laser-induced fluorescence (LIF) and by CARS experiments. In the LIF study, temperatures were derived from OH excitation spectra, CARS temperatures were deduced from N₂ Q-branch spectra. The present study is the first quantitative comparison of these two methods for temperature determination in flames burning at pressures up to 1 bar. The resulting temperatures showed good agreement.     

Flame front analysis of high-pressure turbulent lean premixed methane–air flames

An experimental study on lean turbulent premixed methane–air flames at high pressure is conducted by using a turbulent Bunsen flame configuration. A single equivalence ratio flame at Φ = 0.6 is explored for pressures ranging from atmospheric pressure to 0.9 MPa. LDA measurements of the cold flow indicate that turbulence intensities and the integral length scale are not sensitive to pressure. Due to the decreased kinematic viscosity with increasing pressure, the turbulent Reynolds numbers increase, and isotropic turbulence scaling relations indicate a large decrease of the smallest turbulence scales. Available experimental results and PREMIX code computations indicate a decrease in laminar flame propagation velocities with increasing pressure, essentially between the atmospheric pressure and 0.5 MPa. The u′/S_L ratio increases therefore accordingly. Instantaneous flame images are obtained by Mie scattering tomography. The images and their analysis show that pressure increase generates small scale flame structures. In an attempt to generalize these results, the variance of the flamelet curvatures, the standard deviation of the flamelet orientation angle, and the flamelet crossing lengths have been plotted against which is proportional to the ratio between the integral and Taylor length scales, and which increases with pressure. These three parameters vary linearly with the ratio between large and small turbulence scales and clearly indicate the strong effect of this parameter on premixed turbulent flame dynamics and structure. An obvious consequence is the increase in flame surface density and hence burning rate with pressure, as confirmed by its direct determination from 2D tomographic images.     

Characterizing the fuel-specific combustion chemistry of acetic acid and propanoic acid: Laminar flame propagation and kinetic modeling studies

In order to study the combustion chemistry of carboxyl functionality, the laminar burning velocity of acetic acid/air and propanoic acid/air mixtures was investigated in a high-pressure constant-volume cylindrical combustion vessel at 423 K, 1 atm and equivalence ratios of 0.7–1.4. Experimental results reveal that the flame propagation of propanoic acid flame is much faster than that of acetic acid flame, especially under rich conditions, and the laminar burning velocity of propanoic acid/air mixtures peaks at richer conditions than that of acetic acid. The present theoretical calculations for the isomerization and decomposition of propanoic acid radicals indicate that the primary radical products are HOCO, H and C₂H₅, while those in acetic acid flame are CH₃ and OH based on previous studies. A kinetic model of the two acids was developed mainly based on previous and the present theoretical calculation results. It could reasonably capture the measured laminar burning velocities of acetic acid/air and propanoic acid/air mixtures in this work, as well as the previous experimental data in literature. Based on the present model, CH₃- and ketene-related pathways play an important role in acetic acid flames. Under rich conditions, ketene is mostly converted to CH₃ via CH₂CO+HCH₃+CO, and the chain-termination reaction of CH₃+H(+M)=CH₄(+M) is enhanced, which strongly inhibits the propagation of rich acetic acid flames. In contrast, C₂H₅ and ethylene chemistry play an important role in propanoic acid flames. Rich conditions promote the decomposition of C₂H₅, yielding ethylene and H, which can facilitate the flame propagation. This can explain the shift of the peak laminar burning velocity of propanoic acid/air mixtures towards a slightly richer condition compared with that of acetic acid/air mixtures.     

Skeletal mechanism generation with CSP and validation for premixed n-heptane flames

An automated procedure has been previously developed to generate simplified skeletal reaction mechanisms for the combustion of n-heptane/air mixtures at equivalence ratios between 0.5 and 2.0 and different pressures. The algorithm is based on a Computational Singular Perturbation (CSP)-generated database of importance indices computed from homogeneous n-heptane/air ignition solutions. In this paper, we examine the accuracy of these simplified mechanisms when they are used for modeling laminar n-heptane/air premixed flames. The objective is to evaluate the accuracy of the simplified models when transport processes lead to local mixture compositions that are not necessarily part of the comprehensive homogeneous ignition databases. The detailed mechanism was developed by Curran et al. and involves 560 species and 2538 reactions. The smallest skeletal mechanism considered consists of 66 species and 326 reactions. We show that these skeletal mechanisms yield good agreement with the detailed model for premixed n-heptane flames, over a wide range of equivalence ratios and pressures, for global flame properties. They also exhibit good accuracy in predicting certain elements of internal flame structure, especially the profiles of temperature and major chemical species. On the other hand, we find larger errors in the concentrations of many minor/radical species, particularly in the region where low-temperature chemistry plays a significant role. We also observe that the low-temperature chemistry of n-heptane can play an important role at very lean or very rich mixtures, reaching these limits first at high pressure. This has implications to numerical simulations of non-premixed flames where these lean and rich regions occur naturally.     

Cellular instabilities of expanding hydrogen/propane spherical flames at elevated pressures: theory and experiment

An experimental and theoretical investigation of the onset of cellular instabilities on spherically expanding flames in mixtures of hydrogen and propane in air at elevated pressures was conducted. Critical conditions for the onset of instability were measured and mapped out over a range of pressures and mixture compositions. An asymptotic theory of hydrodynamic and diffusional-thermal cell development on flames in mixtures comprised of two scarce fuels burning in air was also formulated. Predicted values of Peclet number, defined as the flame radius at the onset of instability normalized by the flame thickness, were shown to compare favorably with the experimentally measured values.     

Diffusional-thermal instability in strained diffusion flames with unequal Lewis numbers

Diffusional–thermal instability is analysed for near-extinction counterflow diffusion flames to examine the instability characteristics of strained diffusion flamelets in turbulent flames, with the additional intention of providing a guideline to future experimental investigations. Attention is focused on the linear stability of the instability patterns appearing in the unstrained direction of two-dimensional counterflow diffusion flames, which is treated by the near-equilibrium regime of activation-energy asymptotics with Lewis numbers close to unity. The effects of unequal Lewis numbers for fuel and oxidizer are also taken into account by introducing an effective Lewis number. The resulting formulation describing linear stability of the harmonically decomposed disturbances turns out to be identical to the formulation derived previously for equal fuel and oxidizer Lewis numbers. For effective Lewis numbers less than unity, cellular instability is predicted for the entire range of the equivalence ratio, and the threshold Lewis number maintains a value slightly less than unity. On the other hand, for effective Lewis numbers sufficiently greater than unity, two types of oscillatory instabilities are found. As the effective Lewis number increases from unity, a travelling instability is first encountered for a range of finite wavelengths, and a pulsating instability emerges immediately above the travelling instability. These two types of oscillatory instabilities are predicted only for equivalence ratios sufficiently greater than unity because the threshold Lewis numbers for these instabilities are found to be infinity at unity equivalence ratio. For large values of the equivalence ratio, which is typical of most hydrocarbon flames, oscillatory instabilities are predicted only for flames burning extremely heavy hydrocarbon fuels or for flames heavily diluted by light inert gases.     

Combustion behavior of ammonia blended with diethyl ether

Ammonia (NH₃) is recognized as a carbon-free hydrogen-carrier fuel with a high content of hydrogen atoms per unit volume. Recently, ammonia has received increasing attention as a promising alternative fuel for internal combustion engine and gas turbine applications. However, the viability of ammonia fueling future combustion devices has several barriers to overcome. To overcome the challenge of its low reactivity, it is proposed to blend it with a high-reactivity fuel. In this work, we have investigated the combustion characteristics of ammonia/diethyl ether (NH₃/DEE) blends using a rapid compression machine (RCM) and a constant volume spherical reactor (CVSR). Ignition delay times (IDTs) of NH₃/DEE blends were measured using the RCM over a temperature range of 620 to 942 K, pressures near 20 and 40 bar, equivalence ratios (Φ) of 1 and 0.5, and a range of mole fractions of DEE, χ_DEE, from 0.05 to 0.2 (DEE/NH₃ = 5 – 20%). Laminar burning velocities of NH₃/DEE premixed flames were measured using the CVSR at 298 K, 1 bar, Φ of 0.9 to 1.3, and χ_DEE from 0.1 to 0.4. Our results indicate that DEE promotes the reactivity of fuel blends resulting in significant shortening of the ignition delay times of ammonia under RCM conditions. IDTs expectedly exhibited strong dependence on pressure and equivalence ratio for a given blend. Laminar burning velocity was found to increase with increasing fraction of DEE. The burnt gas Markstein length increased with equivalence ratio for χ_DEE = 0.1 as seen in NH₃-air flames, while the opposite evolution of Markstein length was observed with Φ for 0.1 < χ_DEE ≤ 0.4, as observed in isooctane-air flames. A detailed chemical kinetics model was assembled to analyze and understand the combustion characteristics of NH₃/DEE blends.     

On the two-reactant one-step activation-energy asymptotics for steady,adiabatic, planar flames with Lewis numbers of unity

Aspects of predictions of activation-energy asymptotics concerning the dependence of the burning velocity on the equivalence ratio are examined here through both asymptotic analyses and numerical computation. In typical hydrocarbon–air flames, the burning velocity achieves its maximum value for fuel-rich mixture, the cause being generally attributed to the effects of detailed chemical kinetics and unequal diffusivities of the reactants. The present results demonstrate the possibility of this attribute of the burning velocity occurring even when these two effects are absent. This is accomplished by parametrically studying the burning-velocity formula valid for all equivalence ratios under the conditions specified in the title of this article, with special attention paid to implications for hydrocarbon–air flames.     

Burning velocity correlation of methane/air turbulent premixed flames at high pressure and high temperature

Turbulent burning velocities for methane/air mixtures at pressures ranging from atmospheric pressure up to 1.0 MPa and mixture temperatures of 300 and 573 K were measured, which covers the typical operating conditions of premixed-type gas-turbine combustors. A bunsen-type flame stabilized in a high-pressure chamber was used, and OH-PLIF visualization was performed with the pressure and mixture temperature being kept constant. In addition to a burner with an outlet diameter of 20 mm for the high-pressure experiments, a large-scale burner with an outlet diameter of 60 mm was used at atmospheric pressure to extend the turbulence Reynolds number based on the Taylor microscale, R_λ, as a common parameter to compare the pressure and temperature effects. It was confirmed that R_λ over 100 could be attained and that u′/S_L could be extended even at atmospheric pressure. Based on the contours of the mean progress variable c = 0.1 determined using OH-PLIF images, turbulent burning velocity was measured. S_T/S_L was also found to be greatly affected by pressure for preheated mixtures at 573 K. The bending tendency of the S_T/S_L curves with u′/S_L was seen regardless of pressure and mixture temperature and the R_λ region where the bending occurs corresponded well to the region where the smallest scale of flame wrinkling measured as a fractal inner-cutoff approaches the characteristic flame instability scale and becomes almost constant. A power law of S_T/S_L with (P/P₀)(u′/S_L) was clearly seen when S_T was determined using c = 0.1 contours, and the exponent was close to 0.4, indicating agreement with the previous results using the mean flame cone method and the significant pressure effects on turbulent burning velocity.     

Experimental and numerical study of product gas characteristics of ammonia/air premixed laminar flames stabilized in a stagnation flow

Ammonia has widely attracted interest as a potential candidate not only as a hydrogen energy carrier but also as a carbon free fuel for internal combustion engines, such as gas turbines. Because ammonia contains a nitrogen atom in its molecule, nitrogen oxides (NO_x) and other pollutants may be formed when it burns. Therefore, understanding the fundamental product gas characteristics of ammonia/air laminar flames is important for the design of ammonia-fueled combustors to meet stringent emission regulations. In this study, the product gas characteristics of ammonia/air premixed laminar flames for various equivalence ratios were experimentally and numerically investigated up to elevated pressure conditions. In the experiments, a stagnation flame configuration was employed because an ammonia flame can be stabilized by using such a configuration without a pilot flame. The experimental results showed that the maximum NO mole fraction was about 3,500 ppmv, at an equivalence ratio of 0.9 at 0.1 MPa. The NO mole fraction decreased as the equivalence ratio increased. In addition, the maximum value of the NO mole fraction decreased with an increase in mixture pressure. Furthermore, it was experimentally clarified that the simultaneous reduction of NO and unburnt ammonia can be achieved at an equivalence ratio of about 1.06, which is the target equivalence ratio for emission control in rich-lean two-stage ammonia combustors. Comparison of experimental and numerical results showed that even though the reaction mechanisms employed have been optimized for predicting the laminar burning velocity of ammonia/air flames, they failed to satisfactorily predict the measured species in this study. Sensitivity analysis was used to identify elementary reactions that control the species profiles but have negligible effects on the burning velocity. It is considered that these reaction models need to be updated for accurate prediction of product gas characteristics of ammonia/air flames.