Heat release rate as represented by [OH] × [CH2O] and its role in autoignition

Data from a recent instantaneous, simultaneous, high-resolution imaging experiment of Rayleigh temperature and laser induced fluorescence (LIF) of OH and CH₂O at the base of a turbulent lifted methane flame issuing into a hot vitiated coflow are analysed and contrasted to reference flames to further investigate the stabilization mechanisms involved. The use of the product of the quantified OH and semi-quantified CH₂O images as a marker for heat release rate is validated for transient autoigniting laminar flames. This is combined with temperature gradient information to investigate the flame structure. Super-equilibrium OH, the nature of the profiles of heat release rate with respect to OH mole fraction, and comparatively high peak heat release rates at low temperature gradients is found in the kernel structures at the flame base, and found to be indicative of autoignition stabilization.     

Simultaneous measurement of localized heat release with OH/CH2O-LIF imaging and spatially integrated OH∗ chemiluminescence in turbulent swirl flames

The in-situ and localized observation of heat release in turbulent flames is important for the validation of computational modeling of turbulent flows with combustion. In the present work we obtain localized information on heat release rate (HRR) by the commonly accepted technique of the simultaneous and single-shot planar imaging of OH and CH₂O concentrations by laser-induced fluorescence (LIF). Additionally, we combine this with the simultaneous line-of-sight and temporally resolved chemiluminescence detection of OH^?, spatially integrated within the flame volume, interrogated by the laser sheets used for the HRR imaging technique. The combined diagnostic methods are demonstrated for a swirl-stabilized, premixed turbulent methane/air flame of 30-kW thermal power, and they show the existence of correlations between both HRR-sensitive diagnostic techniques.     

LIF measurements and chemical kinetic analysis of methylidyne formation in high-pressure counter-flow partially premixed and non-premixed flames

We report quantitative, spatially resolved, linear laser-induced fluorescence (LIF) measurements of methylidyne concentration ([CH]) in laminar, methane–air, counter-flow partially premixed and non-premixed flames using excitation near 431.5 nm in the A–X (0,0) band. For partially premixed flames, fuel-side equivalence ratios (_B) of 1.45, 1.6 and 2.0 are studied at pressures of 1, 3, 6, 9 and 12 atm. For non-premixed flames, the fuel-side mixture consists of 25% CH₄ and 75% N₂; measurements are obtained at pressures of 1, 2, 3, 4, 5, 6, 9 and 12 atm. The quantitative CH measurements are compared with predictions from an opposed-flow flame code utilizing two GRI chemical kinetic mechanisms (versions 2.11 and 3.0). LIF measurements of [CH] are corrected for variations in the quenching rate coefficient by using major species concentrations and temperatures generated by the code along with suitable quenching cross sections for CH available from the literature. A pathway analysis provides relative contributions from important elementary reactions to the total amount of CH produced at various pressures. Key reactions controlling peak CH concentrations are also identified by using a sensitivity analysis. For the partially premixed flames, measured CH profiles are reproduced reasonably well by GRI 3.0, although some quantitative disagreement exists at all pressures. Two CH radical peaks are observed for _B=1.45 and _B=1.6 at pressures above 3 atm. Peak CH concentrations for the non-premixed flames are significantly underpredicted by GRI 3.0. The latter agrees with previously reported NO concentrations, which are also underpredicted in these same high-pressure counter-flow diffusion flames. PACS 07.35.+k; 42.62.Fi; 82.33.Vx     

Absolute radical concentration measurements in low-pressure H2/O2 flames during the combustion of graphite

Absolute CN and CH radical concentrations were determined in situ during the combustion of a graphite substrate in premixed, laminar, low-pressure, H₂/O₂ flames for two different equivalence ratios, = 1.0 and = 1.5. For CN measurements, a small amount of NO (1.8%) was added. The concentration of CN was measured by cavity ring-down spectroscopy (CRDS) probing the absorption of the P_1,2 (13) in the B–X (0, 0) band at 388.1 nm, and the concentration of CH was measured by linear unsaturated laser-induced fluorescence (LIF) exciting the fluorescence of the R₁ (4) in the B–X (0, 0) band at 387.4 nm. Temperature measurements were done based on LIF excitation spectra of OH in the A–X (0, 0) band. It was found that the graphite substrate reduces the flame temperature in the vicinity of its surface. The CN concentrations were found to be three times higher for the rich flame than for the stoichiometric flame. CH concentrations were slightly higher for the stoichiometric flame than for the rich flame. The observed CH/CN concentration ratio is substantially lower compared to NO-doped low-pressure CH₄/O₂ flames. The obtained quantitative information can serve as a first calibration point for detailed numerical simulations of the burning solid graphite, which are based on the concept of surface elementary reactions.     

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.     

Evaluation of heat release indicators in lean premixed H2/Air cellular tubular flames

Heat release rate in combustion systems must be understood in order to control thermoacoustic instabilities, flame extinction, and heat losses. Traditionally OH chemiluminescence (OH*) is used to trace heat release rate (HRR) in H₂/air flames, but its accuracy as a tracer has not been assessed. Lean premixed H₂/air cellular tubular flames are a good test case to evaluate HRR tracers due to the presence of highly reactive flame cells surrounded by regions of near extinction. Comparing the calculated heat release rate to OH* concentration, one finds that [OH*] profiles correlate with the regions of high reactivity (flame cells) but the correlation fails in the low reactivity regions where the HRR is much higher than the [OH*] value indicates. Alternate HRR tracers including [H] and pixel-by-pixel products of [O₂]x[H], [OH]x[H₂], and [O]x[H₂] are analyzed with detailed numerical simulations. The chosen products derive from the main chain reaction steps that contribute to overall HRR in lean, premixed H₂/air flames. Findings suggest that [H] is an accurate yet simple way of tracking HRR. Planar measurements of HRR are possible if LIF measurements of [H] are improved.     

Flow characterization and dilution effects of N_2 and CO_2 on premixed CH_4/air flames in a swirl-stabilized combustor

Numerically-aided experimental studies are conducted on a swirl-stabilized combustor to investigate the dilution effects on flame stability, flame structure, and pollutant emissions of premixed CH4/air flames. Our goal is to provide a systematic assessment on combustion characteristics in diluted regimes for its application to environmentally-friendly approaches such as biogas combustion and exhanst-gas recirculation technology. Two main diluting species, N2 and CO2, are tested at various dilution rates. The results obtained by means of optical diagnostics show that five main flame regimes can be observed for Nz-diluted flames by changing excess air and dilution rate. CO2-diluted flames follow the same pattern evolution except that all the domains are shifted to lower excess air. Both N2 and CO2 dilution affect the lean blow- out （LBO） limits negatively. This behavior can be counter-balanced by reactant preheating which is able to broaden the flammability domain of the diluted flames. Flame reactivity is degraded by increasing dilution rate. Meanwhile, flames are thickened in the presence of both diluting species. NOx emissions are significantly reduced with dilution and proved to be relevant to flame stability diagrams： slight augmentation in NOx emission profiles is related to transitional flame states where instability occurs. Although dilution results in increase in CO emissions at certain levels, optimal dilution rates can still be proposed to achieve an ideal compromise.     

The influence of water on extinction and ignition of hydrogen and methane flames

The influence of water vapor on critical conditions of extinction and autoignition of premixed and nonpremixed flames is investigated. The fuels tested are hydrogen (H₂) and methane (CH₄). Studies on premixed systems are carried out by injecting a premixed reactant stream made up of fuel, oxygen (O₂), and nitrogen (N₂) from one duct, and an inert-gas stream of N₂ from the other duct. Critical conditions of extinction are measured for various amounts of water vapor added to the premixed reactant stream. The ratio of fuel to oxygen is maintained at a constant value, and the amounts of water vapor and nitrogen are so chosen that the adiabatic temperature remains the same. This ensures that the physical influence of water is the same for all cases. Therefore, changes in values for the critical conditions of extinction are attributed to the chemical influence of water vapor. Studies on nonpremixed systems are carried out by injecting a fuel stream made up of fuel and N₂ from one duct ,and an oxidizer stream made up of O₂ and N₂ from the other duct. Critical conditions of extinction are measured with water vapor added to the oxidizer stream. The concentrations of reactants are so chosen that the adiabatic temperature and the flame position stay the same for all cases. Critical conditions of autoignition are measured by preheating the oxidizer stream of the nonpremixed system. Water vapor is added to the oxidizer stream. Numerical calculations are performed using a detailed chemical-kinetic mechanism and compared with measurements. Experimental and numerical studies show that addition of water makes the premixed and nonpremixed flames easier to extinguish and harder to ignite. The chemical influence of water is attributed to its enhanced chaperon efficiency in three body reactions.     

Laser-induced fluorescence detection of singlet CH2 in low-pressure methane/oxygen flames

Methylene, CH₂, is a chemically important intermediate in hydrocarbon combustion but has previously eluded optical detection in a combustion environment. The CH₂ signal as a function of height above the burner surface in a premixed, laminar, methane/oxygen flame (5.6 Torr and fuel equivalence ratio 1.05) is measured by laser-induced fluorescence (LIF) in the B ₁ – ã¹ A ₁ electronic system. The ã state which lies 3165 cm^–1 above the ground state is populated at the high temperatures of the flame (800–1800 K). Although less than one photon for each laser pulse is detected, we can unambiguously attribute the LIF features in the region 450 to 650 nm to CH₂ by both scanning the excitation laser and dispersing fluorescence. LIF temperatures and CH and OH LIF concentration profiles are also obtained for the flame. The CH₂ radical concentration maximum occurs closer to the burner than that of either OH or CH, as expected from models of methane combustion chemistry.     

Modeled quenching limits of spherical hydrogen diffusion flames

Hydrogen–air diffusion flames were modeled with an emphasis on kinetic extinction. The flames were one-dimensional spherical laminar diffusion flames supported by adiabatic porous burners of various diameters. Behavior of normal (H₂ flowing into quiescent air) and inverse (air flowing into quiescent H₂) configurations were considered using detailed H₂/O₂ chemistry and transport properties with updated light component diffusivities. For the same heat release rate, inverse flames were found to be smaller and 290 K hotter than normal flames. The weakest normal flame that could be achieved before quenching has an overall heat release rate of 0.25 W, compared to 1.4 W for the weakest inverse flame. There is extensive leakage of the ambient reactant for both normal and inverse flames near extinction, which results in a premixed flame regime for diffusion flames except for the smallest burners with radii on the order of 1 μm. At high flow rates H + OH(+M) → H₂O(+M) contributes nearly 50% of the net heat release. However at flow rates approaching quenching limits, H + O₂(+M) → HO₂(+M) is the elementary reaction with the largest heat release rate.     

Response of non-premixed flames to bulk flow perturbations

This paper describes the dynamics of non-premixed flames responding to bulk velocity fluctuations, and compares the dynamics of the flame sheet position and spatially integrated heat release to that of a premixed flame. The space–time dynamics of the non-premixed flame sheet in the fast chemistry limit is described by the stoichiometric mixture fraction surface, extracted from the solution of the

-equation. This procedure has some analogies to premixed flames, where the premixed flame sheet location is extracted from the G = 0 surface of the solution of the G-equation. A key difference between the premixed and non-premixed flame dynamics, however, is the fact that the non-premixed flame sheet dynamics are a function of the disturbance field everywhere, and not just at the reaction sheet, as in the premixed flame problem. A second key difference is that the non-premixed flame does not propagate and so flame wrinkles are convected downstream at the axial flow velocity, while wrinkles in premixed flames convect downstream at a vector sum of the flame speed and axial velocity. With the exception of the flame wrinkle propagation speed, however, we show that that the solutions for the space–time dynamics of the premixed and non-premixed reaction sheets in high velocity axial flows are quite similar. In contrast, there are important differences in their spatially integrated unsteady heat release dynamics. Premixed flame heat release fluctuations are dominated by area fluctuations, while non-premixed flames are dominated by mass burning rate fluctuations. At low Strouhal numbers, the resultant sensitivity of both flames to flow disturbances is the same, but the non-premixed flame response rolls off slower with frequency. Hence, this analysis suggests that non-premixed flames are more sensitive to flow perturbations than premixed flames at O(1) Strouhal numbers.     

Reaction zone structures and mixing characteristics of partially premixed swirling CH4/air flames in a gas turbine model combustor

The mixing, reaction progress, and flame front structures of partially premixed flames have been investigated in a gas turbine model combustor using different laser techniques comprising laser Doppler velocimetry for the characterization of the flow field, Raman scattering for simultaneous multi-species and temperature measurements, and planar laser-induced fluorescence of CH for the visualization of the reaction zones. Swirling CH₄/air flames with Re numbers between 7500 and 60,000 have been studied to identify the influence of the turbulent flow field on the thermochemical state of the flames and the structures of the CH layers. Turbulence intensities and length scales, as well as the classification of these flames in regime diagrams of turbulent combustion, are addressed. The results indicate that the flames exhibit more characteristics of a diffusion flame (with connected flame zones) than of a uniformly premixed flame.     

Effects of radiation heat loss on laminar premixed ammonia/air flames

Ammonia (NH₃) direct combustion is attracting attention for energy utilization without CO₂ emissions, but fundamental knowledge related to ammonia combustion is still insufficient. This study was designed to examine effects of radiation heat loss on laminar ammonia/air premixed flames because of their very low flame speeds. After numerical simulations for 1-D planar flames with and without radiation heat loss modeled by the optically thin model were conducted, effects of radiation heat loss on flame speeds, flame structure and emissions were investigated. Simulations were also conducted for methane/air mixtures as a reference. Effects of radiation heat loss on flame speeds were strong only near the flammability limits for methane, but were strong over widely diverse equivalence ratios for ammonia. The lower radiative flame temperature suppressed the thermal decomposition of unburned ammonia to hydrogen (H₂) at rich conditions. The equivalence ratio for a low emission window of ammonia and nitric oxide (NO) in the radiative condition shifted to a lower value than that in the adiabatic condition.     

Three-dimensional numerical simulations of cellular jet diffusion flames

Recent experimental investigations have demonstrated that the appearance of particular cellular states in circular non-premixed jet flames significantly depends on a number of parameters, including the initial mixture strength, reactant Lewis numbers, and proximity to the extinction limit (Damköhler number). For CO₂-diluted H₂/O₂ jet diffusion flames, these studies have shown that a variety of different cellular patterns or states can form. For given fuel and oxidizer compositions, several preferred states were found to co-exist, and the particular state realized was determined by the initial conditions. To elucidate the dynamics of cellular instabilities, circular non-premixed jet flames are modeled with a combination of three-dimensional numerical simulation and linear stability analysis (LSA). In both formulations, chemistry is described by a single-step, finite-rate reaction, and different reactant Lewis numbers and molecular weights are specified. The three-dimensional numerical simulations show that different cellular flames can be obtained close to extinction and that different states co-exist for the same parameter values. Similar to the experiments, the behavior of the cell structures is sensitive to (numerical) noise. During the transient blow-off process, the flame undergoes transitions to structures with different number of cells, while the flame edge close to the nozzle oscillates in the streamwise direction. For conditions similar to the experiments discussed, the LSA results reveal various cellular instabilities, typically with azimuthal wavenumber m = 1–6. Consistent with previous theoretical work, the propensity for the cellular instabilities is shown to increase with decreasing reactant Lewis number and Damköhler number.     

Two-dimensional imaging of glyoxal (C2H2O2) in acetylene flames using laser-induced fluorescence

2 H₂O₂). Laser-induced fluorescence spectra from glyoxal vapor using the same excitation wavelength of 428 nm showed the same strongest lines as the signal from the flame. Glyoxal was visualized in two different modes; two-dimensional imaging and a spatial-spectral mode where spectra were obtained at different spatial positions in the flame simultaneously. For the premixed laminar rich flame it is shown that glyoxal is produced early in the flame, before the signals for C₂ and CH appear. For the turbulent non-premixed flames it is shown that glyoxal is produced in a layer on the fuel rich side of the flames. Here the fuel is premixed with ambient air. This layer is thin and has a high spatial resolution. The general trend was that the glyoxal signal appeared in regions with a lower temperature compared with the emission from C₂ and CH. The imaging of glyoxal in turbulent acetylene flames is a promising tool for achieving new insight into flame phenomena, as it gives very good structural information on the flame front. Tests so far do not indicate that the detected glyoxal is a result of photo-production. To our knowledge, this is the first detection of glyoxal in flames using laser-induced fluorescence. Received: 19 December 1996/Revised version: 26 May 1997     

Spectroscopic observations of methane-pulverized coal flames

A premixed laminar flame burner was used to study physical and chemical effects of burning methane and pulverized coal simultaneously. Spectral emissions obtained as a function of height in the flame, for OH, CH, C₂, and CO were used to calculate excited state species number densities. Premixed methane-air flames with a number of equivalence ratios and methane-air-coal dust flames with three equivalence ratios were studied and differences were noted. Spatial temperatures were measured in all flames by means of a thermocouple probe.The introduction of a pulverized coal additive (30mg/min) leads to changes in OH, Ch, C₂, and CO number densities and temperature at various heights, which depend on the stoichiometry of the methane-air flame. Possible chemical and physical mechanisms responsible for these changes are discussed qualitatively. The data pose a severe test for any quantitative model which includes the fluid dynamics, gas-phase chemistry, heterogeneous processes, and radiation transport.     

An investigation of flame zones and burning velocities of laminar unconfined methane-oxygen premixed flames

Numerical and experimental investigations of unconfined methane-oxygen laminar premixed flames are presented. In a lab-scale burner, premixed flame experiments have been conducted using pure methane and pure oxygen mixtures having different equivalence ratios. Digital photographs of the flames have been captured and the radial temperature profiles at different axial locations have been measured using a thermocouple. Numerical simulations have been carried out with a C2 chemical mechanism having 25 species and 121 reactions and with an optically thin radiation sub-model. The numerical results are validated against the experimental and numerical results for methane-air premixed flames reported in literature. Further, the numerical results are validated against the results from the present methane-oxygen flame experiments. Visible regions in digital flame photographs have been compared with OH isopleths predicted by the numerical model. Parametric studies have been carried out for a range of equivalence ratios, varying from 0.24 to 1.55. The contours of OH, temperature and mass fractions of product species such as CO, CO₂ and H₂O, are presented and discussed for various cases. By using the net methane consumption rate, an estimate of the laminar flame speed has been obtained as a function of equivalence ratio.     

Method for absolute OH-concentration measurements in premixed flames by LIF and numerical simulations

We present and apply a methodology for the single-shot measurement of absolute concentrations of the OH-radical in a turbulent, premixed natural gas/air flame. The method is based on a combination of detailed numerical simulations of the turbulent flame and an experimental approach using planar laser-induced fluorescence (LIF). The numerical simulation is used to predict LIF intensities. It shows the existence of a sharp correlation between the LIF signal after excitation of the A–X(3,0) P₂(8) transition near 248.45 nm and OH concentrations for a wide range of conditions, including stationary and instationary laminar flames of different strain rates, with different models to treat molecular transport and different degrees of heat loss. This correlation allows the transformation of measured OH–LIF intensity images into absolute OH concentration maps. PACS 82.33.Vx; 82.20.Wt; 42.62.Fi An erratum to this article can be found at .