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.     

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.     

Experimental and numerical determination of heat release in counterflow premixed laminar flames

This paper presents an experimental and numerical study of heat release in atmospheric laminar counterflow premixed flames. The measurements are based on simultaneous planar laser-induced fluorescence (PLIF) of OH and HCHO. These measurements are compared to numerical results obtained using detailed chemistry and multicomponent transport properties. A low Mach number formulation along the stagnation streamline is employed to describe the reactive flow. The conservation equations are completed with CHEMKIN and EGLIB packages. They are solved using finite differences, Newton iterations, and an adaptive gridding technique. The comparison is done along the burner axis for both, maximum heat release location and heat release profile width. It is shown that the product of OH and HCHO concentrations yields a result closely related to the heat release. These comparisons lead to the conclusion that the experimental method used seems to be a good tool for the determination of heat release in flames.     

Experimental and numerical study of premixed, lean ethylene flames

Ethylene is a key intermediate in the combustion mechanisms of most practical fuels. It plays also an important role in the formation of aromatic hydrocarbons and soot particules. The latter has motivated many experimental and numerical studies carried out on rich ethylene-air mixtures. Less studies have been devoted to lean mixtures, and the development of strategies based on lean, premixed flames to reduce soot and NO_x production requires additional experimental data in lean conditions. In this work, the chemical structure of lean premixed ethylene-oxygen-nitrogen flames stabilized on a flat-flame burner at atmospheric pressure was determined experimentally. The species mole fraction profiles were also computed by the Premix code (Chemkin II version) and four detailed reaction mechanisms. A very good agreement was observed for the main flame properties: reactants consumption, final products (CO₂, H₂O) and the main intermediates: CO and H₂. Marked differences occurred in the prediction of active intermediate species present in small concentrations. Pathways analyses were performed to identify the origins of these discrepancies. It was shown that the same reactions were involved in the four mechanisms to describe the consumption of ethylene, but with marked differences in their relative importance. C₂H₃ and CH₂HCO are the main radicals formed in this first step and their consumption increases the differences between the mechanisms either by the use of different kinetic data for common reactions or by differences in the nature of the consumption reactions.     

Effects of electrodes and imposed flow on forced ignition in laminar premixed hydrogen/air mixtures with large Lewis number

Compared to quiescent premixed reactants, forced ignition of flowing/turbulent premixed reactants is expected to be more difficult because of increased dissipation of the deposited energy. However, the counterintuitive turbulence-facilitated ignition (TFI) has been observed in recent experiments for mixtures with large Lewis number, Le. The mechanisms behind TFI are still not well understood and this study aims to interpret a part of the TFI mechanisms through considering electrodes and imposed flow in the simulations of forced ignition in hydrogen/air mixtures. The imposed flow emulates the local turbulent effects around the electrodes which might blow the ignition kernel away from the electrodes. Since TFI occurs only for mixtures with large Le (e.g., lean hydrocarbon/air or rich H₂/air mixture), a fuel-rich (ϕ=5.1) H₂/air mixture with Le≈2.3 is investigated to reduce computational cost and consider more factors that may lead to TFI. Similar to TFI observed in experiments, the flow-facilitated ignition is observed for H₂/air with ϕ=5.1 and Le≈2.3 when the electrodes have a small gap distance. The detailed effects of including electrodes on forced ignition of quiescent and flowing mixtures are explored. It is found that the existence of electrodes not only induces heat loss but also affects the shape and global curvature/stretch of the ignition kernel. The heat loss to the electrodes is demonstrated to play an important role for the ignition of mixtures with large Le. Compared to quiescent mixtures, considering an imposed flow normal to the electrodes can blow the flame kernel away from the cold electrodes. Such movement of the ignition kernel can greatly reduce both the heat loss to the electrodes and flame curvature/stretch, and thereby promote the ignition in mixtures with large Le. These results help to understand the underlying mechanisms for the TFI observed in experiments.     

CO2 addition and pressure effects on laminar and turbulent lean premixed CH4 air flames

An experimental study on CH₄–CO₂–air flames at various pressures is conducted by using both laminar and turbulent Bunsen flame configurations. The aim of this research is to contribute to the characterization of fuel lean methane/carbon dioxide/air premixed laminar and turbulent flames at different pressures, by studying laminar and turbulent flame propagation velocities, the flame surface density and the instantaneous flame front wrinkling parameters. PREMIX computations and experimental results indicate a decrease of the laminar flame propagation velocities with increasing CO₂ dilution rate. Instantaneous flame images are obtained by Mie scattering tomography. The image analysis shows that although the height of the turbulent flame increases with the CO₂ addition rate, the flame structure is quite similar. This implies that the flame wrinkling parameters and flame surface density are indifferent to the CO₂ addition. However, the pressure increase has a drastic effect on both parameters. This is also confirmed by a fractal analysis of instantaneous images. It is also observed that the combustion intensity S_T/S_L increases both with pressure and the CO₂ rate. Finally, the mean fuel consumption rate decreases with the CO₂ addition rate but increases with the pressure.     

Experimental analysis and theoretical lift-off criterion for H2/air flames stabilized on a dual swirl injector

Stabilization mechanisms of partially premixed H₂/air flames on a coaxial dual swirl injector are investigated at atmospheric conditions. Hydrogen is injected through a central duct, and the air by the outer annular channel. Both channels are swirled and two stabilization modes are observed depending on the geometrical configuration of the injector and on the operating conditions. In certain regimes, the H₂/air flame stabilizes on the injector lips as a diffusion flame. For other operating conditions, the flame is lifted from the injector and burns mainly in partially premixed regime leading to limited NOx emissions. PIV measurements in cold flow conditions and direct observations of the flame indicate that the flame stabilization mode is mainly controlled by the inner hydrogen swirl level, the injector recess and the hydrogen velocity. For a given air flowrate, a minimum hydrogen velocity to lift the flame is determined for each combination of inner swirl level and injector recess. Assuming the flame close to the injector lips behaves like an edge flame, a model for flame stabilization based on the triple flame speed and the location of the stoichiometric mixture fraction line is built. According to this model, the flame is anchored to the injector if the triple flame can propagate to the inner injector lips, i.e., if the velocity along the stoichiometric line is lower than the triple flame speed. The model is tested using hydrogen diluted with argon and air diluted with nitrogen. Two cases producing predicted opposite trends are verified. First, the stoichiometric line is moved in the direction of lower velocity zone keeping the triple flame speed constant in order to anchor a lifted flame. Next, the stoichiometric line is kept constant and the triple flame speed is reduced in order to lift an anchored flame. The mechanisms driving flame stabilization are discussed.     

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.     

Properties of nanocrystalline TiO2 synthesized in premixed flames stabilized on a rotating surface

The properties of TiO₂ nanoparticles synthesized using the flame stabilized on a rotating surface method (FSRS) are investigated. The method uses a laminar, premixed, stagnation flame, combining particle synthesis and film deposition in a single step. The current study examines the effects of flame properties on particle characteristics. Synthesized particles were characterized using X-ray diffractometry, Transmission Electron Microscopy and UV–vis spectrometry in order to quantify the effects of equivalence ratio and precursor loading on particle size, crystallinity and optical band-gap. Results show that flame stoichiometry significantly affects crystal phase, but it has little to no effect on particle size and light absorption band edge. In addition, precursor loading impacts both the particle size and the crystal phase. The study demonstrates the potential of the FSRS method for producing tailored nanoscale TiO₂ particles for a variety of applications.     

The effect of hydrogen addition on flammability limit and NOx emission in ultra-lean counterflow CH4/air premixed flames

The effect of hydrogen addition to ultra lean counterflow CH₄/air premixed flames on the extinction limits and the characteristics of NO_x emission was investigated by numerical simulation. Detailed chemistry and complex thermal and transport properties were employed. The results show that the addition of hydrogen can significantly enlarge the flammable region and extend the flammability limit to lower equivalence ratios. If the equivalence ratio is kept constant, the addition of hydrogen increases the emission of NO in a flame due to the enhancement in the rate of the NNH or N₂O intermediate NO formation routes. The addition of hydrogen causes a monotonic decrease in the formation of NO₂ and N₂O, except flames near the extinction limits, where the emission of NO₂ and N₂O first increases, and then decreases with the increase in the fraction of hydrogen. Overall, hydrogen enrichment technology allows stable combustion under ultra lean conditions, resulting in significant CO₂ and NO emission reduction.     

Cavity ring-down measurements of seeded NO in premixed atmospheric-pressure H2/air and CH4/air flames

Quantitative aspects of using cavity ring-down absorption spectroscopy near 226 nm for measurements of NO mole fractions in premixed atmospheric-pressure flames are discussed. Measurements in methane–air flames showed strong broadband absorption near 226 nm by hot CO₂ molecules, precluding using the cavity ring-down method in these flames at atmospheric pressure. In hydrogen–air flames, the broadband absorption at this wavelength was substantially lower. Absorption cross sections derived from non-seeded cavity ring-down spectra suggest that absorption by water is the major contribution to the background in these flames. The detectability limit for NO by cavity ring-down measurements in hydrogen–air flames using the current setup is estimated to be 10 ppm. Effects of the cold boundary layer on the measured NO mole fraction were accounted for by measuring the radial distributions of temperature and NO mole fraction using coherent anti-Stokes Raman scattering and laser-induced fluorescence (LIF), respectively. Measurements performed in seeded stoichiometric and lean hydrogen–air flames showed no reburning at temperatures above 1750 K, demonstrating the adequacy of using these flames for calibration of LIF measurements. At lower temperatures, the mole fraction of NO in the hot gases was up to 30% lower than that expected from the degree of seeding in the cold gases. PACS 42.62.Fi; 42.68.Ca; 82.33.Vx     

A combustion chemistry study of tetramethylethylene in a laminar premixed low-pressure hydrogen flame

The combustion chemistry of tetramethylethylene (TME) was studied in a premixed laminar low-pressure hydrogen flame by combined photoionization molecular-beam mass spectrometry (PI-MBMS) and photoelectron photoion coincidence (PEPICO) spectroscopy at the Swiss Light Source (SLS) of the Paul Scherrer Institute in Villigen, Switzerland. This hexene isomer with the chemical formula C₆H₁₂ has a special structure with only allylic CH bonds. Several combustion intermediate species were identified by their photoionization and threshold photoelectron spectra, respectively. The experimental mole fraction profiles were compared to modeling results from a recently published kinetic reaction mechanism that includes a TME sub-mechanism to describe the TME/H₂ flame structure. The first stable intermediate species formed early in the flame front during the combustion of TME are 2-methyl-2-butene (C₅H₁₀) at a mass-to-charge ratio (m/z) of 70, 2,3-dimethylbutane (C₆H₁₄) at m/z 86, and 3-methyl-1,2-butadiene (C₅H₈) at m/z 68. Isobutene (C₄H₈) is also a dominant intermediate in the combustion of TME and results from consumption of 2-methyl-2-butene. In addition to these hydrocarbons, some oxygenated species are formed due to low-temperature combustion chemistry in the consumption pathway of TME under the investigated flame conditions.     

Experimental and numerical study of a conical turbulent partially premixed flame

The structure and dynamics of a turbulent partially premixed methane/air flame in a conical burner were investigated using laser diagnostics and large-eddy simulations (LES). The flame structure inside the cone was characterized in detail using LES based on a two-scalar flamelet model, with the mixture fraction for the mixing field and level-set G-function for the partially premixed flame front propagation. In addition, planar laser induced florescence (PLIF) of CH and chemiluminescence imaging with high speed video were performed through a glass cone. CH and CH₂O PLIF were also used to examine the flame structures above the cone. It is shown that in the entire flame the CH layer remains very thin, whereas the CH₂O layer is rather thick. The flame is stabilized inside the cone a short distance above the nozzle. The stabilization of the flame can be simulated by the triple-flame model but not the flamelet-quenching model. The results show that flame stabilization in the cone is a result of premixed flame front propagation and flow reversal near the wall of the cone which is deemed to be dependent on the cone angle. Flamelet based LES is shown to capture the measured CH structures whereas the predicted CH₂O structure is somewhat thinner than the experiments.     

Raman spectroscopic study of a laminar hydrogen diffusion flame in air

Spontaneous Raman spectroscopy has been employed for time-averaged, spatially-resolved measurements of temperature and species concentration in an axisymmetric, laminar hydrogen diffusion flame in quiescent air. Temperatures were obtained from vibrational Q-branch raman spectra of N₂, O₂, and H₂ and the rotational Raman spectra of N₂ and H₂, and concentrations of H₂, and N₂ were determined. The results are compared to existing numerical nonequilibrium calculations for the conditions of this experiment. Significant differences between experimental and predicted temperature and concentration profiles are observed. In particular, the flame is larger in both diameter and length and the flame zone is thicker than predicted. Some possible sources of the discrepancies are discussed.     

Stability and characteristics of NH3/CH4/air flames in a combustor fired by a double swirl stabilized burner

Compared to hydrocarbons, ammonia's low reactivity and higher NO_x emissions limit its practical application. Consequently, its implementation in combustion systems requires a different combustor geometry, by adapting existing systems or developing new ones. This study investigates the flame stability, NO emissions, and flame structure of NH₃/CH₄/air premixed flames in a novel combustor comprising a double swirl burner. A lean premixed CH₄/air mixture of equivalence ratio, Φ_out, was supplied to the outer swirl, while a NH₃/CH₄/Air mixture fed the inner swirl. The molar fraction of NH₃ in the inner fuel blend, x_NH3, was varied from 0 (pure CH₄) to 1 (pure NH₃) over far-lean to far-rich inner stream equivalence ratio, Φ_in. This new burner's stability map was established in terms of Φ_in versus x_NH3 for different Φ_out. Then, NO emissions were measured versus Φ_in for various x_NH3 and Φ_out. Finally, based on the NO emissions, eight flames were down-selected for in-flame measurements, which included temperature and OH-PLIF. The stability measurements revealed that increasing x_NH3 modifies the stability map by increasing the lean blowout limits and narrowing the flashback region. At Φ_out ≥ 0.6, a stable flame was achieved for a pure inner NH₃/air mixture. Low NO emissions were achieved in this burner configuration at x_NH3=1 by either enriching or far-leaning Φ_in. Enriching Φ_in led to a steep decrease in NO concentrations. However, to achieve low NO concentrations, precise control of Φ_out was needed. At Φ_in=1.4, 220 ppm NO at Φ_out=0.7 versus 690 at Φ_out=0.6 was measured. Moreover, substantially enriching Φ_in>1.2 led to a slight decrease in measured NO. Generally, the OH-PLIF images revealed a conical OH-layer at the burner exit. Certain flame conditions created OH-pockets inside the conical structure or formed a V-shaped OH-layer far downstream. This change in flame structure was found to impact NO emissions strongly.