Effect of partial premixing on the sooting structure of methane flames

An experimental investigation of the sooting structure of diluted methane–oxygen counterflow flames is reported for partial premixing in the following two nonpremixed flame configurations:

• Case 1:Nonpremixed flame on the oxidizer side of the stagnation plane,
• Case 2:Nonpremixed flame on the fuel side of the stagnation plane.

Effects of both fuel-side and oxidizer-side partial premixing for Cases 1 and 2 were investigated in a low-strain-rate (∼6–8 s⁻¹) counterflow flame. Computations using OPPDIF code were in excellent agreement with the measured concentrations of major species and [OH]. Distribution of measured soot volume fraction and particle sizes are presented along with measured distributions of C₂ hydrocarbon species. Soot loading can increase or decrease depending on (a) the level of partial premixing, (b) the side of partial premixing (fuel side or oxidizer side), and (c) the nonpremixed flame configuration. Of particular interest is the trend for fuel-side partial premixing of Case 1, where the peak soot loading, the peak soot particle diameter, and the thickness of the soot zone initially decrease and then increase with progressive partial premixing. The trends presented are discussed based on chemical, dilution, and flow-field effects of partial premixing on soot growth in counterflow flames. Unlike previous literature, which focused on soot inception, this work emphasizes the role of partial premixing on soot growth by taking into account the changes in the temperature–time history of soot particulates in addition to the previously reported “chemical” and “dilution” effects.     

Effects of hydrogen addition on structure and NO formation of highly CO-Rich syngas counterflow nonpremixed flames under MILD combustion regime

The present study has numerically investigated the Moderate or Intense Low oxygen Dilution (MILD) combustion regime, combustion processes and NO formation characteristics of the highly CO-rich syngas counterflow nonpremixed flames. To realistically predict the flame properties of the highly CO-rich syngas, the chemistry is represented by the modified GRI 3.0 mechanism. Computations are performed to precisely analyze the flame structure, NO formation rate, and EINO of each NO sub-mechanism. Numerical results reveal that the hydrogen enrichment and oxygen augmentation substantially influence the NO emission characteristics and the dominant NO production route in the CO-rich syngas nonpremixed flames under MILD and high temperature combustion regimes. It is found that the most dominant NO production routes are the NNH path for the lowest oxygen level (3%) and the thermal mechanism for the highest O₂ condition (21%). For the intermediate oxygen level (9%), the most dominant NO production routes are the NNH route for the hydrogen fraction up to 5%, the CO₂ path for the hydrogen fraction range from 5% to 10% and the thermal mechanism for the hydrogen fraction higher than 10%, respectively. To evaluate the contribution of the specific reaction on EINO the sensitivity coefficients are precisely analyzed for NO formation processes with the dominance of NNH/CO₂/Thermal mechanism under the highly CO-rich syngas flames.     

A mechanistic study of Soret diffusion in hydrogen–air flames

The separate and combined effects of Soret diffusion of the hydrogen molecule (H₂) and radical (H) on the structure and propagation speed of the freely-propagating planar premixed flames, and the strain-induced extinction response of premixed and nonpremixed counterflow flames, were computationally studied for hydrogen–air mixtures using a detailed reaction mechanism and transport properties. Results show that, except for the conservative freely-propagating planar flame, Soret diffusion of H₂ increases the fuel concentration entering the flame structure and as such modifies the mixture stoichiometry and flame temperature, which could lead to substantial increase (decrease) of the flame speed for the lean (rich) mixtures respectively. On the other hand, Soret diffusion of H actively modifies its concentration and distribution in the reaction zone, which in turn affects the individual reaction rates. In particular, the reaction rates of the symmetric, twin, counterflow premixed flames, especially at near-extinction states, can be increased for lean flames but decreased for rich flames, whose active reaction regions are respectively located at, and away from, the stagnation surface. However, such a difference is eliminated for the single counterflow flame stabilized by an opposing cold nitrogen stream, as the active reaction zone up to the state of extinction is always located away from the stagnation surface. Finally, the reaction rate is increased in general for diffusion flames because the bell-shaped temperature distribution localizes the H concentration to the reaction region which has the maximum temperature.     

On the similitude between lifted and burner-stabilized triple flames: a numerical and experimental investigation

We have investigated lifted triple flames and addressed issues related to flame stabilization. The stabilization of nonpremixed flames has been argued to result due to the existence of a premixing zone of sufficient reactivity, which causes propagating premixed reaction zones to anchor a nonpremixed zone. We first validate our simulations with detailed measurements in more tractable methane–air burner-stabilized flames. Thereafter, we simulate lifted flames without significantly modifying the boundary conditions used for investigating the burner-stabilized flames. The similarities and differences between the structures of lifted and burner-stabilized flames are elucidated, and the role of the laminar flame speed in the stabilization of lifted triple flames is characterized. The reaction zone topography in the flame is as follows. The flame consists of an outer lean premixed reaction zone, an inner rich premixed reaction zone, and a nonpremixed reaction zone where partially oxidized fuel and oxidizer (from the rich and lean premixed reaction zones, respectively) mix in stoichiometric proportion and thereafter burn. The region with the highest temperatures lies between the inner premixed and the central nonpremixed reaction zone. The heat released in the reaction zones is transported both upstream (by diffusion) and downstream to other portions of the flame. Measured and simulated species concentration profiles of reactant (O₂, CH₄) consumption, intermediate (CO, H₂) formation followed by intermediate consumption and product (CO₂, H₂O) formation are presented. A lifted flame is simulated by conceptualizing a splitter wall of infinitesimal thickness. The flame liftoff increases the height of the inner premixed reaction zone due to the modification of the upstream flow field. However, both the lifted and burner-stabilized flames exhibit remarkable similarity with respect to the shapes and separation distances regarding the three reaction zones. The heat-release distribution and the scalar profiles are also virtually identical for the lifted and burner-stabilized flames in mixture fraction space and attest to the similitude between the burner-stabilized and lifted flames. In the lifted flame, the velocity field diverges upstream of the flame, causing the velocity to reach a minimum value at the triple point. The streamwise velocity at the triple point is ≈0.45 m s⁻¹ (in accord with the propagation speed for stoichiometric methane–air flame), whereas the velocity upstream of the triple point equals 0.7 m s⁻¹, which is in excess of the unstretched flame propagation speed. This is in agreement with measurements reported by other investigators. In future work we will address the behavior of this velocity as the equivalence ratio, the inlet velocity profile, and inlet mixture fraction are changed.     

Liftoff and extinction characteristics of fuel- and air-stream-diluted methane-air flames

Partial premixing of fuel and oxidizer is of common occurrence in fires. However, most previous studies dealing with flame extinction have focused on nonpremixed flames. In this experimental-numerical study, we examine the effectiveness of fuel-stream versus air-stream dilution for extinguishing laminar methane-air partially premixed (PPFs) and nonpremixed flames (NPF) using the chemically inert fire suppressant CO₂. Experimental measurements were made in lifted methane-air coflow flames, while both counterflow and coflow flames were simulated using a time-accurate implicit algorithm that incorporates detailed chemistry and includes radiation effects. Both measurements and simulations show that with fuel-stream dilution, PPFs stabilize at a higher liftoff height and blow out at a lower CO₂ dilution than NPFs. In contrast, with air-stream dilution, NPFs move to a higher liftoff height and blow out at a lower CO₂ dilution than PPFs. Despite different configurations, there is remarkable similarity in the extinction characteristics of coflow and counterflow flames with regard to the level of partial premixing and air- and fuel-stream dilution. The critical fuel-stream CO₂ mole fraction required for the extinction of both counterflow and coflow flames increases as ? is increased, i.e., as the level of partial premixing is reduced. Conversely, the critical air-stream CO₂ mole fraction decreases as ? is increased. Results also indicate a crossover value of ?≈2.0, corresponding to the stoichiometric mixture fraction of fs=0.5, such that flames (including NPFs) with fs<0.5 are more difficult to extinguish with fuel-stream dilution, since oxygen is the deficient reactant, whereas flames with fs>0.5 are more difficult to extinguish with air-stream dilution, since fuel is the deficient reactant for these flames.     

Field measurements of soot volume fractions in laminar partially premixed coflow ethylene/air flames

The conditions under which soot is formed vary widely and depend upon several factors, including pressure, temperature, fuel type, combustor geometry, and extent of premixing. Although it is known that partially premixed flames (PPFs) can become either more or less sooting than their nonpremixed or premixed counterparts, the impact of partial premixing on soot formation across a large equivalence ratio and flow range is still inadequately understood. Comprehensive experimental data are relatively sparse for this important configuration. Herein, we report on soot formation in various ethylene/air PPFs utilizing full-field light extinction. The dimensionless extinction coefficient Kext is an important calibrated constant for the determination of the soot volume fraction for this measurement technique. We find that a value of Kext=7.1 provides results that are in good agreement with benchmark literature data for a nonpremixed flame. We examined the soot microstructures for two flames established at ?=∞ (i.e., nonpremixed) and 5. In both cases, the primary particles were found to be nearly spherical. In case of the nonpremixed flame the average primary soot particle diameter was ∼35 nm, but for the ?=5 flame it was ∼20 nm. However, the parameter responsible for the value of Kext is the average aggregate size and not that of the primary particles. The aggregate sizes are similar for the two flames. We consider this as verification of a constant Kext value over the entire equivalence ratio range. The addition of air to the fuel stream produces an initial increase in the flame height. Further air addition gradually decreases the flame height, which is followed by a more rapid decrease with larger premixing. Likewise, the peak soot concentration first increases with small amounts of air addition (or partial premixing of the fuel stream) and reaches a maximum value at ?∼24. With further air addition, as ? decreases below a value of 20, the soot volume fraction considerably decreases.     

The role of particles in the inhibition of counterflow diffusion flames by iron pentacarbonyl

Laser light scattering and thermophoretic sampling have been used to investigate particle formation in counterflow diffusion flames inhibited by iron pentacarbonyl Fe(CO)₅. Three CH₄-O₂-N₂ reactant mixtures are investigated, with Fe(CO)₅ added to the fuel or the oxidizer stream in each. Flame calculations that incorporate only gas-phase chemistry are used to assist in interpretation of the experimental results. In flames with the inhibitor added on the flame side of the stagnation plane, the region of particle formation overlaps with the region of high H-atom concentration, and particle formation may interfere with the inhibition chemistry. When the inhibitor is added on the non-flame side of the stagnation plane, significant condensation of metal or metal oxide particles is found, and implies that particles prevent active inhibiting species from reaching the region of high radical concentration. As the inhibitor loading increases, the maximum scattering cross section increases sharply, and the difference between the measured and predicted inhibition effect widens, suggesting that particle formation is the cause of the deviation. Laser-based particle size measurements and thermophoretic sampling in low strain rate flames show that the particles have diameters between 10 nm and 30 nm. Thermophoresis affects the nanoparticle distribution in the flames, in some cases causing particles to cross the stagnation plane. The scattering magnitude in the counterflow diffusion flames appears to be strongly dependent on the residence time, and relatively independent of the peak flame temperature.     

Soot and NO formation in methane–oxygen enriched diffusion flames

NO and soot formation were investigated both numerically and experimentally in oxygen-enriched counterflow diffusion flames. Two sets of experiments were conducted. In the first set, the soot volume fraction was measured as a function of oxygen content in the oxidizer jet at constant strain rate (20 s⁻¹). In the second set of experiments, the soot volume fraction was measured as a function of strain rate variation from 10 to 60 s⁻¹ and at constant oxygen content on the oxidizer side. A soot model was developed based on a detailed C₆ gas phase chemistry. The soot and molecular radiation were taken into account. Numerical results were verified against experimental data. The soot volume fraction was predicted with the maximum discrepancy less than 30% for all cases considered. It was found that oxygen variation significantly modified the diffusion flame structure and the flame temperature, resulting in a substantial increase of soot. The temperature increase promotes aromatics production in the fuel pyrolysis zone and changes the relative contributions of the thermal and Fenimore mechanisms into NO formation. As the strain rate increases, the residence time of incipient soot particles in the high temperature zone is reduced and the total amount of soot decreases. High concentration of soot in the flame leads to enhancement of radiant heat exchange: the reduction of temperature due to radiation was found to be between 10 and 50 K. This caused a reduction of peak NO concentrations by 20%–25%. The increase of oxygen content in the oxidizer stream resulted in a reduction of the distance between the plane of the maximum temperature and the stagnation plane.     

An experimental and numerical investigation of n-heptane/air counterflow partially premixed flames and emission of NOx and PAH species

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 NO_x 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 NO_x 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, C₃H_x) 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 NO_x 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, NO_x 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.     

燃料型NO在对冲扩散火焰中的生成和还原特性

在CH4/空气对冲扩散火焰的燃料侧人为地掺混一定体积分数的NH3或HCN,数值模拟燃料型NO的生成和还原.模拟使用CHEMKIN和GRI3.0反应机理.结果表明,NO的生成和还原集中在火焰锋面,在火焰中心附近体积分数值最大.在燃料侧,NO的体积分数分布与燃料N的含量及NO初始体积分数值相关,而在空气侧主要受燃料N的影响.不加燃料N时,火焰中NO主要为热力型NO,受拉伸的影响大于燃料的影响;加入燃料N时,火焰中的NO主要为燃料型NO,受燃料体积分数的影响大于拉伸的影响,含量相同时NH3比HCN有更明显的促进NO生成的作用.     

A detailed numerical study of NOx kinetics in low calorific value H2/CO syngas flames

The present study provides an extensive and detailed numerical analysis of NO_x chemical kinetics in low calorific value H₂/CO syngas flames utilizing predictions by five chemical kinetic mechanisms available out of which four deal with H₂/CO while the fifth mechanism (GRI 3.0) additionally accounts for hydrocarbon chemistry. Comparison of predicted axial NO profiles in premixed flat flames with measurements at 1 bar, 3.05 bar and 9.15 bar shows considerably large quantitative differences among the various mechanisms. However, at each pressure, the quantitative reaction path diagrams show similar NO formation pathways for most of the mechanisms. Interestingly, in counterflow diffusion flames, the quantitative reaction path diagrams and sensitivity analyses using the various mechanisms reveal major differences in the NO formation pathways and reaction rates of important reactions. The NNH and N₂O intermediate pathways are found to be the major contributors for NO formation in all the reaction mechanisms except GRI 3.0 in syngas diffusion flames. The GRI 3.0 mechanism is observed to predict prompt NO pathway as the major contributing pathway to NO formation. This is attributed to prediction of a large concentration of CH radical by the GRI 3.0 as opposed to a relatively negligible value predicted by all other mechanisms. Also, the back-conversion of NNH into N₂O at lower pressures (2–4 bar) was uniquely observed for one of the five mechanisms. The net reaction rates and peak flame temperatures are used to correlate and explain the differences observed in the peak [NO] at different pressures. This study identifies key reactions needing assessment and also highlights the need for experimental data in syngas diffusion flames in order to assess and optimize H₂/CO and nitrogen chemistry.     

Effects of ammonia substitution on extinction limits and structure of counterflow nonpremixed hydrogen/air flames

The potential of partial ammonia substitution to improve the safety of hydrogen use was evaluated computationally, using counterflow nonpremixed ammonia/hydrogen/air flames at normal temperature and pressure. The ammonia-substituted hydrogen/air flames were considered using a recent kinetic mechanism and a statistical narrow-band radiation model for a wide range of flame strain rates and the extent of ammonia substitution. The effects of ammonia substitution on the extinction limits and structure, including nitrogen oxide (NO_x) and nitrous oxide (N₂O) emissions, of nonpremixed hydrogen/air flames were investigated. Results show reduction of the high-stretch extinction (i.e., blow-off) limits, the maximum flame temperature and the concentration of light radicals (e.g., H and OH) with ammonia substitution in hydrogen/air flames, supporting the potential of ammonia as a carbon-free, clean additive for improving the safety of hydrogen use in nonpremixed hydrogen/air flames. For high-stretched flames, however, NO_x and N₂O emissions substantially increase with ammonia substitution even though ammonia substitution reduces flame temperature, implying that chemical effects (rather than thermal effects) of ammonia substitution on flame structure are dominant. Radiation effects on the extinction limits and flame structure are not remarkable particularly for high-stretched flames.     

Hydrogen addition effect on NO formation in methane/air lean-premixed flames at elevated pressure

The present study investigates freely propagating methane/hydrogen lean-premixed laminar flames at elevated pressures to understand the hydrogen addition effect of natural gas on the NO formation under the conditions of industrial gas turbine combustors. The detailed chemical kinetic model which was used in the previous study on the NO formation in high pressure methane/air premixed flames was adopted for the present study to analyze NO formation of methane/hydrogen premixed flames. The present mechanism shows good agreement with experimental data for methane/hydrogen mixtures, including ignition delay times, laminar burning velocities, and NO concentration in premixed flames. Hydrogen addition to methane/air mixtures with maintaining methane content leads to the increase of NO concentration in laminar premixed flames due to the higher flame temperature. Methane/hydrogen/argon/air premixed flames are simulated to avoid the flame temperature effect on NO formation over a pressure range of 1–20atm and equivalence ratio of 0.55. Kinetic analyses shows that the N₂O mechanism is important on NO formation for lean flames between the reaction zone and postflame region, and thermal NO is dominant in the postflame zone. The hydrogen addition leads to the increase of NO formation from prompt NO and NNH mechanisms, while NO formation from thermal and N₂O mechanisms are decreased. Additionally, the NO formation in the postflame zone has positive pressure dependencies for thermal NO with an exponent of 0.5. Sensitivity analysis results identify that the initiation reaction step for the thermal NO and the N₂O mechanism related reactions are sensitive to NO formation near the reaction zone.     

Numerical study on laminar burning velocity and NO formation of premixed methane–hydrogen–air flames

Numerical study on laminar burning velocity and NO formation of the premixed methane–hydrogen–air flames was conducted at room temperature and atmospheric pressure. The unstretched laminar burning velocity, adiabatic flame temperature, and radical mole fractions of H, OH and NO are obtained at various equivalence ratios and hydrogen fractions. The results show that the unstretched laminar burning velocity is increased with the increase of hydrogen fraction. Methane-dominated combustion is presented when hydrogen fraction is less than 40%, where laminar burning velocity is slightly increased with the increase of hydrogen addition. When hydrogen fraction is larger than 40%, laminar burning velocity is exponentially increased with the increase of hydrogen fraction. A strong correlation exists between burning velocity and maximum radical concentration of H + OH radicals in the reaction zone of premixed flames. High burning velocity corresponds to high radical concentration in the reaction zone. With the increase of hydrogen fraction, the overall activation energy of methane–hydrogen mixture is decreased, and the inner layer temperature and Zeldovich number are also decreased. All these factors contribute to the enhancement of combustion as hydrogen is added. The curve of NO versus equivalence ratio shows two peaks, where they occur at the stoichiometric mixture due to Zeldovich thermal-NO mechanism and at the rich mixture with equivalence ratio of 1.3 due to the Fenimore prompt-NO mechanism. In the stoichiometric flames, hydrogen addition has little influence on NO formation, while in rich flames, NO concentration is significantly decreased. Different NO formation responses to stretched and unstretched flames by hydrogen addition are discussed.     

Counterflow diffusion flames

Laminar counterflow diffusion flames are generally referred to as the pure diffusion flame. This paper reviews experimental studies of these counterflow diffusion flames and presents a detailed summary of our present understanding of them. The paper begins by classifying these laminar counterflow diffusion flames into four types: (I) the counterflow diffusion flame between two opposed jets, (II) the flat, counterflow diffusion flame between two opposed matrix burners, (III) the counterflow diffusion flame in the forward stagnation region of a spherical or hemispherical porous burner, and (IV) the counterflow diffusion flame in the forward stagnation region of a cylindrical porous burner. Next, the characteristics of these counterflow diffusion flames are presented, and these flames are then shown as being suitable for a fundamental study of diffusion flame and its combustion characteristics, especially, (1) for a detailed study of the structure of a laminar diffusion flame and of high-temperature flame kinetics, (2) for an accurate study of combustion characteristics closely related to flame-extinction phenomena (e.g. dilution limits of diffusion flames, the overall reaction rates for fuel-oxidant combinations, and the effectiveness of inhibitors), and (3) for a careful study of the various properties of a flame in an electric field.     

Stable negative edge flame formation in a counterflow burner

In nonpremixed combustion, edge flames can form as a region of flame propagation or flame recession. Forwardly propagating edge flames, as occur in lifted flames, have a local gas velocity at the flame edge that is from unburned partially premixed fuel and air into the flame. These flames represent an ignition process, and permit the flame itself to either stabilize against an incoming gas stream or propagate into unburned fuel and air. Negative edge flames represent the opposite case of a local gas velocity from burned products through the flame edge. The negative edge flame represents a local extinction process, and occurs, for example, during vortex-induced extinction of a nonpremixed flame sheet. A technique for generating steady negative edge flames in a standard counterflow burner is presented, which permits detailed examination of their properties. A coannular counterflow burner is used to create a strain gradient that quenches a central diffusion flame. Unlike previous research on strain-induced flame edges, the axisymmetric flow field ensures gas flow from products through the edge. Measurements of the edge flame's sensitivity to global strain rates and fuel mixtures are presented, along with measurements of the edge flame structure using OH fluorescence and CH emission imaging.     

The structure of partially premixed methane flames in high-intensity turbulent flows

Direct numerical simulations (DNS) are conducted to study the structure of partially premixed and non-premixed methane flames in high-intensity two-dimensional isotropic turbulent flows. The results obtained via “flame normal analysis” show local extinction and reignition for both non-premixed and partially premixed flames. Dynamical analysis of the flame with a Lagrangian method indicates that the time integrated strain rate characterizes the finite-rate chemistry effects and the flame extinction better than the strain rate. It is observed that the flame behavior is affected by the “pressure-dilatation” and “viscous-dissipation” in addition to strain rate. Consistent with previous studies, high vorticity values are detected close to the reaction zone, where the vorticity generation by the “baroclinic torque” was found to be significant. The influences of (initial) Reynolds and Damköhler numbers, and various air-fuel premixing levels on flame and turbulence variables are also studied. It is observed that the flame extinction occurs similarly in flames with different fuel-air premixing. Our simulations also indicate that the CO emission increases as the partial premixing of the fuel with air increases. Higher values of the temperature, the OH mass fraction and the CO mass fraction are observed within the flame zone at higher Reynolds numbers.