Conditional moment closure prediction of soot formation in turbulent, nonpremixed ethylene flames

Results obtained from incorporating a semiempirical soot model into a first-order conditional moment closure (CMC) approach to modeling turbulent nonpremixed flames of ethylene and air are presented. Soot formation is determined via the solution of two transport equations for soot mass fraction and particle number density, with acetylene and benzene employed as the incipient species responsible for soot nucleation, and the concentrations of these species calculated using a detailed gas-phase kinetic scheme involving 463 reactions and 70 species. The study focuses on the influence of differential diffusion of soot particles on soot volume fraction predictions. The results of calculations are compared with experimental data for three sooting ethylene flames and, in general, predictions of mixing and temperature fields within the three flames show good agreement with data. Soot volume fraction predictions are found to be in significantly better accord with data when differential diffusion is accounted for in the CMC-based soot model, supporting the importance of such effects in sooting flames, as previously noted by Kronenburg et al. in relation to methane combustion. Overall, the study demonstrates that the CMC-based soot model, when used in conjunction with a model of differential diffusion effects, is capable of accurately predicting soot formation in turbulent nonpremixed ethylene-air flames.     

Stochastic modeling of finite-rate chemistry effects in hydrogen-air turbulent jet diffusion flames with helium dilution

Stochastic simulations of turbulent hydrogen-air jet diffusion flames at three different dilution rates with helium are implemented using the ‘one-dimensional turbulence’ (ODT) model. The approach is based on one-dimensional unsteady solution of boundary layer equations to represent molecular processes and a stochastic implementation of turbulent advection. The 1D scalar and streamwise momentum profiles represent radial profiles within the flames; while, the unsteady evolution of the solution is interpreted as a downstream evolution of the radial scalar and streamwise momentum profiles. Multiple realizations of jet simulations are used to compute conditional statistics of major species, NO, and temperature. The ODT computations are implemented with a five-step reduced mechanism for hydrogen combustion and an optically-thin radiation model. Computed conditional statistics of temperature, major and minor species are compared to the experimental data from a set of documented flames at Sandia National Labs. Reasonable qualitative and quantitative agreement between computed and measured statistics is found, including very good predictions of NO mean and RMS profiles. Both computation and experiment exhibit the role of dilution in enhancing finite-rate chemistry effects, which vary as a function of downstream distance and fuel dilution.     

The effects of hydrogen addition on soot formation in counterflow diffusion n-heptane flames

The effects of H₂ addition on soot formation are investigated in counterflow diffusion n-heptane flames. Three effects including chemical, thermal, and dilution are fully isolated and characterized by additions of H₂, He, and Ar. Soot volume fractions are measured using LE-calibrated LII technique, and flame temperatures are measured using OH-TLAF method along with a thermocouple. Numerical simulations are conducted with a detailed mechanism with soot model. The simulated soot volume fractions and flame temperatures are in good agreement with experimental data. The experimental results show that H₂ addition can greatly reduce the soot formation. It is also found that the chemical and dilution effects suppress soot formation, while the thermal effect with increasing flame temperature promotes soot formation. Kinetic analysis suggests that HACA growth rate could be the dominant factor that controls the final soot formation through the three effects due to H₂ addition.     

Experimental and kinetic studies of soot formation in methanol-gasoline coflow diffusion flames

Methanol has been considered to be a potential alternative fuel to reduce soot emissions from GDI engine. In order to fully understand the effect of methanol addition on soot formation, the 2-D distribution of soot volume fraction in methanol/gasoline laminar diffusion flames was measured quantitatively with two-color laser induced incandescence (TC-LII) technique. In addition, the Methanol-TRF-PAH mechanism is constructed and used to analyze the formation pathways of soot precursors based on the CHEMKIN PRO 0-D constant pressure reactor. In this experiment, the blending ratio of methanol/gasoline was set as M0/20/40/60/80. Considering the carbon content decreasing due to methanol addition, carbon mass flow rate was remained constant. The experimental results showed that methanol is able to decrease the soot significantly, while the effect of methanol on soot reduction is weakened with the increasing methanol ratio. Compared with pure gasoline, the average soot volume fraction in the M20, M40, M60, and M80 flames decrease by 48.2%, 70.4%, 83.8%, and 97.7%, and the peak soot volume fraction decrease by 41.5%, 64.1%, 75.8% and 91.8% respectively. There is little soot formation in the M80 flame, inferring the pure methanol hardly forms soot. The kinetic analysis showed that mole fraction of A1-A4 decrease with the increasing methanol ratio. For the toluene-containing fuel M0-M80, A1 is mainly formed by C₆H₅CH₃ + H = A1 + CH₃ and oxidized by A1 + OH = A1- + H₂O. A4 is mainly produced by C₆H₅CH₂ + C₉H₇ = A4 + 2H₂ and oxidized by H-abstraction reaction with H or OH radical. The major reaction pathways of A1 and A4 formation are consistent under different methanol blending ratios. The soot reduction as methanol added mainly attributes to aromatics dilution effect. In addition, the formation process of soot precursors is largely affected by chemical processes of OH, CH₃, HO₂ radicals.     

Pressure dependence of NO formation in laminar fuel-rich premixed CH4/air flames

Effects of pressure on NO formation in CH₄/air flames at a fixed equivalence ratio of 1.3 are investigated. The axial profiles of temperature, OH, CH, and NO mole fractions are measured using laser-induced fluorescence and compared with one-dimensional flame calculations. The measured and calculated temperature, CH, and NO profiles in free flames are observed to vary upon increasing the pressure from 40 to 75 Torr, following a scaling law derived for a chemical mechanism containing only second-order reactions. At pressures 300–760 Torr, the measurements and calculations in burner-stabilized flames show increasing flame temperature and NO mole fractions when the mass flux is increased linearly with pressure, while the CH profiles remain unchanged. The observed deviation from the scaling law in the temperature profiles arises from the increasing contribution of three-body reactions to the flame front propagation velocity, leading to a decrease in the degree of burner stabilization. The deviation from the pressure scaling law for the NO mole fractions is due to the temperature dependence of the rate coefficient for the reaction between CH and N₂ and the fact that the temperature profiles themselves do not scale. In contrast, the surprisingly good scaling of the CH mole fractions with pressure indicates the dominant role of two-body reactions participating in the chain of chemical reactions leading to CH formation. The calculations using GRI-Mech 3.0 substantially overpredict (up to 50%) the measured nitric oxide concentrations for all pressures studied. The observed differences in the NO mole fraction may be addressed by improving the CH prediction.     

The role of turbulent fluctuations on radiative emission in hydrogen and hydrogen-enriched methane flames

A theoretical analysis is reported in the present work to quantify the increase of radiative emission due to turbulence for hydrogen and hydrogen-enriched methane diffusion flames burning in air. The instantaneous thermochemical state of the reactive mixture is described by a flamelet model along with a detailed chemical mechanism. The shape of the probability density function (pdf) of mixture fraction is assumed. The results show that turbulent fluctuations generally contribute to reduce the Planck mean absorption coefficient of the medium, in contrast with the blackbody emissive power, which is significantly increased by turbulence. If the turbulence level is relatively small, the influence of turbulence on the absorption coefficient is marginal. Otherwise, fluctuations of the absorption coefficient of the medium should be taken into account. The scalar dissipation rate and the fraction of radiative heat loss have a much lower importance than the turbulence intensity on the mean radiative emission.     

Investigation of the effect of air turbulence intensity on NOx emission in non-premixed hydrogen and hydrogen-hydrocarbon composite fuel combustion

In this paper, the effect of air turbulence intensity on NO formation in the combustion of mixed hydrogen-hydrocarbon fuel is numerically studied. The fuels used in this study are 100% H₂, 70% H₂ + 30% CH₄, 10% H₂ + 90% CH₄ and 100% CH₄. Finite volume method is utilized to solve the governing equations. The obtained results using realizable k-ε and β-PDF models show good agreement with other numerical and experimental results. The results show that increasing air turbulence intensity decreases NO concentration in the flame zone and at the combustor outlet. With increasing air turbulence intensity, maximum decreasing of NO at the combustor outlet is for the case of pure hydrogen fuel. It is also found that adding hydrogen to methane rises the peak temperature of the flame.     

Effect of CO2/N2/CH4 dilution on NO formation in laminar coflow syngas diffusion flames

The effect of CO₂/N_2/CH₄ dilution on NO formation in laminar coflow H₂/CO syngas diffusion flames was experimentally and numerically investigated. The results reveal that the NO emission index increases with H₂/CO mole ratio. In all cases, CO₂/N₂/CH₄ dilution can reduce the peak temperature of syngas flame and have the ability to reduce peak flame temperature is decreased in the following order: CO₂>N₂>CH₄. CO₂/N₂ dilution reduces the NO formation in syngas flame while CH₄ dilution promotes the NO formation. Besides, the dilution of CO₂/N₂/CH₄ can reduce the peak mole fraction of OH and its variations with H₂/CO mole ratio and dilution ratio show the same trend as the peak flame temperature variations. The height of the flame with CO₂ and N₂ dilution increases with dilution ratio. The flame with CH₄ dilution becomes higher and wider with the increase of dilution ratio.     

Effect of differential diffusion on turbulent lean premixed hydrogen enriched flames through structure analysis

This study presents the flame structure influenced by the differential diffusion effects and evaluates the structural modifications induced by the turbulence, thus to understand the coupling effects of the diffusively unstable flame fronts and the turbulence distortion. Lean premixed CH₄/H₂/air flames were conducted using a piloted Bunsen burner. Three hydrogen fractions of 0, 30% and 60% were adopted and the laminar flame speed was kept constant. The turbulence was generated with a single-layer perforated plate, which was combined with different bulk velocities to obtain varied turbulence intensities. Quasi-laminar flames without the plate were also performed. Explicit flame morphology was obtained using the OH-PLIF. The curvature, flame surface density and turbulent burning velocity were measured. Results show that the preferential transport of hydrogen produces negatively curved cusps flanked with positively curved bulges, which are featured by skewed curvature pdfs and consistent with the typical structure caused by the Darrieus-Landau instability. Prevalent bulge-cusp like wrinkles remain with relatively weak turbulence. However, stronger turbulence can break the bulges to be finer, and induce random positively curved cusps, therefore to destroy the bulge-cusp structures. Evident positive curvatures are generated in this process modifying the skewed curvature pdfs to be more symmetric, while the negative curvatures are not affected seriously. From low to high turbulence intensities, the hydrogen addition always strengthens the flame wrinkling. The augmentation of flame surface density and turbulent burning velocity with hydrogen is even more obvious at higher turbulence intensity. It is suggested that the differential diffusion can persist and even be strengthened with strong turbulence.     

Effect of hydrogen addition on NOx formation in high-pressure counter-flow premixed CH4/air flames

A laboratory-scale laminar counterflow burner was used to investigate NO formation in high pressure premixed CH₄/H₂/air flames. New experimental results on NO measurements by LIF were obtained at high pressure in CH₄/H₂/air flames with H₂ content fixed at 20% in the fuel at pressures ranging from 0.1 to 0.7 MPa and an equivalence ratio progressively decreased from 0.74 to 0.6. The effects of hydrogen addition, equivalence ratio and pressure are discussed. These results are satisfactorily compared to the simulations using two detailed mechanisms: GDFkin®3.0_NOmecha2.0 and the mechanism from Klippenstein et al., which are the most recent high-pressure NOx formation mechanisms available in the literature. A kinetic analysis based on Rate of Production/Rate of Consumption and sensitivity analyses of NO is then presented to identify the main pathways that lead to the formation and consumption of NO. In addition, the effect of hydrogen addition on NO formation pathways is described and analysed.     

Piloted jet flames of CH4/H2/air: Experiments on localized extinction in the near field at high Reynolds numbers

Measurements of temperature and major species concentrations, based on the simultaneous line-imaged Raman/Rayleigh/CO-LIF technique, are reported for piloted jet flames of CH₄/H₂ fuel with varying amounts of partial premixing with air (jet equivalence ratios of ?_j = 3.2, 2.5, 2.1 corresponding to stoichiometric mixture fraction values of ξ_st = 0.35, 0.43, 0.50, respectively) and varying degrees of localized extinction. Each jet flame is operated at a fixed and relatively high exit Reynolds number (60,000 or 67,000), and the probability of localized extinction is increased in several steps by progressively decreasing the flow rate of the pilot flame. Dimensions of the piloted burner, originally developed at Sydney University, are the same as for previous studies. The present measurements complement previous results from piloted CH₄/air jet flames as targets for combustion model calculations by extending to higher Reynolds number, including more steps in the progression of each flame from a fully burning state to a flame with high probability of local extinction, and adding the degree of partial premixing as an experimental parameter. Local extinction in these flames occurs close to the nozzle near a downstream location of four times the jet exit diameter. Consequently, these data provide the additional modeling challenge of accurately representing the initial development of the reacting jet and the near-field mixing processes.     

One-dimensional turbulence model simulations of autoignition of hydrogen/carbon monoxide fuel mixtures in a turbulent jet

The autoignition of hydrogen/carbon monoxide in a turbulent jet with preheated co-flow air is studied using the one-dimensional turbulence (ODT) model. The simulations are performed at atmospheric pressure based on varying the jet Reynolds number and the oxidizer preheat temperature for two compositions corresponding to varying the ratios of H₂ and CO in the fuel stream. Moreover, simulations for homogeneous autoignition are implemented for similar mixture conditions for comparison with the turbulent jet results. The results identify the key effects of differential diffusion and turbulence on the onset and eventual progress of autoignition in the turbulent jets. The differential diffusion of hydrogen fuels results in a reduction of the ignition delay relative to similar conditions of homogeneous autoignition. Turbulence may play an important role in delaying ignition at high-turbulence conditions, a process countered by the differential diffusion of hydrogen relative to carbon monoxide; however, when ignition is established, turbulence enhances the overall rates of combustion of the non-premixed flame downstream of the ignition point.     

Different chemical effect of hydrogen addition on soot formation in laminar coflow methane and ethylene diffusion flames

Previous studies showed that adding hydrogen (H₂) can have an opposite chemical effect on soot formation: its chemical effect enhances and suppresses soot formation in methane (CH₄) and ethylene (C₂H₄) diffusion flames, respectively. Such opposite chemical effect of H₂ (CE-H₂) remains unresolved. The different CE-H₂ is studied numerically in the two laminar coflow diffusion flames. A detailed chemical mechanism with the addition of a chemically inert virtual species FH₂ is used to model the gas-phase combustion chemistry in this study. Particularly, a reaction pathway analysis was performed based on the numerical results to gain insights into how H₂ addition to fuel affects the pathways leading to the formation of benzene (A₁) in CH₄ and C₂H₄ flames. The numerical results show that the CE-H₂ in CH₄ diffusion flame to prompt soot formation is ascribed that the higher mole fraction of H atom promotes the formation of A₁ and Acetylene (C₂H₂) and leads to higher nucleation rate and eventually higher soot surface growth rate. In contrast, adding H₂ to C₂H₄ diffusion flames decreases soot nucleation and surface growth rate. The lower soot nucleation rate is due to the lower mole fractions of pyrene (A₄), while the lower soot surface growth rate is due to the lower mole fractions of H atom and C₂H₂, higher mole fraction of H₂ and lower soot nucleation rate. Furthermore, the CE-H₂ in C₂H₄ diffusion flames promotes the formation of A₁, but suppresses the formation of A₄.     

Effect of hydrogen enrichment on flame broadening of turbulent premixed flames in thin reaction regime

An experimental study to identify the effect of hydrogen enrichment and differential diffusion on the flame broadening is conducted. Turbulent lean premixed flames in the Broadened Preheat–Thin Reaction (BP-TR) regime are obtained. The flames are stabilized on a Bunsen burner and CH₄/H₂/air mixtures are adopted with three hydrogen fractions of 0, 30% and 60%. The preheat zone and heat release zone are captured with the multi-species Planar Laser-Induced Fluorescence (PLIF) of OH and CH₂O radicals. Flame thicknesses of the preheat and heat release layers are measured. Results show broadened preheat zone and thin heat release layers for the flames, as predicted by the BP-TR regime. The preheat zone thickness can be increased to about 3–6 times compared to the laminar preheat thickness. An apparently decreased preheat zone thickness with hydrogen addition is observed. The differential diffusion is anticipated to locally thicken the heat release zone along the flame front. The mean heat release thickness is nearly not affected by the turbulence or hydrogen addition.     

Evaluation of the influence of OEC on soot formation and thermal radiation in confined acetylene diffusion flames

The effect of OEC on soot formation and thermal radiation was studied in confined acetylene diffusion flames. Confined flames are widely used in industrial settings. The flames were produced in a combustion chamber with a burner operating with a parallel annular coaxial flow of the oxidizer. The soot concentration was calculated by the laser-induced light extinction method. The thermal radiation was measured with a radiometer in the narrow band of influence of soot radiation. The oxygen content in the combustion air was less than 30% – 21 to 25% – which does not require significant retrofitting of existing equipment when combustion conditions are varied. The results suggest that the use of OEC enables soot formation and thermal radiation in confined acetylene flames to be managed and controlled.     

Dilution effects analysis on NOx emissions of opposed-jet H2/CO syngas diffusion flames

Syngas is a promising alternative fuel for stationary power generation due to cleaner combustion than convectional fossil fuels. During the gasification processes, the by-products of CO₂, H₂O, or N₂ may be present in the syngas mixture to control the flame temperature and emissions. Several studies indicated that syngas with dilutions is capable of reducing pollutant emissions such as NO_x emissions. This work applied a numerical model of opposed-jet diffusion fames to explore the dilution effects on NO_x formation and differentiate the inert effect, thermal/diffusion effect, chemical effect, and radiation effect from CO₂, H₂O, or N₂ dilutions. The numerical study was performed by a revised OPPDIF program coupling with narrowband radiation model and detail chemical mechanism. The dilution effects on NO_x formation were analyzed by comparing the realistic and hypothetical cases. Regardless the diluent types, the inert effect is the main cause to reduce NO production, followed by chemical effect and radiation effect. The thermal/diffusion effect may promote NO formation because the preferential diffusion due to different diffusivities between diluents and syngas magnifies the reaction rate locally. CO₂ dilution reduces NO by radiation effect at low strain rate, and contributes NO reduction by chemical effect at high strain rate. At the same dilution percentage, CO₂ dilution reduces NO production the most, followed by H₂O and N₂. Besides the thermal/diffusion effect, the chemical effect of H₂O enhances NO production through thermal route and reburn route.     

Numerical study of the effect of H2O diluents on NOx and CO formation in turbulent premixed methane-air flame

The interaction of turbulence–combustion inside the flame field is studied in a Launder-Sharma Low Reynolds Number (LS-LRN) k−ε/EDM framework, while suitable coefficients have been utilized in the code. A finite volume method (FVM) with staggered grids was applied to discrete set of governing equations. SIMPLE algorithm is applied with a fine grid resolution. The convective terms are discretized using Power Law Scheme (PLS). The system of governing equations is solved simultaneously using numerical or TDMA finite difference methods (Tri-Diagonal Matrix Algorithm). By implementation of the Zeldovich and Westbrook-Dryer mechanisms, NO_x and CO concentrations were obtained, respectively. It is illustrated that the implemented LS-LRN-k−ε/EDM method with the new coefficients by shorter runtimes has very good agreement with previously published experimental measurements. Increasing the H₂O diluent at the inlet leads to an increase in the temperature, which increases the NO_x and CO near the entrance, but gradually towards the outlet of the combustion chamber. The energy absorbed by H₂O leads to a severe decrease in temperature and subsequent reduction in the amount of NO_x and CO emissions. With increasing H₂O diluent, changes in temperature are not very significant, while changes in pollutants CO and especially NO_x, are remarkable. With the increase of H₂O diluent, the maximum amount of CO emission displaces towards the inlet of the combustion chamber. However, it should be noted that, at a specific value of H₂O diluent, the length of the combustion chamber should not be less than critical value, causing the exhaust of the pollutant with large volume to the environment. After the critical point, the increase in the length of the chamber has little effect on reduction of the pollutant exhaust. However, by increasing the H₂O diluent, enclosures with smaller length can be utilized.     

Effects of water vapor addition to the air stream on soot formation and flame properties in a laminar coflow ethylene/air diffusion flame

The effects of adding water vapor to the air stream on flame properties and soot volume fraction were investigated numerically in a laminar coflow ethylene/air diffusion flame at atmospheric pressure by solving the fully elliptic conservation equations and using a detailed C₂ reaction mechanism including PAH up to pyrene and detailed thermal and transport properties. Thermal radiation was calculated using the discrete-ordinates method and a statistical narrow-band correlated-k based wide band model for the absorption coefficients of CO₂ and H₂O. Soot formation was modeled using a PAH based inception model and the HACA mechanism for surface growth and oxidation. Addition of water vapor significantly reduces radiation heat loss from the flame primarily through reduced soot loading and flame temperature. The added water vapor affects soot formation and flame properties through not only dilution and thermal effects, but also through chemical effect. The chemical effect is as significant as the dilution and thermal effects. The primary pathway for the chemical effect of water vapor is the reverse reaction of OH + H₂ ↔ H + H₂O. Our numerical results confirm that the reduced H radical concentration leads to lower PAH concentrations and consequently lower soot inception rates. In contrast, the radiation effect due to the added water vapor was found to have a minor influence on both flame structure and soot formation in the laminar diffusion flame investigated.     

Synergistic effect on soot formation in counterflow diffusion flames of ethylene-propane mixtures with benzene addition

The characteristics of the formation of polycyclic aromatic hydrocarbon (PAH) and soot in counterflow diffusion flames of ethylene/propane mixtures have been investigated experimentally to identify the effect of fuel structure. The synergistic effect, that is, the enhancement of PAH and soot formation by the fuel mixing of ethylene and propane has been further analyzed to examine the suggested mechanisms based on the competition between PAH and soot growths through the H-abstraction-C₂H₂-addition (HACA) mechanism and the incipient ring formation through the propargyl recombination reaction. To mitigate the effect of incipient ring formation on the synergistic effect, a small amount of benzene was added to the fuel stream. Planar laser-induced incandescence and laser-induced fluorescence techniques were employed to measure relative soot volume fractions and PAH concentrations, respectively. Results showed that the synergistic effect on soot formation remained, even though the synergistic effects for relatively small aromatics mitigated with the benzene addition. Larger size PAHs have shown enhanced synergistic effects compared to smaller size PAHs regardless of benzene addition. These results implied that the role of propane mixing on the synergistic effect cannot be explained solely by the incipient ring formation via a propargyl recombination reaction; thus, it is suggested that the C₃ pathways could also contribute to the growth of PAH species.