Influence of pressure on near nozzle flow field and soot formation in laminar co-flow diffusion flames

Soot formation from combustion devices, which tend to operate at high pressure, is a health and environmental concern, thus investigating the effect of pressure on soot formation is important. While most fundamental studies have utilised the co-flow laminar diffusion flame configuration to study the effect of pressure on soot, there is a lack of investigations into the effect of pressure on the flow field of diffusion flames and the resultant influence on soot formation. A recent work has displayed that recirculation zones can form along the centreline of atmospheric pressure diffusion flames. This present work seeks to investigate whether these zones can form due to higher pressure as well, which has never been explored experimentally or numerically. The CoFlame code, which models co-flow laminar, sooting, diffusion flames, is validated for the prediction of recirculation zones using experimental flow field data for a set of atmospheric pressure flames. The code is subsequently utilised to model ethane-air diffusion flames from 2 to 33 atm. Above 10 atm, recirculation zones are predicted to form. The reason for the formation of the zones is determined to be due to increasing shear between the air and fuel steams, with the air stream having higher velocities in the vicinity of the fuel tube tip than the fuel stream. This increase in shear is shown to be the cause of the recirculation zones formed in previously investigated atmospheric flames as well. Finally, the recirculation zone is determined as a probable cause of the experimentally observed formation of a large mass of soot covering the entire fuel tube exit for an ethane diffusion flame at 36.5 atm. Previously, no adequate explanation for the formation of the large mass of soot existed.     

Effects of benzene,cyclo-hexane and n-hexane addition to methane on soot yields in high-pressure laminar diffusion flames

Effects of doping high pressure methane diffusion flames with benzene, cyclo-hexane and n-hexane were investigated to assess the sooting propensity of three hydrocarbons with six carbons at elevated pressures. Amount of liquid hydrocarbons added to methane constituted 7.5% of the total carbon content of the fuel stream. The pressure range investigated extended up to 10 bar and the experiments were carried out in a high pressure combustion chamber capable of establishing stable laminar diffusion flames with various fuels at elevated pressures and was used in similar experiments previously. Temperatures and soot volume fractions were measured using the spectral soot emission technique capturing spectrally-resolved line-of-sight intensities which were subsequently inverted using an Abel type algorithm to obtain radial distributions assuming that the flames are axisymmetric. The total mass carbon flow of the fuel stream was kept constant at 0.524 mg/s in neat methane, benzene-doped methane, cyclo-hexane-doped methane, and n-hexane-doped methane flames to have tractable measurements at all pressures. Measured maximum soot volume fractions and evaluated maximum soot yields showed that benzene-doped methane flame had the higher values than cyclo-hexane doped methane flames which in turn had higher values than n-hexane doped methane flames at all pressures. Sooting propensity dependence of the three hydrocarbons on pressure can be ranked as, in descending order, n-hexane, cyclo-hexane, and benzene; however, the difference between pressure dependencies of n-hexane and cyclo-hexane was within the measurement error margins. Ratio of soot yields of benzene to n-hexane doped flames changed from about 2 at 2 bar to 1.2 at 10 bar; the ratio of benzene to cyclo-hexane doped flames showed similar trends.     

Effects of gas and soot radiation on soot formation in counterflow ethylene diffusion flames

Numerical study of soot formation in counterflow ethylene diffusion flames at atmospheric pressure was conducted using detailed chemistry and complex thermal and transport properties. Soot kinetics was modelled using a semi-empirical two-equation model. Radiation heat transfer was calculated using the discrete-ordinates method coupled with an accurate band model. The calculated soot volume fractions are in reasonably good agreement with the experimental results in the literature. The individual effects of gas and soot radiation on soot formation were also investigated.     

On the sudden reversal of soot formation by oxygen addition in DME flames

Dimethyl ether (DME) is a non-toxic and renewable fuel known for its soot emissions reduction tendencies. In laminar co-flow DME diffusion flames, adding oxygen to the fuel stream increases the sooting tendency until a critical point is reached, at which point the trend suddenly reverses. This work unravels the mechanisms behind this reversal process, and characterizes their contribution to controlling soot production. A series of experimental measurements using diffuse-light line-of-sight attenuation and two-colour pyrometry were performed to measure soot volume fraction and soot temperature considering a fixed mass flow rate of DME and variable addition of oxygen. Soot volume fraction increases from 0.095 ppm in the pure DME flame to 0.32 ppm when the added oxygen concentration reaches 33%. When the oxygen concentration is slightly increased to 35%, soot volume fraction is reduced by 60%. To explain the reasons behind the reversal, a series of numerical simulations were performed, which successfully demonstrated the same trend. Results show that the chemical effects of adding oxygen to the fuel stream are exceedingly more important than the thermal and dilution effects. It was found that the reversal occurred when nearly all DME disassociated before exiting the fuel tube, indicating a sudden transition from a partially premixed DME flame, to one which primarily burns C1 fuel fragments. An analysis of soot formation and oxidation rates showed that near the reversal, soot inception is the least affected process; furthermore, soot precursor availability is not significantly affected in magnitude, rather they appear further upstream. It is concluded that the favourable conditions for rapid DME decomposition into soot precursors enhances soot inception while depleting the necessary species for further soot mass growth, dramatically reducing soot concentration.     

Radiation properties of soot from diffusion flames

The spectral extinction coefficients k_λ of soot from flame transmission data are obtained for small pool diffusion flames of various fuels including solid polystyrene and plexiglas; foam polystyrene and polyurethane; and liquid isooctane and toluene. Good agreement between experimental and predicted k_λ from Mie theory and soot optical properties throughout the visible and infrared ranges substantiates the general applicibility of these optical properties. On the other hand, the determination of soot sizes and volume fractions from visible range data and optical properties requires the form of the size distribution be known. The effect of using different size distributions on these soot results is evaluated by using the three-parameter distribution for the particle number density N(r) = ar^b exp (?br/r_m), with b varied to create different functional dependence on radius r. The most probable radius r_m is found to increase by about 80% as b is changed from 2 to 6, while the volume fraction changes by less than 10%. Hence, the most probable radius is rather sensitive to this functional dependence, while the volume fraction is only slightly affected.     

Numerical study of the effects of gravity on soot formation in laminar coflow methane/air diffusion flames under different air stream velocities

Numerical simulations of laminar coflow methane/air diffusion flames at atmospheric pressure and different gravity levels were conducted to gain a better understanding of the effects of gravity on soot formation by using relatively detailed gas-phase chemistry and complex thermal and transport properties coupled with a semi-empirical two-equation soot model. Thermal radiation was calculated using the discrete-ordinates method coupled with a non-grey model for the radiative properties of CO, CO₂, H₂O, and soot. Calculations were conducted for three coflow air velocities of 77.6, 30, and 5 cm/s to investigate how the coflowing air velocity affects the flame structure and soot formation at different levels of gravity. The coflow air velocity has a rather significant effect on the streamwise velocity and the fluid parcel residence time, especially at reduced gravity levels. The flame height and the visible flame height in general increase with decreasing the gravity level. The peak flame temperature decreases with decreasing either the coflow air stream velocity or the gravity level. The peak soot volume fraction of the flame at microgravity can either be greater or less than that of its normal gravity counterpart, depending on the coflow air velocity. At sufficiently high coflow air velocity, the peak soot volume fraction increases with decreasing the gravity level. When the coflow air velocity is low enough, soot formation is greatly suppressed at microgravity and extinguishment occurs in the upper portion of the flame with soot emission from the tip of the flame owing to incomplete oxidation. The numerical results provide further insights into the intimate coupling between flame size, residence time, thermal radiation, and soot formation at reduced gravity level. The importance of thermal radiation heat transfer and coflow air velocity to the flame structure and soot formation at microgravity is demonstrated for the first time.     

Effect of H-atom concentration on soot formation in premixed ethylene/air flames

Soot formation is a major challenge in the development of clean and efficient combustion systems based on hydrocarbon fuels. Fundamental understanding of the reaction mechanism leading to soot formation can be obtained by investigating the role of key reactive species such as atomic hydrogen taking part in soot formation pathways. In this study, two-dimensional laser induced incandescence (LII) measurements using λ?=?1064?nm laser have been used to measure soot volume fraction (f_V) in a series of rich ethylene (C₂H₄)/air flames, stabilized over a McKenna burner fitted with a flame stabilizing metal disc. Moreover, a comparison of UV (λ?=?283?nm), visible (λ?=?532?nm) and IR (λ?=?1064?nm) laser excited LII measurements of soot is discussed. Recently developed, femtosecond two-photon laser-induced fluorescence (fs-TPLIF) technique has been applied for obtaining spatially resolved H-atom concentration ([H]) profiles under the same flame conditions. The structure of the flames has also been determined using hydroxyl radical (OH) planar laser induced fluorescence (PLIF) imaging. The results indicate an inverse dependence of f_V on [H] for a range of C₂H₄/air rich flames up to an equivalence ratio, Φ?=?3.0. Although an absolute relationship between [H] and f_V cannot be easily derived owing to the multiple steps involving H and other intermediate species in soot formation pathways, the present study demonstrates the feasibility to couple [H] and f_V obtained using advanced optical techniques for soot formation studies.     

Characteristics of microjet methane diffusion flames

Characteristics of microjet methane diffusion flames stabilized on top of the vertically oriented, stainless-steel tubes with an inner diameter ranging from 186 to 778 μ m are investigated experimentally, theoretically and numerically. Of particular interest are the flame shape, flame length and quenching limit, as they may be related to the minimum size and power of the devices in which such flames would be used for future micro-power generation. Experimental measurements of the flame shape, flame length and quenching velocity are compared with theoretical predictions as well as detailed numerical simulations. Comparisons of the theoretical predictions with measured results show that only Roper's model can satisfactorily predict the flame height and quenching velocity of microjet methane flames. Detailed numerical simulations, using skeletal chemical kinetic mechanism, of the flames stabilized at the tip of d = 186, 324 and 529 μ m tubes are performed to investigate the flame structures and the effects of burner materials on the standoff distance near extinction limit. The computed flame shape and flame length for the d = 186 μm flame are in excellent agreement with experimental results. Numerical predictions of the flame structures strongly suggest that the flame burns in a diffusion mode near the extinction limit. The calculated OH mass fraction isopleths indicate that different tube materials have a minor effect on the standoff distance, but influence the quenching gap between the flame and the tube.     

A computational study of soot formation and flame structure of coflow laminar methane/air diffusion flames under microgravity and normal gravity

A numerical study is conducted of methane–air coflow diffusion flames at microgravity (μg) and normal gravity (1g), and comparisons are made with experimental data in the literature. The model employed uses a detailed gas phase chemical kinetic mechanism that includes PAH formation and growth, and is coupled to a sectional soot particle dynamics model. The model is able to accurately predict the trends observed experimentally with reduction of gravity without any tuning of the model for different flames. The microgravity sooting flames were found to have lower temperatures and higher volume fraction than their normal gravity counterparts. In the absence of gravity, the flame radii increase due to elimination of buoyance forces and reduction of flow velocity, which is consistent with experimental observations. Soot formation along the wings is seen to be surface growth dominated, while PAH condensation plays a more major role on centreline soot formation. Surface growth and PAH growth increase in microgravity primarily due to increases in the residence time inside the flame. The rate of increase of surface growth is more significant compared to PAH growth, which causes soot distribution to shift from the centreline of the flame to the wings in microgravity.     

The role of DME addition on the evolution of soot and soot precursors in laminar ethylene jet flames

Dimethyl ether (DME) has received considerable attention as a fuel additive to reduce the emission of particulate matter (PM) due to its low-temperature chemistry, molecularly bound oxygen atom and the absence of CC bonds. However, the effect of DME addition on the evolution of soot and particularly soot precursors is not entirely understood. This study aims to shed light on this issue by blending different proportions of DME with diffusion, E60, and partially premixed, PP12, base cases of laminar ethylene flames using the Yale benchmark burner. Laser-induced fluorescence (LIF) intensity and decay time are used to characterize the structure and evolution of soot precursors, while laser-induced incandescence (LII) is utilized to determine the soot volume fraction (SVF) and the effective primary particle diameter (D_p). For the diffusion flames, the addition of 10% DME increases the concentrations of both soot and soot precursors. With the further addition of DME to 20%, the SVF decreases to levels similar to those of E60 and then decreases further with 30% DME addition. All diffusion flames with DME addition exhibit higher concentrations of soot precursors than those of the reference E60 case. For PP12, the addition of 10% DME shows similar concentrations of soot precursors and a slight reduction in the SVF which continues to decrease with further increases in DME additions to the PP12 flame. The addition of DME seems to have little effect on the soot particle diameters for all the studied flames. Overall, the PP flames result in smaller mean particle diameters than the diffusion flame counterparts.     

Investigation of soot sensitivity to strain rate in ethylene counterflow soot formation oxidation flames

Soot sensitivity to strain rate is mainly responsible for soot formation intermittence in practical combustion devices. This work provides a fundamental study on soot formation in Soot Formation Oxidation (SFO) counterflow flames at varying strain rates. While the problem has been extensively studied in Soot Formation (SF) configurations, where the dominant process is nucleation, investigations remain scarce in the corresponding SFO cases. In the latter, the high temperatures and strong oxidative environments make the surface reactions prevail over nucleation. The work provides a new dataset for ethylene SFO flames in a wide range of strain rates and sheds light on the main processes concurring in determining soot strain rate sensitivity in such conditions. In particular, the peak of soot volume fraction (SVF) is primarily controlled by surface growth and oxidation. The latter becomes progressively more dominant on the side of the SVF distribution toward the oxidizer nozzle, where the presence of oxidizing agents is significant. The soot mechanism adopted predicts a SVF distribution and sensitivity to strain rate in agreement with experimental data. The latter is found similar to corresponding SF cases, although soot loads in the two configurations differ by almost an order magnitude, and the SVF sensitivity is known to be more accentuated for lower soot loads. A deeper investigation revealed that the nucleation process through dimerizations primarily controls the SVF sensitivity, providing the onset of soot necessary for further growth. Then, the latter tends to reduce SVF sensitivity depending on its impact. PAH sensitivities mostly agree with theoretical observation even though further validations on the kinetic mechanism are needed to improve its predictions in lean conditions. The simplistic yet effective model based on the hybrid method of moments and the employment of a reduced kinetic mechanism makes the approach amenable for turbulent computational fluid dynamic (CFD) simulations.     

Investigation of the transition from lightly sooting towards heavily sooting co-flow ethylene diffusion flames

Laminar, sooting, ethylene-fuelled, co-flow diffusion flames at atmospheric pressure have been studied experimentally and theoretically as a function of fuel dilution by inert nitrogen. The flames have been investigated experimentally using a combination of laser diagnostics and thermocouple-gas sampling probe measurements. Numerical simulations have been based on a fully coupled solution of the flow conservation equations, gas-phase species conservation equations with complex chemistry and the dynamical equations for soot spheroid growth. Predicted flame heights, temperatures and the important soot growth species, acetylene, are in good agreement with experiment. Benzene simulations are less satisfactory and are significantly under-predicted at low dilution levels of ethylene. As ethylene dilution is decreased and soot levels increase, the experimental maximum in soot moves from the flame centreline toward the wings of the flame. Simulations of the soot field show similar trends with decreasing dilution of the fuel and predicted peak soot levels are in reasonable agreement with the data. Computations are also presented for modifications to the model that include: (i) use of a more comprehensive chemical kinetics model; (ii) a revised inception model; (iii) a maximum size limit to the primary particle size; and (iv) estimates of radiative optical thickness corrections to computed flame temperatures.     

Effects of soot absorption and scattering on LII intensities in laminar coflow diffusion flames

Absorption and scattering of laser-induced incandescence (LII) intensities by soot particles present between the measurement volume and the detector were numerically investigated at detection wavelengths of 400 and 780 nm in a laminar coflow ethylene/air flame. The radiative properties of aggregated soot particles were calculated using the Rayleigh-Debye-Gans polydisperse fractal aggregate theory. The radiative transfer equation in emitting, absorbing, and scattering media was solved using the discrete-ordinates method. The radiation intensity along an arbitrary direction was obtained using the infinitely small weight technique. The effects of absorption and scattering on LII intensities are found to be significant under the conditions of this study, especially at the shorter detection wavelength and when the soot volume fraction is higher. Such a wavelength-dependent signal-trapping effect leads to a lower soot particle temperature estimated from the ratio of uncorrected LII intensities at the two detection wavelengths. The corresponding soot volume fraction derived from the absolute LII intensity technique is overestimated. The Beer-Lambert relationship can be used to describe radiation attenuation in absorbing and scattering media with good accuracy provided the effective extinction coefficient is adequately.     

Understanding soot particle size evolution in laminar ethylene/air diffusion flames using novel soot coalescence models

Two coalescence models based on different merging mechanisms are introduced. The effects of the soot coalescence process on soot particle diameter predictions are studied using a detailed sectional aerosol dynamic model. The models are applied to a laminar ethylene/air diffusion flame, and comparisons are made with experimental data to validate the models. The implementation of coalescence models significantly improves the agreement of prediction of particle diameters with the experimental data. Sensitivity of the soot prediction to the coalescence parameters is analysed. Finally, an update to the coalescence model based on experimental observations of soot particles in the flame oxidation regions has been introduced to improve its predicting capabilities.     

Soot emission reduction in oxygenated co-flow jet flames

A computational study was performed for ethylene/air non-premixed laminar co-flow jet flames using an axisymmetric CFD code to explore the effect of oxygenation on PAH and soot emissions. Oxygenated flames were established using N₂ diluted fuel stream along with O₂ enriched air stream such that the stoichiometric mixture fraction (Ζ_st) is varied but the adiabatic flame temperature is not materially changed. Simulations were carried out using a spatially and temporally accurate algorithm with detailed chemistry and transport. A detailed kinetic model involving 111 species and 784 reactions and a fairly detailed soot model were incorporated into the code. Two different approaches, one with constant flame height and other with constant inlet velocity are comprehensively examined to bring out the effects of changes in flame structure and residence time on soot emissions with respect to Z_st. With increase in Ζ_st, a drastic reduction in the formation of soot precursors (acetylene and benzene) and thus in soot emissions are observed. In the present study, oxygenated flames with Ζ_st ≥ 0.424 are considered as blue flames or completely soot free. For various oxygenated flames a C/O ratio between 0.45 and 0.6 is found to be most favorable for soot formation.     

Pressure and temperature dependence of soot in highly controlled counterflow ethylene diffusion flames

Soot volume fraction and dispersion index were measured by pyrometry in a series of highly controlled counterflow diffusion flames, with peak temperatures, T_max, spanning a few hundred degrees and pressure covering the 0.1–0.8 MPa range. An unprecedented level of control was implemented by selecting flames with a self-similar structure to ensure that the normalized temperature-time history experienced by the reactants was the same, regardless of pressure. The self-similarity was verified by suitably rescaling the transverse coordinate with respect to a characteristic diffusion length. At constant T_max, the soot volume fraction increases approximately by two orders of magnitude as the pressure is raised from 1 atm to 4 atm, and by one to two additional orders of magnitude with an additional doubling of the pressure to 8 atm. At constant pressure, the soot load spans two to three orders of magnitude and soot formation exhibits increased sensitivity to temperature as the pressure is raised. Soot inception occurs near the flame, with an increase in soot concentration that becomes steeper at higher T_max. The increase is accompanied by a decrease in the dispersion exponent that is suggestive of dehydrogenation and aging of the particles and is sharper at higher T_max. Soot experiences continuous growth in a monotonically decreasing temperature field until it is convected away radially at the stagnation plane, with essentially no opportunity for oxidation. Evidence of two distinct mechanisms for soot formation was found: the classic high temperature, high activation energy process affecting soot formed in the vicinity of the flame and followed by dehydrogenation; and a relatively low-temperature, zero activation energy process, associated with the increase in volume fraction at low-temperatures in proximity of the stagnation plane. The latter is tentatively attributed to dimerization of aromatics, as revealed by the concurrent increase in the dispersion index corresponding to an increase in the particle hydrogen content.     

Soot formation and temperature field structure in co-flow laminar methane-air diffusion flames at pressures from 10 to 60 atm

The effects of pressure on soot formation and the structure of the temperature field were studied in co-flow methane-air laminar diffusion flames over a wide pressure range, from 10 to 60 atm in a high-pressure combustion chamber. The selected fuel mass flow rate provided diffusion flames in which the soot was completely oxidized within the visible flame envelope and the flame was stable at all pressures considered. The spatially resolved soot volume fraction and soot temperature were measured by spectral soot emission as a function of pressure. The visible (luminous) flame height remained almost unchanged from 10 to 100 atm. Peak soot concentrations showed a strong dependence on pressure at relatively lower pressures; but this dependence got weaker as the pressure is increased. The maximum conversion of the fuel’s carbon to soot, 12.6%, was observed at 60 atm at approximately the mid-height of the flame. Radial temperature gradients within the flame increased with pressure and decreased with flame height above the burner rim. Higher radial temperature gradients near the burner exit at higher pressures mean that the thermal diffusion from the hot regions of the flame towards the flame centerline is enhanced. This leads to higher fuel pyrolysis rates causing accelerated soot nucleation and growth as the pressure increases.