Soot formation and temperature field structure in laminar propane-air diffusion flames at elevated pressures

The effect of pressure on soot formation and the structure of the temperature field was studied in coflow propane-air laminar diffusion flames over the pressure range of 0.1 to 0.73 MPa in a high-pressure combustion chamber. The fuel flow rate was selected so that the soot was completely oxidized within the visible flame and the flame was stable at all pressures. Spectral soot emission was used to measure radially resolved soot volume fraction and soot temperature as a function of pressure. Additional soot volume fraction measurements were made at selected heights using line-of-sight light attenuation. Soot concentration values from these two techniques agreed to within 30% and both methods exhibited similar trends in the spatial distribution of soot concentration. Maximum line-of-sight soot concentration along the flame centerline scaled with pressure; the pressure exponent was about 1.4 for pressures between 0.2 and 0.73 MPa. Peak carbon conversion to soot, defined as the percentage of fuel carbon content converted to soot, also followed a power-law dependence on pressure, where the pressure exponent was near to unity for pressures between 0.2 and 0.73 MPa. Soot temperature measurements indicated that the overall temperatures decreased with increasing pressure; however, the temperature gradients increased with increasing pressure.     

A model of particulate and species formation applied to laminar, nonpremixed flames for three aliphatic-hydrocarbon fuels

A detailed kinetic mechanism is developed that includes aromatic growth and particulate formation. The model includes reaction pathways leading to the formation of nanosized particles and their coagulation and growth to larger soot particles using a sectional approach for the particle phase. It is tested against literature data of species concentrations and particulate measurements in nonpremixed laminar flames of methane, ethylene, and butene. Reasonably good predictions of gas and particle-phase concentrations and particle sizes are obtained without any change to the kinetic scheme for the different fuels. The model predicts the low concentration of particulates in the methane flame (about 0.5 ppm) and the higher concentration of soot in the ethylene and butene flames (near 10 ppm). Model predictions show that in the methane flame small precursor particles dominate the particulate loading, whereas soot is the major component in ethylene and butene flames, in accordance with the experimental data. The driving factors in the model responsible for the quite different soot predictions in the ethylene and butene flames compared with the methane flame are benzene and acetylene concentrations, which are higher in the ethylene and butene flames. Soot loadings in the ethylene flame are sensitive to the acetylene soot growth reaction, whereas particle inception rates are linked to benzene in the model. A coagulation model is used to obtain collision efficiencies for some of the particle reactions, and tests show that the modeled results are not particularly sensitive to coagulation at the rates used in our model. Soot oxidation rates are not high enough to correctly predict burnout, and this aspect of the model needs further attention.     

Unified behaviour of maximum soot yields of methane, ethane and propane laminar diffusion flames at high pressures

Soot concentration and temperature distributions within the flame envelope of laminar diffusion flames of methane and ethane at elevated pressures were measured in a high-pressure combustion chamber. Methane measurements were made with two different fuel flow rates: 0.43 mg/s (0.32 mg/s carbon flow rate) for the pressure range of 15–60 atm, and 0.83 mg/s for the pressure range of 5–20 atm (0.62 mg/s carbon flow rate). For the ethane flames, the flow rate was 0.78 mg/s (0.62 mg/s carbon flow rate) and the pressure range was 2–15 atm. From the soot concentration distribution, soot yields were calculated as a function of flame height and pressure. Maximum soot yields from the current study and the previous measurements in similar flames with methane, ethane, and propane flames were shown to display a unified behaviour. Maximum soot yields, when scaled properly, were represented by an empirical exponential function in terms of the reduced pressure, actual pressure divided by the critical pressure of the fuel. The maximum soot yield seems to reach a plateau asymptotically as the pressure exceeds the critical pressure of the fuel.     

Measurements of sooting tendency in laminar diffusion flames of n-heptane at elevated pressure

This research focuses on the effects of an increasing pressure on the soot formation during combustion of vaporized liquid fuel. Therefore soot formation is measured in a laminar diffusion flame, with n-heptane as fuel, over a range of pressures from 1.0 to 3.0 bar. The soot volume fraction in the diffusion flames has been measured using Laser-Induced Incandescence (LII) calibrated by means of the Line Of Sight Attenuation (LOSA) technique. The values of the calibration factors between LII intensities and soot volume fraction from LOSA are slightly varied for different pressure. The integral soot volume fractions show power law dependence on pressures, being proportional to pⁿ, with n being 3.4 ± 0.3 in the pressure range of 1.0–3.0 bar.     

Laser-induced incandescence study of diesel soot formation in a rapid compression machine at elevated pressures

Simultaneous laser-induced incandescence (LII) and laser-induced scattering (LIS) were applied to investigate soot formation and distribution in a single cylinder rapid compression machine. The fuel used was a low sulfur reference diesel fuel with 0.04% volume 2-ethylhexyl nitrate. LII images were acquired at time intervals of 1 CA throughout the soot formation period, for a range of injection pressures up to 160 MPa, and in-cylinder pressures (ICP) up to 9 MPa. The data collected shows that although cycle-to-cycle variations in soot production were observed, the LII signal intensities converged to a constant value when sufficient cycles were averaged. The amount of soot produced was not significantly affected by changes in in-cylinder pressure. Soot was observed distributed in definite clusters, which were linked to slugs of fuel caused by oscillations in the injector needle. The highest injection pressure exhibited lower soot productions and more homogeneous soot distributions within the flame. Despite diffusion flames lasting longer with lower injection pressure, it appeared that the extended oxidation time was insufficient to oxidize the excess production of soot. In addition, soot particles were detected closer to the nozzle tip with higher injection pressures. The recording of LII sequences at high temporal resolutions has shown that three distinct phases in soot formation can be observed. First, high soot formation rates are observed before the establishment of the diffusion flame. Second, a reduced soot formation rate is apparent from the start of diffusion flame until the end of injection. Finally, high soot oxidation rates occur after the end of injection and for the duration of the flame.     

Experimental study of soot and temperature field structure of laminar co-flow ethylene–air diffusion flames with nitrogen dilution at elevated pressures

An experimental study has been conducted to investigate soot formation in laminar co-flow ethylene–air diffusion flames with nitrogen dilution from a co-flow circular nozzle at pressures from 10 to 35 atm. Spectral soot emission (SSE) diagnostic technique was used to determine the radially resolved soot and temperature field structure. Constancy of ethylene and nitrogen flow rates were maintained and the flow rates of ethylene and nitrogen were selected such that no smoke was emitted even at the highest soot loadings. The flame height, marked by visible flame radiation, remained constant at about 5.5 mm and the cross-sectional area of the flame decreased with increasing pressure. At 10 atm, the peak soot concentration of less than 8 ppm, was measured near the flame tip. At 35 atm, the peak soot concentration of about 62 ppm, was measured near the mid-height of the flame. The conversion of carbon in the fuel to soot was strongly dependent on pressure particularly in the lower pressure range. At higher pressure this dependence was weaker. The peak carbon conversion to soot, 6.5%, was observed at 30 atm and remained constant to 35 atm. Temperatures increased along the flame axis and the peak temperature was observed near the flame tip to indicate complete soot oxidation.     

Pressure effects on nonpremixed strained flames

This article deals with the effect of pressure on the structure and consumption rate of nonpremixed strained flames. An analysis based on the fast chemistry limit indicates that the flame thickness is inversely proportional to the square root of pressure and that the flame structure may be described in terms of a similarity variable that scales like the product of pressure and the strain rate to the power 1/2. This scaling rule also applies to flames submitted to a time-variable strain rate provided that the frequencies characterizing these changes are low compared to the mean strain rate. It is also confirmed that reactants consumption rates per unit flame surface vary like the square root of pressure and that this rule holds for time-variable strain rates of arbitrary nature. Complex chemistry calculations carried out over a broad range of operating pressures indicate that the pressure dependences deduced analytically are remarkably accurate and can be used for a broad range of strain rates, excluding values in the near vicinity of extinction conditions, where finite rate chemistry effects become important and influence the flame response to pressure. Thus, it appears that the pressure exponent characterizing the heat release rate in nonpremixed strained flames is essentially constant and equal to 1/2. This exponent is independent of finite rate chemistry effects, except when conditions are close to extinction.     

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.     

Soot surface growth and oxidation at pressures up to 8.0 atm in laminar nonpremixed and partially premixed flames

The flame structure and soot particle surface reaction properties, including growth and oxidation, of laminar jet nonpremixed flames were studied experimentally at pressures of 1.0-8.0 atm. Ethylene-helium mixtures were used in an oxygen/helium coflow at normal temperature (300 K) in order to minimize the effects of buoyancy. The following properties along the axis of flames were measured as a function of distance from the burner exit: soot concentrations by laser extinction, soot temperatures by multiline emission, soot structure by thermophoretic sampling and analysis using transmission electron microscopy (TEM), concentrations of major stable gas species by isokinetic sampling and gas chromatography, concentrations of radical species (H, OH, O) by Li/LiOH atomic absorption, and flow velocities by laser velocimetry. The measurements were analyzed to determine local flame properties in order to find soot surface growth and oxidation rates. The measurements of soot surface growth rates (corrected for soot surface oxidation) were found to be consistent with earlier measurements at atmospheric and subatmospheric pressures involving laminar premixed and diffusion flames fueled with a variety of hydrocarbons. The growth rates from all the available flames were in good agreement with each other and with existing hydrogen-abstraction/carbon-addition (HACA) soot surface growth mechanisms available in the literature. Measurements of early soot surface oxidation rates at pressures of 1.0-8.0 atm (corrected for soot surface growth and prior to consumption of 70% of the maximum mass of the primary soot particles) were found to be consistent with earlier measurements at atmospheric and subatmospheric pressures. The oxidation rates of up to 8 atm in flame environment could be explained by reaction with OH, having a collision efficiency of 0.12.     

Comparison of structures of laminar methane–oxygen and methane–air diffusion flames from atmospheric to 60 atm

A combined experimental and numerical study was conducted to examine the structure of laminar methane–oxygen diffusion flames in comparison with methane–air flames. Soot measurements made in these flames indicated that the maximum soot yields of methane–air flames are consistently higher than methane–oxygen flames at all pressures. The maximum soot yield of the methane–oxygen flames reaches a peak near 40 atm and then starts decreasing as the pressure further increased. The maximum soot yield of the methane–air flames plateaus at about 40 atm and does not change much with further increases in pressure. Methane–oxygen flames display a distinct two-zone structure which is visible from atmospheric pressure up to 60 atm. The inner zone, similar to hydrocarbon-air diffusion flames, has a yellow/orange colour and is surrounded by an outer blue zone. This outer zone was shown to have a stratified structure with a very steep equivalence ratio gradient. The main reactions in this zone were shown to be the oxidation of hydrogen and carbon monoxide produced within the inner zone. The methane–air diffusion flames had a thin layer of blue outer zone at atmospheric pressure; however, this zone completely disappeared when the pressure was increased above atmospheric. The presence of the two-zone structure in the methane–oxygen flames was attributed to the intensified penetration of oxygen into the core flow. The higher diffusivities, steeper oxygen concentration gradients, and enhanced entrainment increase the transport of oxygen to the flame. As such, there is sufficient oxygen present near the base of the flame to support the diffusion flame in the inner zone of the methane–oxygen flames. The abundance of oxygen near the centerline, even in the lower portion of the flame, also promotes the oxidation of soot.     

Hydrogen addition to acetylene-air laminar diffusion flames: Studies on soot formation under different flow arrangements

Axisymmetric co-flowing acetylene/air laminar diffusion flames have been experimentally investigated to study the effect of hydrogen addition on soot formation and soot morphology. An acetylene-hydrogen jet burning in co-flowing air at atmospheric pressure has been studied under different flow arrangements, i.e., premixed and with separate addition of acetylene and hydrogen. Thermophoretic sampling and analysis by transmission electron microscopy are employed for soot diagnostics. Soot microstructure, primary particle size, soot volume fraction, and fractal geometry results are reported. The effect of hydrogen addition on the temperature field is moderate (maximum increase ∼100 K), the effect being greater when hydrogen is premixed with acetylene. Soot volume fraction decreases with hydrogen addition. A shift was noted in the soot volume fraction peak with change in the Reynolds and Froude numbers at the burner exit. The primary soot particle diameter is in the range of 20-35 nm. Soot particles are larger in size close to the burner for the pure acetylene flame. A reverse trend is observed with hydrogen addition. The fractal dimension of the soot aggregates is about 1.7-1.8. It is unaffected by hydrogen addition and location in the flame. Soot aggregate size tends to decrease with hydrogen addition. The results of the present study on the effect of hydrogen addition on soot volume fraction and mean primary particle size are in good correlation with the results of other investigators for ethylene-, propane-, and butane-air flames, which have been described with regard to the HACA mechanism of soot nucleation and growth and enhanced soot oxidation in fuel-rich flames by increased OH radical concentration.     

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.     

A numerical study on the effects of pressure and gravity in laminar ethylene diffusion flames

The effects of pressure and gravity on sooting characteristics and flame structure were studied numerically in coflow ethylene–air laminar diffusion flames between 0.5 and 5 atm. Computations were performed by solving the unmodified and fully-coupled equations governing reactive, compressible, gaseous mixtures which include complex chemistry, detailed radiation heat transfer, and soot formation/oxidation. Soot formation/oxidation was modeled using an acetylene-based, semi-empirical model which has been verified with previously published experimental data to correctly capture many of the observed trends at normal-gravity. Calculations for each pressure considered were performed for both normal- and zero-gravity conditions to help separate the effects of pressure and buoyancy on soot formation. Based on the numerical predictions, pressure and gravity were observed to significantly influence the flames through their effects on buoyancy and reaction rates. The zero-gravity flames have higher soot concentrations, lower temperatures and broader soot-containing zones than normal-gravity flames at the same pressure. The zero-gravity flames were also found to be longer and wider. Differences were observed between the two levels of gravity when pressure was increased. The zero-gravity flames displayed a stronger dependence of the maximum soot yield on pressure from 0.5 to 2 atm and a weaker dependence from 2 to 5 atm as compared to the normal-gravity flames. In addition, flame diameter decreased with increasing pressure under normal-gravity while it increased with pressure in the zero-gravity cases. Changing the prescribed wall boundary condition from fixed-temperature to adiabatic significantly altered the numerical predictions at 5 atm. When the walls were assumed to be adiabatic, peak soot volume fractions and temperatures increased in both the zero- and normal-gravity flames, emphasizing the importance of heat conduction to the burner rim on flame structure.     

Soot formation in high pressure laminar diffusion flames

The details of the chemical and physical mechanisms of the soot formation process in combustion remain uncertain due to the highly complex nature of hydrocarbon flames, and only a few principles are firmly established mostly for atmospheric conditions. In spite of the fact that most combustion devices used for transportation operate at very high pressures (e.g., aircraft gas turbines up to 40 atm, diesel engines exceeding 100 atm), our understanding of soot formation at these pressures is not at a desirable level, and there is a fundamental lack of experimental data and complementary predictive models. The focus of this review is to assess the experimental results available from laminar co-flow diffusion flames burning at elevated pressures. First, a brief review of soot formation mechanisms in diffusion flames is presented. This is followed by an assessment of soot diagnostics techniques, both intrusive and non-intrusive, most commonly used in soot experiments including the laser induced incandescence. Then the experimental results of soot measurements done at elevated pressures in diffusion flames are reviewed and critically assessed. Soot studies in shock tubes and in premixed flames are not covered. Smoke point fuel mass flow rate is revisited, and shortcomings in recent measurements are pointed. The basic requirements for tractable and comparable measurements as a function of pressure are summarized. Most recent studies at high pressures with aliphatic gaseous fuels show that the soot yield displays a unified behaviour with reduced pressure. The maximum soot yield seems to reach a plateau asymptotically as the pressure exceeds the critical pressure of the fuel. Lack of experimental data on the sensitivity of soot morphology to pressure is emphasized. A short summary of efforts in the literature on the numerical simulation of soot formation in diffusion flames at high pressures is the last section of the paper.     

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.     

The effects of molecular structure on soot formation II. Diffusion flames

Soot thresholds, in the form of flame heights and fuel mass consumption rates at the smoke points, have been measured in atmospheric pressure, laminar diffusion flames of 42 pure hydrocarbons using a wick-fed burner. The smoke point fuel consumption rates were converted into threshold soot indices, TSIs, and compared with fuel structural parameters and with previous data from the literature. Averaged TSI values are given for 103 fuels.Soot particle emission temperatures and line-of-sight averaged soot volume fractions were measured at half the total smoke point flame heights, the location at which the soot concentration maximizes. All of the soot emission temperatures were between 1450 and 1550K, with aromatic fuels exhibiting the highest temperatures. Maximum soot volume fractions ranged from 2 to 11 × 10⁻⁶, with aromatic fuels producing the highest total soot concentrations.     

Instabilities and soot formation in high-pressure, rich, iso-octane-air explosion flames: 1. Dynamical structure

Simultaneous OH planar laser-induced fluorescence (PLIF) and Rayleigh scattering measurements have been performed on 2-bar rich iso-octane-air explosion flames obtained in the optically accessible Leeds combustion bomb. Separate shadowgraph high-speed video images have been obtained from explosion flames under similar mixture conditions. Shadowgraph images, quantitative Rayleigh images, and normalized OH concentration images have been presented for a selection of these explosion flames. Normalized experimental equilibrium OH concentrations behind the flame fronts have been compared with normalized computed equilibrium OH concentrations as a function of equivalence ratio. The ratio of superequilibrium OH concentration in the flame front to equilibrium OH concentration behind the flame front reveals the response of the flame to the thermal-diffusive instability and the resistance of the flame front to rich quenching. Burned gas temperatures have been determined from the Rayleigh scattering images in the range 1.4???1.9 and are found to be in good agreement with the corresponding predicted adiabatic flame temperatures. Soot formation was observed to occur behind deep cusps associated with large-wavelength cracks occurring in the flame front for equivalence ratio ??1.8 (C/O?0.576). The reaction time-scale for iso-octane pyrolysis to soot formation has been estimated to be approximately 7.5-10 ms.     

Effects of gravity and pressure on laminar coflow methane–air diffusion flames at pressures from 1 to 60 atmospheres

The effects of pressure and gravity on the sooting characteristics and flame structure of coflow methane–air laminar diffusion flames between 1 and 60 atm were studied numerically. Computations were performed by solving the unmodified and fully-coupled equations governing reactive, compressible flows which include complex chemistry, detailed radiation heat transfer and soot formation/oxidation. Soot formation/oxidation was modeled using an acetylene-based, semi-empirical model which was verified with previously published experimental data to correctly capture many of the observed trends at normal-gravity. Calculations for each pressure considered were performed under both normal- and zero-gravity conditions to help separate and identify the effects of pressure and buoyancy on soot formation. Based on the numerical predictions, pressure and gravity were observed to significantly influence the sooting behavior and structure of the flames through their effects on buoyancy and temperature. Zero-gravity flames generally have lower temperatures, broader soot-containing zones, and higher soot volume fractions than normal-gravity flames at the same pressure. Buoyancy forces caused the normal-gravity flames to narrow with increasing pressure while the increased soot concentrations and radiation at high pressures caused the zero-gravity flames to lengthen. Low-pressure flames at both gravity levels exhibited a similar power-law dependence of the maximum carbon conversion on pressure that weakened as pressure was increased. In the zero-gravity flames, increasing pressure beyond 20 atm caused the maximum carbon conversion factor to decrease.     

Parametric effects on sooting in turbulent acetylene diffusion flames

Optical extinction and temperature measurements have been made in free turbulent diffusion acetylene flames over a wide range of velocities and nozzle sizes. The measurements show that the soot volume profiles scale as the flame time constant. Soot formation and oxidation rates are controlled by mixing rates at low flow rates and by soot kinetics at high flow rates. The temperature in the downstream oxidizing region is the most important determinant of the flame's smoking propensity. Inert diluents greatly reduce soot formation and burnout rates and O₂ addition increases formation rates.     

Influences of elevated pressures on soot formation in coaxial ethylene–air diffusion flames under different ventilation conditions

The effect of elevated pressures on the soot formation in coaxial ethylene-diffusion flame was investigated under different ventilation conditions, i.e. one with a chamber valve closed and the other with a chamber valve open. Experimental measurements include the soot volume fraction and macroscopic flame behaviors such as visible height and flame shape. The presence of ventilation-assisted flow around the flame was found to further increase the visible flame radius and height at elevated pressures. The maximum soot volume fraction measured within the flame was also increased with the ventilation-assisted flow as well as with the ambient pressure. Experimental results clearly indicate that changes in the physical appearance of the flames altered by ventilation-assisted flow are an important factor to affect the sooting behavior in coaxial diffusion flames.