Ethylene Diffusion Flames Research Articles

Effects of Oxygen Concentration on Soot Formation in Ethylene and Ethane Fuel Laminar Diffusion Flames

In studying the effects of oxygen concentration and molecular structure on the morphologies of the soot particles produced by hydrocarbon fuels, ethylene and ethane were chosen as experimental fuels. With a Gülde laminar coaxial diffusion flame device, a soot particle device was used to sample soot particles at different oxygen concentrations (21%, 24%, 26%, 28%, and 31%) and at different heights above a burner (HABs = 10 mm, 20 mm, 30 mm, 40 mm, and 50 mm). High-resolution transmission electron microscopy (HRTEM) was used to scrutinize and analyze the soot particles at varying oxygen concentrations. The findings suggest that at the same oxygen concentration, ethylene produces brighter and taller flames. With an increase in the oxygen concentration, ethylene flames and ethane flames gradually decrease in height and become brighter. With an increase in the HAB, the average primary soot particle diameter (Dp) increases initially and then decreases, the fractal dimension (Df) increases, and the aggregates transition from strips and chains to clusters. At the same flame height (HAB = 30 mm), the Dp decreases, the Df increases, the carbon layer torsion resistance (Tf) and the carbon layer spacing (Ds) increase, and the carbon layer changes from a parallel arrangement to a curved arrangement to form denser network aggregations.

Effect of H2/CO addition on soot formation in ethylene diffusion flame

Coupling the San Diego gas phase reaction mechanism and the Moss Brookes soot model using FLUENT14.0 software, the effect of adding H2/CO on the fuel side on soot formation in an ethylene/air laminar diffusion flame was studied. A specific analysis was conducted on the effects of H2, CO and its chemical effects on flame temperature, soot volume fraction, mole fractions of important intermediate products OH, H, and C2H2, as well as rate of soot mass nucleation, surface growth, and oxidation. In the numerical calculation, the virtual substances FH2 and FCO are set to separate the chemical effect of H2 and CO and to analyze the chemical effect of adding H2 and CO on soot formation. The results show that the flame temperature increases slightly, and the soot volume fraction decreases monotonically with adding H2 and CO. The chemical effect of H2 increases the temperature, the mole fraction of C2H2 and H, the soot nucleation rate, and the surface growth rate, and finally, it promotes soot formation. The chemical effect of CO increases the temperature and H mole fraction, reduces the OH mole fraction, and then increases the soot surface growth rate and reduces the soot oxidation rate. The higher soot nucleation, surface growth rate, and lower oxidation rate jointly promote soot formation.

Physical and Chemical Effects of Ammonia on Gas Emissions and Soot Formation in Laminar Coflow Ethylene Diffusion Flames

Physical and Chemical Effects of Ammonia on Gas Emissions and Soot Formation in Laminar Coflow Ethylene Diffusion Flames

The kinetics and warm flame chemistry associated with radiative extinction of spherical diffusion flames

Several studies have found that microgravity diffusion flames with sufficient heat loss cool until they extinguish at a critical temperature near 1130 K. In this work, the associated chemical kinetics are explored for spherical diffusion flames burning ethylene. The flames are simulated with a transient numerical model with detailed chemistry, transport, and radiation. This incorporates the UCSD mechanism with 57 species and 270 reactions. Species concentrations, reaction rates, and heat release rates are examined. Upon ignition, the peak temperature is above 2000 K, but this decreases until extinction due to radiative losses. This allows the chemistry to be studied over a wide range of peak temperatures for the same fuel and oxidiser. When the peak temperature is high, the dominant chemistry is similar to that for typical normal-gravity ethylene diffusion flames. There are two distinct zones: an ethylene pyrolysis zone and an oxidation zone, and negligible reactant leakage. The ethylene mainly reacts with H and OH. The concentration of OH in the ethylene pyrolysis zone is high due to the long residence times and reactions of CO2 and H2O with H. As the flame cools and the peak temperature approaches the critical extinction temperature, there is increased reactant leakage leading to higher O, OH, and HO2 concentrations on the fuel side. Most reactions shift towards the oxidiser side and there is large overlap between the two zones. Reactions involving HO2 become more significant and the large consumption rates of H by HO2 increase the concentrations of OH and O on the fuel side. The appearance of warm flame chemistry delays extinction but is not sufficiently exothermic to prevent it.

A numerical study of NOX and soot emissions in ethylene-ammonia diffusion flames with oxygen enrichment

Blending ammonia with hydrocarbon fuels is gaining interest due to its potential to significantly reduce carbon emissions from the combustion of these blends. Additionally, studies have provided strong evidence of oxygen enhanced combustion to reduce soot emissions and improve flame stability. The present work attempts to leverage the benefits of both strategies, ammonia doping and oxygen enhanced combustion, by considering ethylene diffusion flames. Simulations are performed using the CHEMKIN-Pro software. A reaction mechanism with 372 species and 13,847 reactions is developed by combining gas phase chemistries for ethylene, NH3 and NOX, along with a detailed soot mode. The mechanism is extensively validated for a range of fuel blends in terms of flame structure, intermediate hydrocarbons, soot precursors and soot. Oxygen enrichment is achieved by removing certain amount of nitrogen from oxidizer stream and adding it to fuel stream, and thereby maintaining a nearly constant flame temperature. Extensive analysis is carried out to characterize the chemical and dilution effects of ammonia doping on flame structure, soot precursors, soot, and NOX in ethylene flames with varying levels of oxygenation. Further, dominant reaction pathways for several soot precursors and NOx are identified through detailed rate of production analyses. Results indicate that ammonia doping in ethylene flames leads to substantial increase in NOX emissions, while oxygenation has negligible influence on NOX emissions. In contrast, both NH3 doping and oxygenation provide significant reduction in the formation of soot precursors and soot. Oxygenation achieves this reduction through both hydrodynamic and flame structure effects, as the flame shifts from oxidizer side to fuel side. On the other hand, NH3 doping reduces the rates of important reactions for the formation of soot precursors, as the concentrations of relevant species (C2H2, C3H3, C3H3-P, C3H3-A etc.) decrease due to their consumption through reactions with species like NCO and CN formed from NH3. Moreover, the effectiveness of NH3 doping is further enhanced when combined with oxygenation. Hence, NH3 doping and oxygenation are found to be effective and synergistic strategies in reducing soot emissions, and their proper combination could provide near zero soot emissions.

Effect of ammonia addition on nanostructure of soot in laminar coflow diffusion flames of ethylene diluted with nitrogen

The effect of ammonia addition on the nanostructure of soot particles was studied experimentally for ethylene diffusion flames. To compensate the thermal effect and nitrogen-containing species production when ammonia was added, the total mole fraction of ammonia and nitrogen was fixed in the fuel stream. Soot particle size, fringe length, and fringe tortuosity were measured through transmission electron microscopy (TEM) and high-resolution transmission electron microscopy (HRTEM). A complementary X-ray photoelectron spectroscopy (XPS) analysis provided information about the chemical bonding of soot. A significant delay in soot growth was observed and the particle size increased with the addition of ammonia. While there was no obvious correlation between the fractal dimension of soot and ammonia mole fraction (XNH3) or sampling location. With the addition of ammonia, the mean fringe length increased reasonably linearly with XNH3 and the fringe tortuosity increased up to XNH3 ≈ 0.17 and then decreased with XNH3, which suggested that ammonia addition led to higher graphitization and lower oxidative activity. The soot from ammonia diluted flame exhibited lower reactivity, implying the delay of soot surface growth. With the addition of ammonia, the value of sp2/sp3 (indication of the graphitization degree of soot particles) did not change much for XNH3 from 0 to 0.17 then increased significantly, which indicated the degree of graphitization of soot particles significantly increased with ammonia addition. The intensity of the N1s peak (indication of the N-containing species in soot) increased with the addition of ammonia. This study confirmed that the addition of NH3 promotes the graphitization of soot.

An easy but quantitative assessment of soot production rate and its dependence on temperature and pressure

The challenge of soot emission persists in combustion research due to the complexities of tracking the crucial stages of growth from fuel to soot nuclei and ultimately mature particles. Studying soot formation in flames often requires a sophisticated approach, involving detailed measurements of gaseous soot precursors and soot particles using multiple complementary diagnostics. On the other end of the spectrum of studies are simpler methods that capture the sooting tendency using a single index, akin to the cetane number in compression ignition engines and the octane number in spark ignition engines. This article seeks a middle ground, aiming to quantify the soot production rate while maintaining the simplicity of single-index characterizations. The approach involves establishing counterflow diffusion flames, measuring soot volume fraction through pyrometry, and accurately computing velocity and temperature profiles using a commercial code. These data allow for the quantification of the production rate from the soot governing equation. The methodology is applied to counterflow ethylene diffusion flames to examine the temperature dependence of the soot production rate across peak temperatures varying by several hundred degrees and pressures in the 1–32 atm range. The soot production rate per unit flame area falls within the range of 10−7–10−3 g/(cm2s) range and, when normalized with respect to the carbon flux, it ranges between 10−6 and nearly 10−2. On a logarithmic scale, it linearly correlates with the peak temperature at a fixed pressure. Although this study deals only with flames of ethylene, the approach can be generalized to any fuel. The resulting database should be valuable not only for industry practitioners but also to the scientific community for the global validation of detailed soot models.

Coupled interactive effects of ammonia and hydrogen additions on ethylene diffusion flames: A detailed kinetic study

Coupled interactive effects of ammonia and hydrogen additions on ethylene diffusion flames: A detailed kinetic study

The effect of ammonia on soot formation in ethylene diffusion flames

The effect of ammonia on soot formation in ethylene diffusion flames

On the mechanisms affecting soot production in oxygen-depleted buoyant flames

The objective of this article is to apply a detailed polycyclic aromatic hydrocarbons (PAH)-based soot production model to investigate the effects of oxygen depletion on the overall soot production processes in laminar coflow ethylene diffusion flames. This task is accomplished by simulating the flames, studied experimentally by Sun et al. (Combust. Flame 211:96–111, 2020), burning under oxygen concentration in the oxidizer down to 16.8% and characterized by a constant volumetric stoichiometric air to fuel ratio to keep the residence time unchanged. This configuration allows isolating the effects of reducing oxygen on both soot formation and oxidation processes and avoiding the complex interactions between soot production and turbulence. Model predictions are in reasonable agreement with the experiments in terms of temperature, soot volume fraction, and primary particle diameter and capture quantitatively the effects of oxygen depletion on soot production. In all the flames, both the H-abstraction and acetylene addition (HACA) and PAH condensation contribute significantly to the soot mass growth, with the HACA slightly dominating the overall process. Reducing the oxygen concentration affects similarly all the formation and oxidation processes with a reduction in the range 30–40% from 21.0% to 18.9% and in the range from 60 to 70% as it is further reduced to 16.8%. Among the formation processes, the PAH condensation and surface growth by HACA have a similar sensitivity to oxygen depletion, followed by soot inception.

Effect of N2 Diluent on Soot Formation Characteristics in Ethylene Diffusion Flames

Effect of N2 Diluent on Soot Formation Characteristics in Ethylene Diffusion Flames

Skeletal kinetic mechanism for predicting formation of non-fuel hydrocarbons and soot in ethylene flames – A CFD approach

Since existing reduced mechanisms of ethylene oxidation are either too large or lack of sufficient chemical reactions to describe aromatics formation, the study aims at developing a skeletal mechanism with extended predictive capability and lowered computational cost in computational fluid dynamics modeling of ethylene combustion. The newly assembled and refined kinetic mechanism composed of 664 species and 3582 reactions is minimized to 79 species and 538 reactions without empirically adjusting kinetic parameters. In the 1-D simulation for a premixed flame of ethylene, the ethylene-PAH mechanism generally well predicts experimental profiles of five hydrocarbons and nine aromatics. Integrated into a 2-D axisymmetric laminar finite-rate model, the ethylene-PAH mechanism reproduces experimental data of seven C2–C5 hydrocarbons, five aromatic hydrocarbons and soot in a diffusion flame of ethylene. In comparison with the 158-species (Narayanaswamy) mechanism, the newly proposed ethylene mechanism leads to a speedup of approximately 5.5 times in the 2-D laminar diffusion flame simulation and improved accuracy for predicting species formation in both premixed and nonpremixed flames. Moreover, we unveil the correlation between reaction pathways and intermediate formation from ethylene oxidation at the low temperature regime.

Effect of NH3 addition on soot morphology and nanostructure evolution in laminar ethylene diffusion flame

Ammonia, as a carbon neutral alternative fuel, has attracted wide attention. However, due to the defects in the combustion performance of pure ammonia, it is still necessary to further solve this problem in practical utilization. The purpose of this paper is to study the influence of ammonia on the morphology of soot and the evolution of nanoparticle structure in laminar flame of ethylene. In this work, the soot collected by thermophoresis probe was observed by the high resolution transmission electron microscope (HRTEM), and the image information in HRTEM images was statistically processed, and the graphitization degree of soot was measured by X-ray diffraction (XRD) spectrum of soot samples. The experimental results show that the addition of ammonia can inhibit the growth of soot nuclei and delay the formation of incipient soot, and has different effects on the evolution of soot morphology and structure in ethylene flame. It is noteworthy that the soot samples collected in the upstream part of the ammonia-doped flame show more mature core–shell structure in HRTEM images and more graphitized XRD diffraction data than those collected in pure ethylene flame. The main reason may be the chemical effect of ammonia and the thermal effect caused by the reduction of flame radiation loss, which have different effects on the nanostructure and morphology of soot at different stages of soot formation. Fringe structure model is used to describe and explain the influence of soot in flame with height before and after ammonia doped.

Experimental study on soot formation and primary particle size in oxy-combustion ethylene diffusion flames under CO2 substitution for N2

This paper reports an experimental study on the effects of O2 concentration and CO2 concentration on soot volume fraction and primary particle size of flame centre in ethylene laminar co-diffusion flame. The incandescent light was induced by a two-color band method and laser-excited by wavelength 1064 nm. Previous studies have shown that the oxygen concentration affects the soot volume fraction in the flame. However, the effects of O2 concentration on the primary particle size under CO2 atmosphere are unclear and need to be further discussed. Seven flames were optically detected, in which the oxygen concentration of the accompanying gas varied from 21% to 50% by volume. One primary flame was burned in co-flowing ethylene/air. Six ethylene flames were burned in an oxygen-rich O2/N2 or O2/CO2 atmosphere with an oxygen mole fraction from 30% to 50%. The C2H4 flow rate remained constant in all operating conditions. The results show that the SVF observed by the LII method and spectroscopy in the oxygen-enriched flame are in good agreement. Furthermore, the soot's primary particle diameter measured by the time-resolved LII method is in good agreement with the transmission electron microscope image analysis.With the increase of oxygen concentration, the flame height becomes shorter, the luminosity becomes brighter, and the soot yield increases. Compared with an N2 atmosphere with the same oxygen concentration, the soot yield in a CO2 atmosphere was significantly inhibited. In all the flames studied, the SVF along the flame axis showed a similar distribution: it first increased to the maximum value and then decreased rapidly until the flame tip. The maximum SVF on the axis appears between 0.64 and 0.78 based on the normalized height of the visible flame. In all ethylene/(O2/N2) flames, the maximum primary particle diameter and average primary particle diameter increase with oxygen content. For ethylene/(O2/CO2) flame, the maximum diameter of primary particles decreases with the increased oxygen content. The uncertainty of primary diameter is mainly caused by the thermal adaptation coefficient, the lower LII signal of smaller particles and the uncertainty of local flame temperature.

Evaluation of the chemical effect of carbon dioxide dilution to fuel on soot formation in co-flow laminar ethylene and propane diffusion flames

In this study, the effects of carbon dioxide (CO2) addition on soot evolution were isolated systematically by adding 50% N2, 31% Ar+19% CO2, and 50% CO2 to the fuel side, respectively. Two series of diffusion flames, ethylene and propane, were experimentally investigated. Optical diagnostics, including laser-induced fluorescence (LIF), ratio pyrometry, and laser-induced incandescence (LII), were utilized to measure the spatial distributions of polycyclic aromatic hydrocarbons (PAHs), flame temperature, soot volume fraction fv, primary particle size dp, and number density of soot np. It was found that the flame height decreased gradually for the ethylene flame with adding N2/Ar + CO2/CO2. In contrast, the flame height remained essentially unchanged for propane-based flames. The results showed that adding N2/Ar + CO2/CO2 increased the temperature in the upper part of the ethylene flame, while the temperature change in the upper part of the propane flame was subtle and almost negligible. The total PAHs-LIF loading and the spatial distributions of fv/dp/np indicated that the chemical effect of CO2 added to ethylene flames in inhibiting the formation of large-size PAHs and retarding the soot inception stage was insignificant. However, it was not negligible for propane flames. The quantitative results revealed that the inhibition of total soot loading ST in propane flames was dominated by the chemical effect of CO2, while in ethylene flames, it was dominated by the thermal and dilution effect of CO2. The same conclusion was also found in the results of the maximum carbon conversion factor ηmax and the average particle size of soot. The specific growth rate of soot mass was almost unchanged regardless of the mixture on the fuel side. Adding CO2 had a more substantial chemical effect in inhibiting soot formation in propane flames than that in ethylene flames, which could mainly be attributed to a more effective reduction in the time for the increase of soot mass τg during soot evolution.

Effect of ammonia on the soot surface characteristics in ammonia/ethylene co-flow diffusion flames

As a carbon free and hydrogen rich fuel, ammonia is attracting more and more attention. The co-combustion of ammonia and hydrocarbon fuel can improve the combustion characteristics of ammonia and reduce CO2 emissions, and the influence of co-combustion of ammonia and hydrocarbon fuel on reducing soot emission characteristics has also aroused people's interest. In this study, the laminar co-flow ethylene diffusion flame with different ammonia addition ratios (0 %, 10 %, 20 %, and 30 %) was studied and the soot surface functional groups and graphitization structure characteristics were explored by Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) respectively. The results showed that ammonia accelerated the soot graphitization process, improved the degree of graphitization, and increased the content of oxygen containing functional groups on the surface of soot particles. The XPS N1s analysis showed that, a certain amount of nitrogen-containing functional groups can be detected in ammonia/ethylene co-flow diffusion flames. The N-Ox content increased with the increase of ammonia ratio when the NHAB was>0.7. The N-5 content decreased linearly along the flame height for different the NH3 ratios, and the transforms between N-5, N-6 and N-Q were observed with the soot formation, growth and oxidation.

Study on effects of NH3 and/or H2 addition on the characteristics of soot formation and gas emissions in a laminar ethylene diffusion flame

The effects of NH3 and/or H2 addition on the soot formation and gas emission in a laminar ethylene diffusion flame were investigated with laser diagnosis methods, thermophoretic sampling method and a Fourier Transform infrared device in this work. The flame doped with N2 was also studied to evaluate dilution effect. The soot, polycyclic aromatic hydrocarbon (PAH), OH evolutions with flame height and the gas emission were obtained. The flame temperature was simulated to identify the thermal effect, and found the temperature rise of H2 enriched flame is slightly larger than that of the flame with NH3 by <50 K. This indicates the temperature does not dominate the soot evolution. NH3 addition can obviously suppress PAH and soot formation by both dilutive and chemical effects, and the rich soot region moves from the two wings to the flame centerline with flame height increases. However, H2 addition chemically promotes soot formation. The soot formation of flames with NH3-H2 blends is between the flames doped with pure NH3 and H2. Adding the blends with low ratio NH3 and high ratio H2 can achieve dramatic soot reduction and moderate NOx emission. This result is significant for guiding future utilization of carbon-free fuel.

Effects of mechanically-induced oscillations on soot formation and flame temperature in laminar diffusion flames of ethylene

An experimental study was performed to measure the effects of flame oscillations on soot concentration and flame temperature in co-flow laminar diffusion flames of ethylene. One novel aspect of this study is that flame oscillations were mechanically induced by moving the burner assembly in a reciprocating motion with an industrial computer-controlled linear stage. Motor speed was used to control the oscillation frequency. The peak-to-peak oscillation amplitude was defined as stroke, which was then used to calculate the Strouhal number. Oscillation frequencies of 5‒20 Hz and peak-to-peak amplitudes of 0.5‒3 mm were studied. At 1 mm peak-to-peak oscillation amplitude, flame oscillations switched from tip flickering type to tip-clipping type oscillations above 10 Hz. Time-averaged soot concentration increased from its value in the steady-state flame when the flame was perturbed by small oscillation frequencies and amplitudes but then decreased as the oscillation intensity was increased. The peak time-averaged soot volume fraction was 9.5 ppm in the steady-state flame and 4.5 ppm at a peak-to-peak oscillation amplitude and an oscillation frequency of 1 mm and 20 Hz, respectively. Similarly, the peak soot volume fraction was 5.8 ppm at a peak-to-peak oscillation amplitude and an oscillation frequency of 3 mm and 10 Hz, respectively. The time-averaged flame temperatures were in the range of 1500‒2000 K. The low-temperature zone was observed at the flame core in the steady-state flame and for low-intensity oscillations, and at the flame tip for high-intensity oscillations. The literature has discrepancies on how flame oscillations affect the total soot loading in ethylene flames. Our results show that the total soot loading increased by about 10% from steady-state to low-intensity oscillations, then slightly decreased as either oscillation frequency or amplitude was increased. The effects of increasing the oscillation frequency or amplitude were similar and well captured by the revised Strouhal number.

Effect of maturity on soot volume fraction measurements using the AC-LII technique in a laminar coflow ethylene diffusion flame

The auto-compensating laser-induced incandescence (AC-LII) technique has been frequently used to measure soot volume fraction (fv) in flames. AC-LII relies on an assumption about the spectral variation of soot absorption function E(m,λ) at the two detection wavelengths for soot temperature determination. It has been a common practice to assume a constant E(m,λ) based on the believe that LII measures mature soot only. Since soot maturity in flames is a continuous phenomenon from young to mature, it is unclear how soot maturity affects the AC-LII measured fv. In this study, a correction to the AC-LII measured fv with the conventional hypothesis of mature soot is proposed based on the soot maturity coefficient β and absorption function E(m,λ) in a laminar coflow ethylene diffusion flame. The application of this correction is first demonstrated for synthetic time-resolved LII signals based on the spatial distribution of soot properties in the ethylene diffusion flame predicted by the CoFlame code. A significant decrease of the simulated incandescence signals SLII and soot temperature Teff is observed when the maturity coefficient is increased from 0 for fully mature soot to 1.2 for highly immature soot. Then the proposed correction is applied to AC-LII measured fv in the same flame with the help of spatial distributions of β and ratio of spectrally-resolved E(m,λ) by multiwavelength line-of-sight attenuation and emission (MW-LOSA/EMI) measurements. The uncorrected AC-LII measured fv is in general significantly lower than that measured by MW-LOSA/EMI, which inherently considers soot maturity. The corrected AC-LII fv results are in good agreement, within the experimental error, with those measured by MW-LOSA/EMI. Therefore, the proposed methodology can quantify the effect of soot maturity on AC-LII measured fv and largely eliminate the difference in the measurements of fv by AC-LII and MW-LOSA/EMI.

Effects of blending methane, propane, and propylene on soot evolution in ethylene diffusion flames based on optical diagnostics

Soot evolution of the ethylene-based laminar coflow diffusion flame doping with methane, propane, and propylene with the blending ratio ranging from 0 to 50% has been investigated experimentally. These fuels were selected for their different fuel structure. Spatially resolved distribution maps of the flame temperature, soot volume fraction, the fluorescence signals of polycyclic aromatic hydrocarbons (PAHs), and primary soot particle diameter and number density were determined utilizing laser-induced incandescence (LII), laser-induced fluorescence (LIF), and ratio pyrometry (RP). It was found that the flame height surged and the flame temperature dropped dramatically when the propylene blending ratio was 20% while they were almost constant with the increasing addition of methane or propane. The soot/PAHs loading decreased monotonically with the addition of methane and the opposite was true in the cases of blending propylene. The synergistic effect of mixing propane into ethylene was found on both the soot/PAHs loading. The same trends were observed in the percentage of carbon conversion to soot and the primary soot particle diameter. It can be seen from the soot evolution analysis that methane addition suppressed the soot nucleation and surface growth simultaneously. The enhanced soot surface growth for the flames doping with propane at a low addition level and for the whole flame sets doping with propylene were attributed to the earlier inception time and the longer mass growth time. The preferential diffusion and weakened oxidation of soot particles because of the decreased flame temperature perhaps accounted for the transition from a non-smoking flame to a smoking flame when the propylene blending ratio was greater than 40%.