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1.
A combined computational and experimental investigation that examines the relationship of soot formation and NO in coflow ethylene air diffusion flames is presented. While both NO and soot formation are often studied independently, there is a need to understand their coupled relationship as a function of system parameters such as fuel type, temperature and pressure. The temperature decrease due to radiative losses in systems in which significant soot is produced can affect flame length and other temperature-dependent processes such as the formation of NO. The results of a computational model that includes a sectional representation for soot formation with a radiation model are compared against laser-induced fluorescence measurements of NO. The sooting characteristics of these flames have been studied previously. Experimentally, a laser near 225.8 nm is used to excite the γ(0, 0) band in NO. Spectrally resolved fluorescence emission is imaged radially, for the (0, 0), (0, 1), (0, 2), (0, 3), and (0, 4) vibrational bands, at varying axial heights to create a two-dimensional image of NO fluorescence. A reverse quenching correction is applied to the computational results to determine an expected fluorescence signal for comparison with experimental results. Modeling results confirm that Fenimore NO is the dominant mechanism for NO production and suggest that for lightly sooting flames (peak soot volume fraction < 0.5 ppm), soot reduces only the Zeldovich NO formation (by a factor of two). For flames with increased soot levels (peak soot volume fraction ∼ 4 ppm), the model indicates not only that Zeldovich NO decreases by a factor of 2.5 through radiation loss, but that non-Zeldovich NO is reduced in the top center of the flame by about 30% through the oxidation of soot.  相似文献   

2.
This paper describes the unusual sooting structure of three flames established by the laminar recirculation zones of a centerbody burner. The vertically mounted burner consists of an annular air jet and a central fuel jet separated by a bluff-body. The three ethylene fueled flames are identified as: fully sooting, donut-shape, and ring-shape sooting flames. Different shapes of the soot structures are obtained by varying the N2 dilution in the fuel and air jets while maintaining a constant air and fuel velocity of 1.2 m/s. All three flames have the unusual characteristic that the soot, entrained into the recirculation zone, follows discrete spiral trajectories that terminate at the center of the vortex. The questions are what cause: (1) the unusual sooting structures and (2) the spiral trajectories of the soot? Flame photographs, laser sheet visualizations, and calculations with a 2D CFD-based code (UNICORN) are used to answer these questions. The different sooting structures are related to the spiral transport of the soot, the spatial location of the stoichiometric flame surface with respect to the vortex center, and the burnout of the soot particles. Computations indicate that the spiral trajectories of the soot particles are due to thermophoresis.  相似文献   

3.
This study integrates new and existing numerical modeling and experimental observations to provide a consistent explanation to observations pertaining flame length and soot volume fractions for laminar diffusion flames. Integration has been attempted by means of scaling analysis. Emphasis has been given to boundary layer flames. For the experiments, ethylene is injected through a flat porous burner into an oxidizer flowing parallel to the burner surface. The oxidizer is a mixture of oxygen and nitrogen, flowing at various velocities. All experiments were conducted in microgravity to minimize the role of buoyancy in distorting the aerodynamics of the flames. A previous numerical study emphasizing fuel transport was extended to include the oxidizer flow. Fictitious tracer particles were used to establish the conditions in which fuel and oxidizer interact. This allowed establishing regions of soot formation and oxidation as well as relevant characteristic length and time scales. Adequate scaling parameters then allow to establish explanations that are consistent for different burner configurations as well as “open-tip” and “closed-tip” flames.  相似文献   

4.
Modelling of aromatics and soot formation from large fuel molecules   总被引:2,自引:0,他引:2  
There is a need for prediction models of soot particles and polycyclic aromatic hydrocarbons (PAHs) formation in parametric conditions prevailing in automotive engines: large fuel molecules and high pressure. A detailed kinetic mechanism able to predict the formation of benzene and PAHs up to four rings from C2 fuels, recently complemented by consumption reactions of decane, was extended in this work to heptane and iso-octane oxidation. Species concentrations measured in rich, premixed flat flames and in a jet stirred reactor (JSR) were used to check the ability of the mechanism to accurately predict the formation of C2 and C3 intermediates and benzene at pressures ranging from 0.1 to 2.0 MPa. Pathways analyses show that propargyl recombination is the only significant route to benzene in rich heptane and iso-octane flames. When included as the first step of a soot particle formation model, the gas-phase kinetic mechanism predicts very accurately the final soot volume fraction measured in a rich decane flame at 0.1 MPa and in rich ethylene flames at 1.0 and 2.0 MPa.  相似文献   

5.
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.  相似文献   

6.
Experiments were conducted on a laminar premixed ethylene-air flame at equivalence ratios of 2.34 and 2.64. Comparisons were made between flames with 5% NO2 added by volume. Soot volume fraction was measured using light extinction and light scattering and fluorescence measurements were also obtained to provide added insight into the soot formation process. The flame temperature profiles in these flames were measured using a spectral line reversal technique in the non-sooting region, while two-color pyrometry was used in the sooting region. Chemical kinetics modeling using the PREMIX 1-D laminar flame code was used to understand the chemical role of the NO2 in the soot formation process. The modeling used kinetic mechanisms available in the literature. Experimental results indicated a reduction in the soot volume fraction in the flame with NO2 added and a delay in the onset of soot as a function of height above the burner. In addition, fluorescence signals—often argued to be an indicator of PAH—were observed to be lower near the burner surface for the flames with NO2 added as compared to the baseline flames. These trends were captured using a chemical kinetics model that was used to simulate the flame prior to soot inception. The reduction in soot is attributed to a decrease in the H-atom concentration induced by the reaction with NO2 and a subsequent reduction in acetylene in the pre-soot inception region.  相似文献   

7.
In this study, the influence of pressure and fuel dilution on the structure and geometry of coflow laminar methane–air diffusion flames is examined. A series of methane-fuelled, nitrogen-diluted flames has been investigated both computationally and experimentally, with pressure ranging from 1.0 to 2.7 atm and CH4 mole fraction ranging from 0.50 to 0.65. Computationally, the MC-Smooth vorticity–velocity formulation was employed to describe the reactive gaseous mixture, and soot evolution was modelled by sectional aerosol equations. The governing equations and boundary conditions were discretised on a two-dimensional computational domain by finite differences, and the resulting set of fully coupled, strongly nonlinear equations was solved simultaneously at all points using a damped, modified Newton's method. Experimentally, chemiluminescence measurements of CH* were taken to determine its relative concentration profile and the structure of the flame front. A thin-filament ratio pyrometry method using a colour digital camera was employed to determine the temperature profiles of the non-sooty, atmospheric pressure flames, while soot volume fraction was quantified, after evaluation of soot temperature, through an absolute light calibration using a thermocouple. For a broad spectrum of flames in atmospheric and elevated pressures, the computed and measured flame quantities were examined to characterise the influence of pressure and fuel dilution, and the major conclusions were as follows: (1) maximum temperature increases with increasing pressure or CH4 concentration; (2) lift-off height decreases significantly with increasing pressure, modified flame length is roughly independent of pressure, and flame radius decreases with pressure approximately as P?1/2; and (3) pressure and fuel stream dilution significantly affect the spatial distribution and the peak value of the soot volume fraction.  相似文献   

8.
Soot formation is compared in turbulent diffusion flames burning a commercial Diesel and two Diesel surrogates containing n-decane and α-methylnaphthalene. A burner equipped with a high-efficiency atomisation system has been specially designed and allows the stabilisation of liquid fuels flames with similar hydrodynamics conditions. The initial surrogate composition (70% n-decane, 30% α-methylnaphthalene) was previously used in the literature to simulate combustion in Diesel engines. In this work, a direct comparison of Diesel and surrogates soot tendencies is undertaken and relies on soot and fluorescent species mappings obtained respectively by Laser-Induced Incandescence (LII) at 1064 nm and Laser-Induced Fluorescence at 532 nm. LIF was assigned to soot precursors and mainly to high-number ring Polycyclic Aromatic Hydrocarbons (PAH). The initial surrogate was found to form 40% more soot than the tested Diesel. Consequently, a second surrogate containing a lower α-methylnaphthalene concentration (20%) has been formulated. That composition which presents a Threshold Soot Index (TSI) very close to Diesel one is also consistent with our Diesel composition that indicates a relatively low PAH content. The spatially resolved measurements of soot and fluorescent soot precursors are quite identical (in shape and intensity) in the Diesel and in the second surrogate flames. Furthermore the concordance of the LII temporal decays suggests that a similar growth of the primary soot particles has occurred for Diesel and surrogates. In addition, the comparison of the LII fluence curves indicates that physical/optical properties of soot contained in the different flames might be similar. The chemical composition present at the surface of soot particles collected in Diesel and surrogate flames has been obtained by laser-desorption ionisation time-of-flight mass spectrometry. An important difference is found between Diesel and surrogate samples indicating the influence of the fuel composition on soot content.  相似文献   

9.
Soot volume fraction and dispersion index were measured by pyrometry in a series of highly controlled counterflow diffusion flames, with peak temperatures, Tmax, 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 Tmax, 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 Tmax. 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 Tmax. 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.  相似文献   

10.
We investigate the effect of pressure on both flame structure and soot formation in nitrogen diluted counterflow diffusion flames of ethylene in the 8–32atm pressure range. Capillary-probe gas sampling is performed to resolve spatially the profiles of gaseous species up to three-ring aromatics by GC/MS analysis and multi-color pyrometry is used to quantify the soot volume fraction and dispersion exponent. Self-similarity of flames is preserved by keeping constant mixture fraction and strain rate, so that profiles of concentrations and temperature, normalized with respect to their peak values, are unaffected by changes in pressure, once the axial coordinate is nondimensionalized with respect to the pressure-dependent diffusion length scale. When conditions are chosen so that the overall soot loading is approximately constant and compatible with the diagnostics, it is found that both the soot volume fraction and the profiles of key aromatics in the high-temperature nucleation region are virtually invariant. For it to happen, a twofold increase in pressure must be compensated by a ~100 K decrease in peak flame temperature and, therefore, in the temperature across the soot forming region. The implication is that from the perspective of the chemical kinetics of soot formation these two actions counterbalance each other. As pressure increases (and temperature decreases) the peak production rate of the high-temperature soot mechanism decreases and, further downstream, towards the particle stagnation plane, a low-temperature soot mechanism sets in, yielding an increase in soot H/C content. This mechanism is enhanced as the pressure is raised, causing a higher overall soot volume production rate in the 16atm flame and, especially, in the 32atm one. The role of C4/C2 species in the formation of C6H6 increases with increasing pressure and dominates over the recombination of propargyl radical at sufficiently high pressures. A comprehensive database is established for soot models at high pressures of relevance to applications.  相似文献   

11.
Experimental data and modelling results of the main products and intermediates from a fuel-rich sooting premixed cyclohexane flame were presented in this work. Model predictions well agree with experimental data both in sooting and non-sooting flames. Major and minor species are properly predicted, together with the soot yield. The initial benzene peak was demonstrated to be due to the fast dehydrogenation reactions of the cycloalkane, which gives rise to cyclohexene and cyclohexadiene both via molecular and radical pathways. Once formed cyclohexadiene quickly forms benzene whereas in the postflame zone, benzene comes from the recombination and addition reactions of small radicals, with C3H3 + C3H3 playing the most important role in these conditions. An earlier soot inception was detected in the cyclohexane flame with respect to a n-hexane flame and this feature is not reproduced by the model that foresees soot formation significant only in the second part of the flame. The model insensitivity of soot to the reactant hydrocarbon was also observed comparing the predictions of three flames of cyclohexane, 1-hexene and n-hexane with the same temperature profile. A sensitivity analysis revealed that soot primarily comes from the HACA mechanism for the three flames, acetylene being the key species in the nucleation. Experimental data on soot inception seem to indicate the importance of the early formation of benzene, that depends on the fuel structure. It is thus important to further investigate the role of benzene and aromatics in order to explain this discrepancy.  相似文献   

12.
Examination of the surface behavior and flame structure of a bimodal ammonium perchlorate (AP) composite propellant at elevated pressure was performed using high speed (5 kHz) planar laser-induced fluorescence (PLIF) from 1 to 12 atm and visible surface imaging spanning 1–20 atm. The dynamics of the combustion of single, coarse AP crystals were resolved using these techniques. It was found that the ignition delay time for individual AP crystals contributed significant to the particle lifetime only at pressures below about 6 atm. In situ AP crystal burning rates were found to be higher than rates reported for pure AP deflagration studies. The flame structure was studied by exciting OH molecules in the gas phase. Two types of diffusion flames were observed above the composite propellant: jet-like flames and v-shaped, inverted, overventilated, flames (IOF) lifted off the surface. While jet-like diffusion flames have been imaged at low pressures and simulated by models, the lifted IOFs have not been previously reported or predicted. The causes for the observed flame structures are explained by drawing on an understanding of the surface topography and disparities in the burning rates of the fuel and oxidizer.  相似文献   

13.
Recent advances in the field of laser desorption/laser ionization mass spectrometry (LD/LI/MS) have renewed interest in these separation methods for fast analysis of chemical species adsorbed on soot particles. These techniques provide mass-separation of the desorbed phase with high selectivity and sensitivity and require very small soot samples. Combining LD/LI/MS with in situ measurements of soot and gaseous species is very promising for a better understanding of the early stage of soot growth in flames. In this work, three lightly sooting laminar jet flames (a methane diffusion flame and two premixed acetylene flames of equivalence ratio (?) = 2.9 and 3.5) were investigated by combining prompt and 50 ns-delayed laser-induced incandescence (LII) for spatially resolved measurements of soot volume fraction (fv) and laser-induced fluorescence (LIF) of polycyclic aromatic hydrocarbons (PAH). Soot and PAH calibration is performed by two-colour cavity ring-down spectroscopy (CRDS) at 1064 and 532 nm. Soot particles were sampled in the flames and analysed by LD/LI/Time-of-flight- MS. Soot samples are cooled to −170 °C to avoid adsorbed phase sublimation (under high vacuum in the TOF-MS). Our set-up is novel because of its ability to measure very low concentration of soot and PAH together with the ability to identify a large mass range of PAHs adsorbed on soot, especially volatile two-rings and three-rings PAHs. Studied flames exhibited a peak fv ranging from 15 ppb (acetylene, ? = 2.9) to 470 ppb (acetylene, ? = 3.5). Different mass spectra were found in the three flames, each exhibiting one predominant PAH mass; 202 amu (4-rings) in methane, 178 amu (3-rings) in acetylene,? = 2.9 and 128 amu (2-rings) in acetylene, ? = 3.5. These variations with flame condition contrasts with other recent studies and is discussed. The other PAH masses ranged from 102 (C8H6) to 424 amu (C34H16) and are well predicted by the stabilomer grid of Stein and Farr.  相似文献   

14.
In this contribution we report upon our static and dynamic light scattering experiments to characterize soot particles in flames. We studied sooting laminar premixed flame with acetylene as fuel mixed with air as oxidizer. The air equivalence ratio of the combustion was larger than one. We used a Kaskan type burner with circular geometry and a stabilizing flow of nitrogen around the flame. We focused on the determination of the size of the soot particles in the center of the flame as a function of height above burner. In addition we investigated the influence of the mixing ratio of the gases on the size of the particles. Our results show that static light scattering is better suited than dynamic light scattering for a fast and reliable characterization of soot particles in flames. The latter needs detailed a priori information about the flame to allow the unique determination of sizes from the diffusion measurements. The soot particles grow monotonously with height above burner and with decreasing air equivalence ratio. The aggregates have a fractal dimension lower than two.  相似文献   

15.
The growing demand of clean and efficient propulsion and energy systems has sparked an interest in understanding low-temperature combustion at high pressure. Cool flame transition and extinction limits as well as oxygen concentration dependence at elevated pressures provide insights of the low-temperature and high-pressure fuel reactivity. A new experimental high-pressure counterflow burner platform was designed and developed to achieve the studies of high-pressure cool flames. Dimethyl ether (DME) was chosen to study its non-premixed cool flame in high-pressure counterflow burner at pressure up to 5 atm, perhaps for the first time. This paper investigates the effects of pressure on cool flame structure, extinction and transition limits, and oxygen concentration dependence as well as ozone assisted warm flames of DME in experiments and numerical simulations. The results show that the reignition transition from cool flame to hot flame occurs either with the decrease of the strain rate at a given fuel concentration and pressure or with the increase of fuel mole fraction or pressure at a given strain rate. Furthermore, it is shown that the higher pressure shifts the cool flame to higher strain rates and results in higher cool flame extinction strain rates. However, the existing kinetic model of DME fails in predicting the cool flame extinction limit at elevated pressures. Besides, the cool flame extinction limits are proportional to nth power of the oxygen concentration, [O2]n, and the increase of pressure leads to stronger extinction limit dependence (larger n) on oxygen concentration. The present experiment and detailed kinetic analysis show clearly that increasing pressure promotes the low-temperature chemistry including the oxygen addition reactions. In addition, stable warm flame was first experimentally observed by using DME at elevated pressure with ozone sensitization.  相似文献   

16.
This study demonstrates the major differences in the evolution of the particle size distributions (PSDs), both measured and modeled, of soot in premixed benzene and ethylene flat flames. In the experiments, soot concentration and PSDs were measured by using a scanning mobility particle sizer (SMPS, over the size range of 3-80 nm). The model employed calculations of gas phase species coupled with a discrete sectional approach for the gas-to-particle conversion. The model includes reaction pathways leading to the formation of nano-sized particles and their coagulation to larger soot particles. The particle size distribution, both experimental and modeled, evolved from a single particle mode (the nucleation mode) to a bimodal size distribution. An important distinction between the results for the ethylene and benzene flames is the behavior of the nucleation mode which persists at all heights above the burner (HAB) for ethylene whereas it was greatly suppressed at greater HAB for the benzene flames. The explanation for the decreased nucleation mode at higher elevations in the benzene flame is that the aromatics are consumed in the oxidation zone of the flame. Fair predictions of particle-phase concentrations and particle sizes in the two flames were obtained with no adjustments to the kinetic scheme. In agreement with experimental data, the model predicts a higher formation of particulate in the benzene flame as compared with the ethylene flame.  相似文献   

17.
18.
建立了碳氢燃料在反射激波作用下高温裂解碳烟生成的检测系统,利用激光消光法测量了甲苯/氩气在高温条件下裂解生成碳烟的产率。实验条件:甲苯摩尔浓度0.25%和0.5%,压力约2和4 atm,温度1 630~2 273 K。获得了碳烟产率随温度、压力和燃料浓度的变化规律。碳烟产率随温度变化呈高斯分布,随着压力或浓度的增大,碳烟产率增大,碳烟产率最大达55%。产率的峰值温度随压力变化不大,但甲苯摩尔浓度从0.25%增大到0.5%时,峰值温度从1 852变为1 921 K。对比了压力为4 atm,燃料摩尔浓度为0.5%的甲基环己烷和甲苯的碳烟产率,甲基环己烷裂解碳烟产率峰值对应的温度为2 045 K,比甲苯约高135 K,但其最大碳烟产率仅有甲苯的1/8。结果为研究发动机内碳烟颗粒物排放及碳烟形成机理提供了实验依据。  相似文献   

19.
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.  相似文献   

20.
Particle size distribution functions of nascent soot formed in four burner-stabilized, premixed ethylene-oxygen-argon flames were studied in a spatially resolved manner by online sampling/scanning mobility particle sizer. Particle morphology was analyzed by atomic force microscopy (AFM) of substrate-deposited samples. Two of the four flames were doped with benzene. An aerosol electrometer is introduced to extend the lower detection limit to around 1.5 nm in diameter. The results show that the bimodal behavior of particle size is applicable to all premixed ethylene flames studied. The variation of the size distribution from flame to flame is conclusively attributed to flame temperature variation. Under the condition of an equal carbon concentration, benzene doping leads to negligible changes in the characteristics of the size distribution. For all flames studied, AFM observations show that nascent soot is liquid-like and spreads extensively upon impact on a substrate surface.  相似文献   

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