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1.
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   

2.
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   

3.
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   

4.
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   

5.
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   

6.
Soot formation from the combustion of toluene (C6H5CH3) and of two concentrations of nano-sized-ceria-laden toluene was monitored using a shock tube to observe the effect of the organometallic additive on the formation of soot from its point of inception. Two concentrations of ceria, of chemical composition CeO1.63, were employed to examine the effect on soot production of toluene over the range of temperature 1588-2370 K using two levels of inert gas dilution in which reflected-shock pressure was maintained near 1.5 atm. The ceria nanoparticles were synthesized using a microemulsion technique which employs sodium dioctyl sulfosuccinate (AOT), a surfactant, to retard agglomeration. Introduction of the nanoparticles into the shock tube is achieved using a novel, two-stage injection procedure. Soot yield measurements reveal that the presence of ceria has no direct implications on peak soot concentration near 1950 K. A shift in the parabolic soot profile of toluene in the direction of increased temperature was observed for each concentration of ceria with a larger shift occurring for increased concentration of ceria, although the same effect was exhibited for the toluene-AOT mixtures in absence of ceria, supporting an inefficaciousness of ceria on soot suppression on kinetic timescales. It is evidenced in measured soot delay times that the presence of the surfactant in absence of ceria significantly slows the rate of soot growth for T < 2000 K, while the presence of ceria has a relatively negligible impact. Under conditions of higher fuel concentration, a remarkable decrease in soot accumulation on the shock tube walls was observed in experiments using the ceria-toluene mixtures over that yielded by pure toluene combustion. In the present paper, the authors report the first measurements of nanoparticle-influenced combustion of a hydrocarbon as performed in a shock tube.  相似文献   

7.
This paper presents the study we carried out on the formation of soot particles in low-pressure premixed CH4/O2/N2 flames by using Laser-Induced Incandescence (LII). Flames were stabilised at 26.6 kPa (200 torr). Four different equivalence ratios were tested (Φ = 1.95, 205, 2.15 and 2.32), Φ = 1.95 corresponding to the equivalence ratio for which LII signals begin to be measurable along the flame. The evolution of the LII signals with laser fluence (fluence curve), time (temporal decay) and emission wavelength is reported at different heights above the burner. We specifically took advantage of the low-pressure conditions to probe with a good spatial resolution the soot inception zone of the flames. Significant different behaviours of the fluence curves are observed according to the probed region of the flames and Φ. In addition, while the surface growth process is accompanied by an increase in the LII decay-times (indicator of the primary particle diameter) at higher Φ, decay-times become increasingly short at lower Φ reaching a constant value along the flame at Φ = 1.95. These behaviours are consistent with the detection of the smallest incandescent particles in the investigated flames, these particles having experienced very weak surface growth. Flame modelling including soot formation has been implemented in flames Φ = 2.05 and 2.32. Experimental quantitative soot volume fraction profiles were satisfactorily reproduced by adjusting the fraction of reactive soot surface available for reactions. The qualitative variation of the computed soot particle diameter and the relative weight of surface growth versus nucleation were consistent with the experimental observations.  相似文献   

8.
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 (fV) 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 fV 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 fV 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 fV obtained using advanced optical techniques for soot formation studies.  相似文献   

9.
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   

10.
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.  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.
Accurate measurements and modelling of soot formation in turbulent flames at elevated pressures form a crucial step towards design methods that can support the development of practical combustion devices. A mass and number density preserving sectional model is here combined with a transported joint-scalar probability density function (JDPF) method that enables a fully coupled scalar space of soot, gas-phase species and enthalpy. The approach is extended to the KAUST turbulent non-premixed ethylene-nitrogen flames at pressures from 1 to 5 bar via an updated global bimolecular (second order) nucleation step from acetylene to pyrene. The latter accounts for pressure-induced density effects with the rate fitted using comparisons with full detailed chemistry up to 20 bar pressure and with experimental data from a WSR/PFR configuration and laminar premixed flames. Soot surface growth is treated via a PAH analogy and soot oxidation is considered via O, OH and O2 using a Hertz-Knudsen approach. The impact of differential diffusion between soot and gas-phase particles is included by a gradual decline of diffusivity among soot sections. Comparisons with normalised experimental OH-PLIF and PAH-PLIF signals suggest good predictions of the evolution of the flame structure. Good agreement was also found for predicted soot volume statistics at all pressures. The importance of differential diffusion between soot and gas-phase species intensifies with pressure with the impact on PSDs more evident for larger particles which tend to be transported towards the fuel rich centreline leading to reduced soot oxidation.  相似文献   

13.
Samples of condensable material from opposed flow diffusion flames of methane and acetylene and oxygen enriched air at atmospheric pressure were collected and analyzed by high-pressure liquid chromatography to determine the fullerene yield. High resolution transmission electron microscopy studies revealed the presence of fullerenes and well-defined carbon layers with various degrees of curvature. Results show that fullerene formation strongly increases with the acetylene content in the fuel. Increasing strain rate positively affects the fullerene content in the condensable material; higher strain rate flames favor fullerenes over soot, indicating lower fullerene consumption by soot due to lower soot concentration. If the oxygen content in the oxidizing oxygen/nitrogen mixture is increased, fullerene concentration increases due to the higher temperatures and higher precursor concentration. Similar relative variations of fullerene concentrations with flame conditions are predicted by the numerical model. However, the absolute concentrations of fullerenes are, in general, underpredicted by 4 orders of magnitude. This result can be partially attributed to uncertainties in the rate coefficients for H-abstraction and C2H2-addition. This discrepancy also suggests that other important fullerene formation pathways are to be included in the numerical model.  相似文献   

14.
Strategies for spatially resolved soot volume-fraction measurements have been investigated in sooting laboratory flames with known soot characteristics. Two techniques were compared: Laser-Induced Fluorescence in C2 from Laser-Vaporized Soot (LIF(C2)LVS), and Laser-Induced Incandescence of soot (LII). The LII signal is the increased temperature radiation from soot particles which have been heated to temperatures of several thousand degrees as a consequence of absorption of laser radiation. The LIF(C2)LVS technique is based on the production of C2 radicals from laser-vaporized soot which occurs for laser intensities ≥107 W/cm2. A laser wavelength is chosen such that besides vaporizizng the soot, it also excites the C2 radicals, and the subsequent C2 fluorescence signal is detected. The signals from both techniques showed good correlation with soot volume fractions in the studied flame. The dependence of the signals on experimental parameters was studied, and the influence of interfering radiation, such as background flame luminosity and fluorescence from polyaromatic hydrocarbons, on studied signals was established. The potential of the two techniques for imaging of soot volume fractions in laboratory flames was demonstrated. Advantages and disadvantages of the studied techniques are discussed.  相似文献   

15.
The effect of multiple laser pulses reaching soot particles before an actual laser-induced incandescence (LII) measurement is investigated in order to gain some insights on soot morphological and fine structure changes due to rapid laser heating. Soot, extracted from a premixed and a quenched diffusion flames, is flowing through a tubular cell and undergoes a variable number of pulses at different fluence. The response of soot is studied by the two-color LII technique. Transmission electron microscopy (TEM) analysis of laser-modified soot aggregates from the diffusion flame is also presented. The results indicate that even at low laser fluences a permanent soot transformation is induced causing an increase in the absorption function E(m). This is interpreted as an induced graphitization of soot particles by the laser pulse heating. At high fluences the vaporization process and a profound restructuring of soot particles affect the morphology of the aggregates. Soot from diffusion and premixed flames behaves in a similar way although this similarity occurs at different fluence levels indicating a different initial fine structure of soot particles.  相似文献   

16.
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.  相似文献   

17.
O. Checa  R. A. Vargas  J. E. Diosa 《Ionics》2014,20(4):545-550
The dispersion curves of the dielectric response for KHSeO4 were obtained in the radio frequency range at several isotherms below the fast proton conducting phase (T?<?415 K). The results reveal a distinct dielectric relaxation at low frequency, which is about 682 Hz at 320 K, and then, it shifts to higher frequencies (~10 kHz) as the temperature increases. The f max vs. reciprocal T shows an activated relaxation process with an activation energy of 0.5 eV, which is in close agreement with that associated with transport of charge carriers. We suggest that the observed dielectric relaxation could be attributed to polarization induced by the proton jump and selenate tetrahedral reorientations. The displacement of mobile H+ proton accompanied by SeO 4 ??2 tetrahedra reorientations creates structural distortion in both sublattices which induce localized dipoles like HSeO 4 ? .  相似文献   

18.
19.
Scanning mobility particle sizer (SMPS) and transmission electron microscopy (TEM) studies were conducted for TiO2 and soot particles. The TiO2 particles were produced from a premixed stagnation ethylene-oxygen-argon flame (? = 0.36) doped with titanium tetraisopropoxide. Soot was generated from a burner-stabilized premixed ethylene-oxygen-argon flame (? = 2.5). The close agreement among SMPS, TEM, and X-ray diffraction results for TiO2 nanoparticles demonstrates that the probe sampling/mobility measurement technique is accurate for on-line analysis of the size distribution of particles as small as 3 nm in diameter. In the case of soot, notable disagreement between the SMPS and TEM sizes was found and attributable to the fact that the soot taken from the flame studied herein is liquid-like and that upon deposition on the TEM grid, the primary particles do not retain their sphericity. This interpretation is supported by measurements with photo ionization aerosol mass spectrometry, small angle neutron scattering, and thermocouple particle densitometry.  相似文献   

20.
Many proposed oxy-combustion concepts for carbon capture incorporate the recycling of flue gas which is used as a dilution gas to aid in the control of temperature and heat flux. Improvements in efficiency may be realized by significantly reducing the recycle flue gas (RFG), however, in application, care must be taken to avoid excessive radiant heat flux and gas temperature. One of the features oxy-combustion, unlike air-fired combustion, is that the oxygen and dilution gases are initially separated. RFG can, for example, be strategically blended with either the fuel stream, or oxidizer stream, or both, which affects the stoichiometric mixture fraction, Zst. In this work, the effects of the amount of dilution, or RFG, and Zst on soot fraction are experimentally investigated in a laminar coflow flame. Carbon dioxide is employed as the dilution gas to simulate the recycling of dry flue gas. Soot fraction and temperature are quantitatively determined by a flame image processing technique. In addition, the visible and near-IR emission spectra are given. When dilution, or RFG, is reduced, while holding Zst constant, soot formation and thermal radiation increase due to higher temperature. However, high temperature flames with reduced or zero soot are achieved by increasing Zst via the combination of fuel dilution and oxygen enrichment. This study highlights the inherent flexibility of oxy-fuel combustion, which offers the opportunity to control flame temperature and gas volume while independently controlling soot formation and radiant heat transfer.  相似文献   

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