Simultaneously calibrated two-line atomic fluorescence for high-precision temperature imaging in sooting flames

Simultaneously calibrated, non-linear two-line atomic fluorescence (SC-nTLAF) thermometry for application in turbulent sooting flames has been developed to increase the precision of single-shot, planar measurements of gas temperature. The technique has been demonstrated in both steady and turbulent sooting flames, showing good agreements with previous optical measurements. The SC-nTLAF involves imaging simultaneously laser-induced fluorescence (LIF) of atomic indium in both the target flame and a non-sooting calibration flame for which the temperature distribution is known. The LIF intensities from the reference flame enable correction for fluctuations, not only in the laser power, but also in the laser mode. The resulting precision was found to be ±67 K and ±75 K (based on one standard deviation) in the rich and oxidizing regions of a steady sooting flame for which the measured temperature was 1610 K and 1854 K, respectively, with a spatial resolution of 550 × 550 µm². This corresponds to a relative precision of ∼ 4.1%. The resulting precision in the single-shot temperature images for a well-characterized, lifted ethylene jet diffusion flame (fuel jet Reynolds number = 10,000) compares favorably with previously reported data obtained with shifted-vibrational coherent anti-Stokes Raman spectroscopy (CARS), together with increased spatial resolution. The planar imaging also provides more details of the temperature distribution, particularly in the flame brush region, which offers potential for measurement of more parameters, such as gradients and spatial corrections. The new calibration method has also achieved a significant time-saving in both data collection and processing, which is an estimated total of ∼ 60%–70% compared with conventional nTLAF.     

On existence of nanoparticles below the sooting threshold

Nanometer-sized particles were studied by photoionisation mass spectrometry and scanning mobility particle sizer in laminar premixed ethylene flames above and below the critical sooting threshold. For sooting flames, both techniques detected a large number of particles with masses between 1 and 50 ku or diameter around a few nanometers. Neither method detected an appreciable number of particles below the sooting threshold in flames similar to those studied earlier for UV absorption and scattering of transparent soot. The absence of particle signals in both experimental techniques raises the question about the origin of UV absorption under nonsooting conditions.     

Temperature measurements in sooting counterflow diffusion flames using laser-induced fluorescence of flame-produced nitric oxide

Laser-based diagnostic methods are often used for non-intrusive studies of delicate processes of soot formation. When soot particles are heated by the laser pulse, their size distribution can be estimated from the cooling rate, provided that the local gas temperature is known. However, strong light absorption, scattering and fluorescence in sooting environment hinder non-intrusive laser-based temperature measurements. Methods based on fitting of laser-induced fluorescence spectra work well in stationary flames but usually require temperature tracer seeded into the flame. We have shown that in counterflow diffusion flames, often used for soot-formation studies, enough nitric oxide is produced for two-dimensional temperature imaging. Measured temperature profiles agree very well with chemical kinetic calculations for a variety of fuels if laser intensity is reduced to keep NO excitation in the linear regime. Gas composition affects line shapes at temperatures below 600 K and should be taken into account for accurate measurements.     

Soot studies of laminar diffusion flames with recirculation zones

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.     

Validation experiments for spatially resolved one-dimensional emission spectroscopy temperature measurements by dual-pump CARS in a sooting flame

In this work, an emission spectroscopic (ES) technique for the determination of soot temperatures in an axisymmetric flame is validated against coherent anti-Stokes Raman spectroscopy (CARS) as preparation for a zero gravity measurement campaign. In order to reduce valuable measurement times during the parabolic flights, a setup for spatially resolved one-dimensional measurements along a line has been built up using an imaging spectrometer and a CCD-camera for data acquisition.In order to assess the performance of the ES technique, accurate coherent anti-Stokes Raman scattering (CARS) measurements have been performed at the same conditions. Hereby, great care has to be taken to minimize the known interferences in sooting flames. The non-resonant signal contribution was suppressed by a polarization technique and the signal wavelength was shifted to an interference free region. These modifications are discussed in detail. The temperatures obtained by both methods are in good agreement in most regions of the flame. It turned out that the described approach for ES is an appropriate and robust alternative for measuring temperatures in sooting axisymmetric flames, if more accurate techniques cannot be applied, e.g., during investigations in zero-g parabolic flight experiments.     

Measurement of nanoparticles of organic carbon in non-sooting flame conditions

In this work we compare the results of several nanoparticle measurement techniques with the aim of investigating the formation of nanoparticles in non-sooting to slightly sooting flames. In slightly sooting conditions there is quite good agreement between Differential Mobility Analyser (DMA), Atomic Force Microscopy (AFM), and optical measurements on particle size and concentration. However, in rich flames below the onset of soot, DMA measures a strong drop-off in the total particle volume fraction at low fuel to air mixtures, which is not observed in optical or AFM measurements that detect a more gradual decrease in particle concentration with decreasing C/O and almost constant spectroscopic properties. The disagreement is significantly larger than experimental error and is only observed when the particle size distribution includes solely particles smaller than about 3 nm.Particle losses in the DMA sampling system does not seem to be the only possible reason for justifying the discrepancy with the other techniques. Further investigations are necessary in order to characterize chemically and physically this class of nanoparticles which constitute the earliest stage in the formation of particulate carbon.     

Computational and experimental investigation of the interaction of soot and NO in coflow diffusion flames

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.     

Nitric oxide concentration measurements in atmospheric pressure flames using electronic-resonance-enhanced coherent anti-Stokes Raman scattering

We report the application of electronic-resonance-enhanced coherent anti-Stokes Raman scattering (ERE-CARS) for measurements of nitric oxide concentration ([NO]) in three different atmospheric pressure flames. Visible pump (532 nm) and Stokes (591 nm) beams are used to probe the Q-branch of the Raman transition. A significant resonance enhancement is obtained by tuning an ultraviolet probe beam (236 nm) into resonance with specific rotational transitions in the (v’=0, v”=1) vibrational band of the A²Σ⁺–X²Π electronic system of NO. ERE-CARS spectra are recorded at various heights within a hydrogen-air flame producing relatively low concentrations of NO over a Hencken burner. Good agreement is obtained between NO ERE-CARS measurements and the results of flame computations using UNICORN, a two-dimensional flame code. Excellent agreement between measured and calculated NO spectra is also obtained when using a modified version of the Sandia CARSFT code for heavily sooting acetylene-air flames (φ=0.8 to φ=1.6) on the same Hencken burner. Finally, NO concentration profiles are measured using ERE-CARS in a laminar, counter-flow, non-premixed hydrogen-air flame. Spectral scans are recorded by probing the Q₁ (9.5), Q₁ (13.5) and Q₁ (17.5) Raman transitions. The measured shape of the [NO] profile is in good agreement with that predicted using the OPPDIF code, even without correcting for collisional effects. These comparisons between [NO] measurements and predictions establish the utility of ERE-CARS for detection of NO in flames with large temperature and concentration gradients as well as in sooting environments. PACS 07.88.+y; 42.62.Fi; 42.65.Dr     

轴对称含烟黑火焰非均匀温度与烟黑浓度分布同时重建模拟研究

对于非均匀吸收、发射、无散射的轴对称含烟黑火焰对象,常规双色法不再适用。本文基于烟黑辐射特性,提出并模拟研究了同时重建火焰温度与烟黑容积份额的新的辐射测量方法。从重建结果看,重建误差主要集中在火焰中心区域,这是观测路径上测量误差累积的结果。温度重建主要受火焰断面参数分布类型影响,而烟黑容积份额重建主要受测量误差的影响,这由它们与单色辐射强度的内在关系所决定。     

发射CT法测量层流乙烯扩散火焰中温度与烟黑浓度分布的实验研究

对于非均匀吸收、发射、无散射的轴对称含烟黑火焰对象,常规双色法不再适用。本文基于烟黑辐射特性,利用烟黑单色辐射强度图像信息采用CT算法同时重建含烟黑火焰温度与烟黑浓度分布,对层流乙烯扩散火焰的温度与烟黑容积份额进行测量,得到了较好的结果。     

Effect of fuel/air ratio and aromaticity on the molecular weight distribution of soot in premixed n-heptane flames

Soot growth from inception to mass-loading is studied in a wide range of molecular weights (MW) from 10⁵ to 10¹⁰u by means of size exclusion chromatography (SEC) coupled with on-line UV-visible spectroscopy. The evolution of MW distributions of soot is also numerically predicted by using a detailed kinetic model coupled with a discrete-sectional approach for the modeling of the gas-to-particle process. Two premixed flames burning n-heptane in slightly sooting and heavily sooting conditions are studied. The effect of aromatic addition to the fuel is studied by adding n-propylbenzene (10% by volume) to n-heptane in the heavily sooting condition. A progressive reduction of the MW distribution from multimodal to unimodal is observed along the flames testifying the occurrence of particle growth and agglomeration. These processes occur earlier in the aromatic-doped n-heptane flame due to the overriding role of benzene on soot formation which results in bigger young soot particles. Modeled MW distributions are in reasonable agreement with experimental data although the model predicts a slower coagulation process particularly in the slightly sooting n-heptane flame. Given the good agreement between model predictions and experiments, the model is used to explore the role of fuel chemistry on MW distributions. Two flames of n-heptane and n-heptane/n-propylbenzene in heavily sooting conditions with the same temperature profile and inert dilution are modeled. The formation of larger soot particles is still evident in the n-heptane/n-propylbenzene flame with respect to the n-heptane flame in the same operating conditions of temperature and dilution. In addition the model predicts a larger formation of molecular particles in the flame containing n-propylbenzene and shows that soot inception occurs in correspondence of their maximum formation thus indicating the importance of molecular growth in soot inception.     

RADIATIVE AND TOTAL HEAT FEEDBACK FROM FLAMES TO SURFACE IN VERTICAL WALL FIRES

Measurements of radiative and total heat transfer from turbulent flames to a wall are presented for combustion of propane, methane, and natural gas. Flames were generated by a linear burner placed at the bottom of an instrumented, cooled copper wall. The radiative heat feedback from the flames to the wall was determined from measurements using a narrow-angle radiometer and by employing mean-beam-length analysis. The radiative fraction of the total heat feedback was found to be almost independent of the burner power output when plotted against scaled height (vertical distance normalized with flame length). Among the three fuels tested, radiative fraction in flame-to-wall heat transfer was the maximum, for propane and minimum for methane, which can be explained based on sooting characteristics of flames. The total radiative energy transfer as a fraction of the burner output power is also presented for the three fuels.     

Influence of oxygen concentration on the sooting behavior of ethanol droplet flames in microgravity conditions

The influence of oxygen (O₂) concentration and inert on the sooting and burning behavior of large ethanol droplets under microgravity conditions was investigated through measurements of burning rate, flame temperature, sootshell diameter, and soot volume fraction. The experiments were performed at the NASA Glenn Research Center (GRC) 2.2 s drop tower in Cleveland, OH. Argon (Ar), helium (He), and nitrogen (N₂) were used as the inerts and the O₂ concentration was varied between 21% and 50% mole fraction at 2.4 atm. The unique configuration of spherically symmetric droplet flames enables effective control of sooting over a wide range of residence time of fuel vapor transport, flame temperature, and regimes of sooting to investigate attendant influences on burning behavior of droplets. For all inert cases, soot volume fraction initially increased as a function of the O₂ concentration. The highest soot volume fractions were measured for experiments in Ar environments and the lowest soot volume fractions were measured for the He environments. These differences were attributed to the changes in the residence time for fuel vapor transport and the flame temperature. For the He inert and N₂ inert cases, the soot volume fraction began to decrease after reaching a maximum value. The competition between the influence of residence time, rate of pyrolysis reactions, and soot oxidation can lead to this interesting behavior in which the soot volume fraction varies non-monotonically with increase in O₂ concentration. These experiments have developed new understanding of the burning and sooting behaviors of ethanol droplets under various O₂ concentrations and inert substitutions.     

Addition of NO2 to a laminar premixed ethylene-air flame: Effect on soot formation

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.     

Highly radiating hydrogen flames: Effect of toluene concentration and phase

Adapting hydrogen as a carbon-free fuel for industrial applications requires new, innovative approaches, especially when radiant heat transfer is required. One possible option is to dope hydrogen with bio-oils, containing aromatics that help produce highly sooting flames. This study investigates the potential doping effects of toluene on a hydrogen-nitrogen (1:1 vol) flames. Flames with 1–5% toluene, based on the mole concentration of hydrogen, are measured using a combination of techniques including: still photographs and laser-based techniques. Toluene was mixed with hydrogen-nitrogen fuel mixture as either a vapour carried by nitrogen, or as a dilute spray. Spray flames are found to produce substantially more polycylic aromatic hydrocarbons, with significantly more soot near the nozzle exit plane, than the prevaporised flames. Increasing the dopant concentration from 1 to 3% of the hydrogen has a marked effect on soot loading in the flame, although the further increasing the dopant concentration to 5% has a far smaller effect on the soot produced in the flame. Simulations of laminar flames using detailed chemical kinetics support the above findings and reveal details of the competition between soot precursor formation and hydrocarbon oxidation. Correlations of formation rates are non-linear with toluene concentration in cases where toluene represents less than 10% of the fuel, although expected linear relationships are noted beyond this regime up to 1:1 toluene/hydrogen blends. The study provides insight and explanation into effects of toluene as a dopant, comparison between flame doping in gaseous or liquid phases and suggests that flame doping and blending should be treated as different regimes for their global effect on flame sooting characteristics.     

Infrared cavity ringdown laser absorption spectroscopy (IR-CRLAS) in low pressure flames

-5 fractional absorption) and generality of IR-CRLAS for combustion studies is demonstrated for low pressure laminar flames and is shown to be robust even in sooting environments with high temperature gradients. The ability to obtain (1-D) spatially resolved spectra of both reactants and products within a narrow spectral region is also demonstrated. In these initial flame studies, two information rich mid-infrared spectral regions are probed at Doppler-limited resolution, centered about 1.5 μm and 3.3 μm. Received: 30 August 1996     

Water vapour effects on temperature and soot loading in ethylene flames in hot and vitiated coflows

Flames in hot, low oxygen environments exist in a variety of practical applications. These conditions result in significant mixing between fuel and combustion products, such as water vapour, or diluents included for emissions control. The chemical and physical effects of water vapour as a diluent are investigated in a series of ethylene flames in a jet in hot coflow burner to determine the effects on temperature and soot fields. The combined analyses of photographs, non-linear excitation regime two-line atomic fluorescence (NTLAF) of indium, planar laser-induced incandescence (LII) and one-dimensional opposed-flow flame simulations demonstrate the dominance of the chemistry, driven by the hot and vitiated oxidant, in soot reduction. Although photographs appear to suggest that both highly vitiated coflows, and highly diluted jet flames have global effect on the flames, detailed measurements reveal significantly different trends in their soot and temperature fields. The chemical contribution of water vapour as a reactant, as a third-body in ethylene decomposition and a source of H and OH in the rich mixture is further described, and trends subsequently identified, in the context of formation of polycyclic aromatic hydrocarbons and soot reduction.     

Experimental and kinetic modeling study of sooting atmospheric-pressure cyclohexane flame

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.     

Diode laser atomic fluorescence temperature measurements in low-pressure flames

Temperature measurements have been performed in a low-pressure flame by the technique of diode laser induced atomic fluorescence. The experiments were done in a near-stoichiometric flat-flame of premixed methane, oxygen and nitrogen, at a pressure of 5.3 kPa. Indium atoms were seeded to the flame and probed using blue diode lasers; the lineshapes of the resulting fluorescence spectra were used to determine the flame temperature at a range of heights above the burner plate. The particular issues associated with the implementation of this measurement approach at low pressure are discussed, and it is shown to work especially well under these conditions. The atomic fluorescence lineshape thermometry technique is quicker to perform and requires less elaborate equipment than other methods that have previously been implemented in low-pressure flames, including OH-LIF and NO-LIF. There was sufficient indium present to perform measurements at all locations in the flame, including in the pre-heat zone close to the burner plate. Two sets of temperature measurements have been independently performed by using two different diode lasers to probe two separate transitions in atomic indium. The good agreement between the two sets of data provides a validation of the technique. By comparing thermocouple profiles recorded with and without seeding of the flame, we demonstrate that any influence of seeding on the flame temperature is negligible. The overall uncertainty of the measurements reported here is estimated to be ±2.5% in the burnt gas region.     

A computational framework for predicting laminar reactive flows with soot formation

Numerical modeling is an attractive option for cost-effective development of new high-efficiency, soot-free combustion devices. However, the inherent complexities of hydrocarbon combustion require that combustion models rely heavily on engineering approximations to remain computationally tractable. More efficient numerical algorithms for reacting flows are needed so that more realistic physics models can be used to provide quantitative soot predictions. A new, highly-scalable combustion modeling tool has been developed specifically for use on large multiprocessor computer architectures. The tool is capable of capturing complex processes such as detailed chemistry, molecular transport, radiation, and soot formation/destruction in laminar diffusion flames. The proposed algorithm represents the current state of the art in combustion modeling, making use of a second-order accurate finite-volume scheme and a parallel adaptive mesh refinement (AMR) algorithm on body-fitted, multiblock meshes. Radiation is modeled using the discrete ordinates method (DOM) to solve the radiative transfer equation and the statistical narrow-band correlated-k (SNBCK) method to quantify gas band absorption. At present, a semi-empirical model is used to predict the nucleation, growth, and oxidation of soot particles. The framework is applied to two laminar coflow diffusion flames which were previously studied numerically and experimentally. Both a weakly-sooting methane–air flame and a heavily-sooting ethylene–air flame are considered for validation purposes. Numerical predictions for these flames are verified with published experimental results and the parallel performance of the algorithm analyzed. The effects of grid resolution and gas-phase reaction mechanism on the overall flame solutions were also assessed. Reasonable agreement with experimental measurements was obtained for both flames for predictions of flame height, temperature and soot volume fraction. Overall, the algorithm displayed excellent strong scaling performance by achieving a parallel efficiency of 70% on 384 processors. The proposed algorithm proved to be a robust, highly-scalable solution method for sooting laminar flames.