Large eddy simulation of soot evolution in turbulent nonpremixed bluff body flames

Large Eddy Simulation (LES) is utilized to investigate soot evolution in a series of turbulent nonpremixed bluff body flames featuring different bluff body diameters. The modeling framework relies on recent development in the soot subfilter Probability Density Function (PDF) model that can correctly account for the distribution of soot with respect to mixture fraction, correcting errors in previous soot subfilter PDF models that significantly overpredict soot oxidation. With the previous soot subfilter PDF model, no soot was observed outside of the recirculation zone in past studies on similar bluff body flames. Results obtained with the current LES modeling approach compare favorably with the experimental measurements of the flow field and the soot volume fraction. Notably, the current LES modeling approach correctly predicts large soot volume fractions in the recirculation zone, a decrease in the soot volume fraction through the high-strain neck region, and then an increase again in the downstream jet-like region. Consistent with the experimental measurements, the larger bluff body diameter, with its larger recirculation zone with longer residence times, generates more soot in the recirculation zone and also more soot in the high-strain neck region. Analysis of the soot volume fraction source terms lead to mechanistic understanding of soot evolution in the entirety of the bluff body flames. Most of the soot generated in the recirculation zone is oxidized but some escapes unoxidized and is passively transported through the neck region. Virtually no new soot forms in the downstream jet-like region, and the increase in the soot volume fraction in the jet-like region is due to acetylene-based surface growth of the soot transported through the neck region. This mechanism could not be predicted with the previous soot subfilter PDF model, with the recent soot subfilter PDF model being critical in the understanding of this basic mechanism.     

Assessment of interferences to nonlinear two-line atomic fluorescence (NTLAF) in sooty flames

Nonlinear excitation regime two-line atomic fluorescence (NTLAF) is a laser-based thermometry technique that has application in turbulent flames with soot. However, no assessment of the various interferences from soot or its precursors in flames with high soot loadings on the technique is available. To examine these issues, both on- and off-wavelength NTLAF measurements are presented and compared for laminar nonpremixed ethylene-air flames. Laser-induced incandescence (LII) measurements were used to determine the corresponding soot concentration and location in the investigated flames. The measurements indicate that interferences, such as spurious scattering and laser-induced incandescence from soot, are not significant for the present set of flame conditions. However, interferences from soot precursors, predominantly condensed species (CS) and perhaps polycyclic aromatic hydrocarbons (PAH), can be significant. Potential detection schemes to correct or circumvent these interference issues are also presented.     

Nano organic carbon and soot in turbulent non-premixed ethylene flames

Spectral optical techniques are combined to characterise the distribution of large-molecule soot precursors, nanoparticles of organic carbon, and soot in two turbulent non-premixed ethylene flames with differing residence times. Laser-induced fluorescence, laser-induced incandescence and light scattering are used to define distributions across the particle size distribution. From the scattering and laser-induced emission measurements it appears that two classes of particles are formed. The first ones are preferentially formed in the fuel-rich region of the flame closer to the nozzle, have sizes of the order of few nanometers but are not fully solid particles, because the constituent molecules still maintain their individual identity exhibiting strong broadband fluorescence in the UV. The second class of particles constituted by solid particles, with sizes of the order of tens of nanometers are able to absorb a sufficient number of photons to be heated to incandescent temperatures. These larger particles are formed at larger residence times in the flame since they are the result of slow growth processes such as coagulation or carbonization. The flames are also modeled in order to produce mixture fraction maps. A new discovery is that nanoparticles of organic carbon concentration, unlike soot, does correlate well with mixture fraction, independent of position in the flame. This is likely to be a significant benefit to future modelling of soot inception processes in turbulent non-premixed flames.     

Numerical investigation of the effect of signal trapping on soot measurements using LII in laminar coflow diffusion flames

Laser-induced incandescence has been rapidly developed into a powerful diagnostic technique for measurements of soot in many applications. The incandescence intensity generated by laser-heated soot particles at the measurement location suffers the signal trapping effect caused by absorption and scattering by soot particles present between the measurement location and the detector. The signal trapping effect was numerically investigated in soot measurements using both a 2D LII setup and the corresponding point LII setup at detection wavelengths of 400 and 780 nm in a laminar coflow ethylene/air flame. The radiative properties of aggregated soot particles were calculated using the Rayleigh–Debye–Gans polydisperse fractal aggregate theory. The radiative transfer equation in emitting, absorbing, and scattering media was solved using the discrete-ordinates method. The radiation intensity along an arbitrary direction was obtained using the infinitely small weight technique. The contribution of scattering to signal trapping was found to be negligible in atmospheric laminar diffusion flames. When uncorrected LII intensities are used to determine soot particle temperature and the soot volume fraction, the errors are smaller in 2D LII setup where soot particles are excited by a laser sheet. The simple Beer–Lambert exponential attenuation relationship holds in LII applications to axisymmetric flames as long as the effective extinction coefficient is adequately defined.     

Single-shot measurement of soot aggregate sizes by wide-angle light scattering (WALS)

The wide-angle light scattering (WALS) approach has been utilized for the measurement of soot aggregate sizes (radii of gyration) in flames on a single-shot basis. Key elements are a pulsed laser and an ellipsoidal mirror, which images the light scattered within a plane onto an intensified CCD camera, thus allowing for an instantaneous acquisition of a full scattering diagram with high resolution. Results for a laminar premixed flame exhibit good agreement with averaged data and demonstrate the feasibility of the method. The applicability of the technique to unsteady combustion processes is demonstrated by measuring aggregate sizes in a weakly turbulent jet-diffusion flame. In both cases light scattering results are verified by data obtained from electron microscopy analysis of sampled soot.     

Determination of Soot Particle Size in a Premixed Flame: a Static and Dynamic Light Scattering Study

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.     

Studies of the flow and turbulence fields in a turbulent pulsed jet flame using LES/PDF

A turbulent piloted jet flame subject to a rapid velocity pulse in its fuel jet inflow is proposed as a new benchmark case for the study of turbulent combustion models. In this work, we perform modelling studies of this turbulent pulsed jet flame and focus on the predictions of its flow and turbulence fields. An advanced modelling strategy combining the large eddy simulation (LES) and the probability density function (PDF) methods is employed to model the turbulent pulsed jet flame. Characteristics of the velocity measurements are analysed to produce a time-dependent inflow condition that can be fed into the simulations. The effect of the uncertainty in the inflow turbulence intensity is investigated and is found to be very small. A method of specifying the inflow turbulence boundary condition for the simulations of the pulsed jet flame is assessed. The strategies for validating LES of statistically transient flames are discussed, and a new framework is developed consisting of different averaging strategies and a bootstrap method for constructing confidence intervals. Parametric studies are performed to examine the sensitivity of the predictions of the flow and turbulence fields to model and numerical parameters. A direct comparison of the predicted and measured time series of the axial velocity demonstrates a satisfactory prediction of the flow and turbulence fields of the pulsed jet flame by the employed modelling methods.     

Investigation on the influence of soot size on prompt LII signals in flames

Theoretical papers predict that prompt LII signals are weakly dependent on the soot size due to the fact that larger particles reach higher temperatures during the heating process by nanosecond laser pulses. This question is of crucial importance for establishing LII as a practical technique for soot volume fraction measurements. In this work two-color prompt LII measurements have been performed in several locations of diffusion and rich premixed ethylene-air flames. The experimental apparatus was carefully designed with a probe volume of uniform light distribution and sharp edges, a 4 ns integration time around the signal pulse peak and narrow spectral bandwidth. Measurements did not confirm the theoretical predictions concerning an increase of temperature for larger particles. On the contrary, larger particles in richer premixed flames exhibit a lower 400/700 signal ratio. This can probably be attributed to small differences in the refractive index of soot.     

Transported JPDF modelling and measurements of soot at elevated pressures

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.     

Ray tracing of chemiluminescence in an unconfined non-premixed turbulent jet flame using large-eddy simulation

Optical diagnostic techniques, such as chemiluminescence imaging, are commonly used to study turbulent flames. Inherent to turbulent flames is the spatio-temporal variation of the volumetric distribution of temperature and chemical composition. In consequence, the index of refraction varies accordingly and causes distortion of any optical ray intersecting the turbulent flame. This distortion is well known as beam steering. Beam steering may degrade imaging quality by reducing the overall spatial resolution. Its impact of course depends on the actual specifications of the imaging system itself. In this study a methodology is proposed to tackle this issue numerically and is exemplified for chemiluminescence imaging in a well-known turbulent hydrogen-fueled jet flame. Large-eddy simulation (LES) of this unconfined non-premixed flame is used to simulate instantaneous volumetric distributions of the flow and scalar fields including the local index of refraction. This simulation additionally predicts local concentrations of electronically excited chemiluminescent active species. At locations with significantly high concentrations of luminescent species, optical rays are initiated in the direction of the array detector used for recording single chemiluminescence images. Assuming the validity of geometrical optics, these rays are tracked along their pathways. Their direction of propagation changes according to the local instantaneous distribution of the index of refraction. After leaving the computational domain of the ray tracing code which is fed by the LES, each ray is processed by the commercial code ZEMAX^® and imaged onto an array detector. Measured and numerically simulated ensemble-averaged chemiluminescence images are compared to each other. Overall, a satisfying agreement is observed. The primary aim of this paper is the exposition of this method where numerical and experimental results are not any more compared in the flame but where this comparison is shifted to the imaging plane. Future extensions to higher pressures in enclosed combustors or internal combustion engines where beam-steering effects are much more pronounced than in atmospheric jet flames are addressed.     

Investigation of optical properties of aging soot

The optical properties of soot, in particular the propensity of soot to absorb and scatter light as a function of wavelength, are key parameters for the correct interpretation of soot optical diagnostics. An overview of the data available in the literature highlights the differences in the reported optical properties of aging soot. In many cases, the properties of mature soot are used when evaluating in-flame soot but this assumption might not be suitable for all conditions and should be checked. This need has been demonstrated by performed spectral resolved line-of-sight attenuation (Spec-LOSA) measurements on an ethylene/air premixed and non-premixed flame. Transmission electron microscopy of thermophoretically sampled soot was also performed to qualify the soot aging and to establish soot morphology in order to correct light extinction coefficients for the scattering contribution. The measured refractive index absorption function, E(m) _λ , showed a very strong spectral dependence which also varied with height above the burner for both flames. However, above 700 nm, the slope of the refractive index function was near zero for both flames and all measurement heights. The upper visible and near infrared wavelengths are therefore recommended for soot optical measurements.     

Large scale effects in weakly turbulent premixed flames

In this study we numerically investigate large scale premixed flames in weakly turbulent flow fields. A large scale flame is classified as such based on a reference hydrodynamic lengthscale being larger than a neutral (cutoff) lengthscale for which the hydrodynamic or Darrieus–Landau (DL) instability is balanced by stabilizing diffusive effects. As a result, DL instability can develop for large scale flames and is inhibited otherwise. Direct numerical simulations of both large scale and small scale three-dimensional, weakly turbulent flames are performed at constant Karlovitz and turbulent Reynolds number, using two paradigmatic configurations, namely a statistically planar flame and a slot Bunsen flame. As expected from linear stability analysis, DL instability induces its characteristic cusp-like corrugation only on large scale flames. We therefore observe significant morphological and topological differences as well as DL-enhanced turbulent flame speeds in large scale flames. Furthermore, we investigate issues related to reaction rate modeling in the context of flame surface density closure. Thicker flame brushes are observed for large scale flames resulting in smaller flame surface densities and overall larger wrinkling factors.     

Instantaneous in-flame measurement of soot volume fraction, primary particle diameter, and aggregate radius of gyration via auto-compensating laser-induced incandescence and two-angle elastic light scattering

A new combination of soot diagnostics employing two-angle elastic light scattering and laser-induced incandescence is described that is capable of producing non-intrusive, instantaneous, and simultaneous, in situ measurements of soot volume fraction, primary particle size, and aggregate radius of gyration within flames. Controlled tests of the new apparatus on a well-characterized laminar flame show good agreement with existing measurements in the literature. From a detailed and comprehensive Monte Carlo uncertainty analysis of the results, it was found that the uncertainty in all three measured parameters is dominated by knowledge of soot properties and aggregation behavior. The soot volume fraction uncertainty is dominated by uncertainty in the soot refractive index light absorption function; the primary particle diameter uncertainty is dominated by uncertainty in the fractal prefactor; while the uncertainty in the aggregate radius of gyration is dominated by the uncertainty in the width of the distribution of aggregate sizes.     

Subgrid combustion modeling of 3-D premixed flames in the thin-reaction-zone regime

Large eddy simulation (LES) is used to investigate three-dimensional (3D) lean premixed turbulent methane–air flames in the thin-reaction-zone regime. In this regime, the Kolmogorov scale is smaller than the preheat zone thickness, but larger than the reaction zone thickness. Past numerical studies of similar flames were primarily direct numerical simulation either in two-dimensions or using the artificially thickened flame approach in 3D. For an LES the effect of small (unresolved) scales on the scalar field must be, modeled accurately to capture the correct flame structure. A subgrid combustion model based on the linear-eddy-mixing (LEM) model is used within an LES framework (called LEM–LES hereafter) to capture the 3D flame-structure of the highly stretched premixed flames. A finite-rate, one-step methane–air chemistry with a non-unity Lewis number formulation is used in this study. The simulated flame structure resembles flames experimentally studied in the thin-reaction-zone regime. Even though the preheat zone is broadened by the penetration of small eddies, the chemical reaction zone remains thin and localized. This feature is captured properly in the current LEM–LES approach. The flame structure and other statistics such as the flame area evolution, curvature, and strain-rate statistics computed using the LEM–LES are also in good agreement with the past DNS studies.     

Two-dimensional soot distributions in buoyant turbulent fires

Spatially resolved two-dimensional soot volume fractions were measured using laser-induced incandescence in 7.1 cm methane and ethylene turbulent buoyant flames to study the distributions of soot in vertical and horizontal planes, and to provide data for soot model validation. Factors affecting the LII signals were considered including the laser energy profile and the laser attenuation effects. The absolute soot volume fractions were obtained by comparison to existing extinction measurements. The instantaneous soot images were collected to cover the entire flame height. Statistical quantities of soot volume fractions including mean, root mean square, probability density function, and spatial correlation coefficient were calculated at five downstream locations. The results show that instantaneous distributions of soot volume fractions exhibit significant differences compared to the ensemble averages, strong fluctuation around the mean, relatively homogeneous probability density function, and highly anisotropic spatial correlation.     

Identification and analysis of instability in non-premixed swirling flames using LES

Large eddy simulations (LES) of turbulent non-premixed swirling flames based on the Sydney swirl burner experiments under different flame characteristics are used to uncover the underlying instability modes responsible for the centre jet precession and large scale recirculation zone. The selected flame series known as SMH flames have a fuel mixture of methane-hydrogen (50:50 by volume). The LES solves the governing equations on a structured Cartesian grid using a finite volume method, with turbulence and combustion modelling based on the localised dynamic Smagorinsky model and the steady laminar flamelet model respectively. The LES results are validated against experimental measurements and overall the LES yields good qualitative and quantitative agreement with the experimental observations. Analysis showed that the LES predicted two types of instability modes near fuel jet region and bluff body stabilised recirculation zone region. The mode I instability defined as cyclic precession of a centre jet is identified using the time periodicity of the centre jet in flames SMH1 and SMH2 and the mode II instability defined as cyclic expansion and collapse of the recirculation zone is identified using the time periodicity of the recirculation zone in flame SMH3. Finally frequency spectra obtained from the LES are found to be in good agreement with the experimentally observed precession frequencies.     

Several applications of laser diagnostics for visualization of combustion phenomena

Several applications of laser diagnostic techniques to visualize combustion phenomena are presented, including reactive Mie scattering for flow, Rayleigh and Raman spectroscopy for major species, laser-induced fluorescence for minor species, and laser extinction, scattering, and laser-induced incandescence for soot. These techniques have been applied to diffusion flame oscillation, a recirculation zone in a burner, laminar and turbulent lifted flames, flame propagation along a vortex tube, and soot zone characteristics, to demonstrate the usefulness of the techniques to provide a better understanding of physical mechanisms.     

Two-color laser-induced incandescence and cavity ring-down spectroscopy for sensitive and quantitative imaging of soot and PAHs in flames

Laser-induced incandescence is a technique which enables the measurement of soot volume fractions. However, the laser-induced soot emission might be affected by a fluorescence background generally ascribed to the polycyclic aromatic hydrocarbon compounds (PAHs) present at the soot location. In this paper, spatially resolved distributions of PAH absorbance and soot are obtained in sooting diffusion flames. The original method developed here consists in comparing the emission distributions induced by two different laser wavelengths: (1) at 1064 nm emission signals are exempt from PAH fluorescence and (2) at 532 nm both soot incandescence and PAH emission contribute to the total signal. In addition, the absolute absorption coefficient of the PAH mixture is determined by comparing absorption measurements obtained by cavity ring-down spectroscopy (CRDS) at 1064 nm and 532 nm. The proposed method can provide highly sensitive 2D imaging of PAHs and soot using the fundamental and the second-harmonic frequencies of a single YAG laser. Finally, 2D distributions of PAH absorbance and soot volume fraction calibrated by CRDS are obtained in two diffusion flames, particularly in a very low-sooting flame exhibiting a maximum PAH absorbance of 6×10^-4 cm^-1 and a maximum soot volume fraction of 3 ppb only. The respective spatial distributions of PAHs and soot are shown to vary with the initial C/O ratio. PACS 33.20.Lg; 42.62.Fi; 44.40.+a     

Polarimetric weak-localization effect in scattering of natural light in the region of small phase angles

Results of laboratory measurements and interpretations of the polarimetric effect of weak localization (negative polarization) appearing under scattering of natural light by a dark ultradisperse surface (soot with albedo of 2.5%) are presented. The measurements were carried out in red light in a range of phase angles of 0.2°–4.2°. It was revealed that the soot, despite the low albedo, shows the polarimetric weak-localization effect inherent in bright surfaces such as the surface formed by smoked MgO. The results of measurements are interpreted using numerical simulation of multiple light scattering in a medium consisting of particles whose characteristics are close to those observed for soot. As the result of simulation, it was found that the scattering with the multiplicity exceeding two can give rise to a negative polarization branch, which becomes narrower with increasing scattering order. For the case of soot, four orders of scattering is sufficient to describe the observed polarimetric effect of weak localization with a necessary accuracy.