Surface deposition and coagulation efficiency of combustion generated nanoparticles in the size range from 1 to 10 nm

The size distribution of the nanoparticles formed in premixed ethylene–air flames and collected thermophoretically on mica cleaved substrates is obtained by atomic force microscopy (AFM). The distribution function extends from 1 to about 5 nm in non-sooting flames and in the soot pre-inception region of the richer flames, while it becomes bimodal and larger particles are formed in the soot inception region of the slightly sooting flames. The distribution is compared with the size distribution of nano-sized organic carbon (NOC) and soot particles, obtained by “in situ” multi-wavelength extinction and light scattering methods. The deposition efficiency is estimated from the differences between these two size distribution functions as a function of the equivalent diameter of the nanoparticles. Furthermore, the coagulation coefficient of particles in flame is obtained from the temporal evolution of the number concentration of the nanoparticles inside the flames. NOC particles, which are rapidly produced in locally rich combustion regions, have peculiar properties since their sticking coefficient both for coagulation and adhesion result to be orders of magnitudes lower than that expected by larger aerosols, like soot particles. The experimental results are interpreted by modelling the van der Waals interactions of the nanoparticles in terms of Lennard-Jones potentials and in the framework of the gas kinetic theory. The estimated adhesion and coagulation efficiencies are in good agreement with those calculated from AFM and optical data. The very low efficiency values observed for the smaller particles could be ascribed to the high energy of these particles due to their Brownian motion, which causes thermal rebound effects prevailing over adhesion mechanisms due to van der Waals forces.     

Measurements of flame orientation and scalar dissipation in turbulent partially premixed methane flames

Three turbulent flames were studied using a new experimental facility developed at Sandia National Laboratories. Line imaging of Raman and Rayleigh scattering and CO laser-induced fluorescence (LIF) yielded information on all major species, temperature, mixture fraction, and a 1D surrogate measure of scalar dissipation. Simultaneously, crossed planar OH LIF imaging provided information on the instantaneous flame orientation, allowing estimation of the full 3D (flame-normal) scalar dissipation rate. The three flames studied were methane–air piloted jet flames (Sandia flames C, D, and E), which cover a range in Reynolds number from 13,400 to 33,600. The statistics of the instantaneous flame orientation are examined in the different flames, with the purpose of studying the prevailing kinematics of isoscalar contours. The 1D and 3D results for scalar dissipation rate are examined in detail, both in the form of conditional averages and in the form of probability density functions. The effect of overall strain and Reynolds number on flame suppression and eventual extinction is also investigated, by examining the doubly conditional statistics of temperature in the form of S-shaped curves. This latter analysis reveals that double conditioning of temperature on both mixture fraction and scalar dissipation does not collapse the data from these flames onto the same curve at low scalar dissipation rates, as might be expected from simple flamelet concepts.     

The two-dimensional structure of low strain rate counterflow nonpremixed-methane flames in normal and microgravity

The structure and extinction of low strain rate nonpremixed methane–air flames was studied numerically and experimentally. A time-dependent axisymmetric two-dimensional (2D) model considering buoyancy effects and radiative heat transfer was developed to capture the structure and extinction limits of normal gravity (1-g) and zero gravity (0-g) flames. For comparison with the 2D modelling results, a one-dimensional (1D) flamelet computation using a previously developed numerical code was exercised to provide information on the 0-g flames. A 3-step global reaction mechanism was used in both the 1D and 2D computations to predict the measured extinction limit and flame temperature. Photographic images of flames undergoing the process of extinction were compared with model calculations. The axisymmetric numerical model was validated by comparing flame shapes, temperature profiles, and extinction limits with experiments and with the 1D computational results. The 2D computations yielded insight into the extinction mode and flame structure. A specific maximum heat release rate was introduced to quantify the local flame strength and to elucidate the extinction mechanism. The contribution by each term in the energy equation to the heat release rate was evaluated to investigate the multi-dimensional structure and radiative extinction of the 1-g flames. Two combustion regimes depending on the extinction mode were identified. Lateral heat loss effects and multi-dimensional flame and flow structure were also found. At low strain rates in 1-g flames (‘regime A’), the flame is extinguished from the weak outer edge of the flame, which is attributed to a multi-dimensional flame structure and flow field. At high strain rates, (‘regime B’), the flame extinction initiates near the flame centreline owing to an increased diluent concentration in the reaction zone, similar to the extinction mode of 1D flames. These two extinction modes can be clearly explained by consideration of the specific maximum heat release rate.     

Appearances of internal micro bubbling, multiple micro explosions, multiple micro jets and micro diffusion flames around an abruptly heated micro plastic-resin particle

Heating, gasifying and burning processes of a micro plastic-resin particle, which has a diameter of about 200 μm and is suddenly exposed to a hot oxidizing atmosphere, are observed and optically processed by combining a micro schlieren system with a high-speed CCD video camera. The following three devised approaches are introduced: the use of an oxidizing combustion gas downstream of a spark-ignited propane–air lean premixed flame as a sudden heat source, the use of a spherically reformed micro particle on a fine tungsten wire of 5 μm diameter, and the use of a simultaneous direct and schlieren optical system. The first technique realizes slow heating and enables a micro resin particle to undergo the same circumstances as those experienced by plastic-resin particles in the plastic-resin powder combustion. The second approach improves the accuracy and reproducibility of image processing, whereas the third optical system gives simultaneous pictures of the transparent visible image and the schlieren image around a micro resin particle of one heating process. The results show that there exists intense multiple internal bubbling, multiple micro explosions, multiple micro jets and micro diffusion flames, and that their existence exerts strong influences on gasification characteristics of a micro resin particle and results in a high burning rate constant.     

Simultaneous PIV/PTV/OH PLIF imaging: Conditional flow field statistics in partially premixed turbulent opposed jet flames

A combination of particle imaging velocimetry (PIV), particle tracking velocimetry (PTV) and planar laser-induced fluorescence (PLIF) was employed to measure conditional flow field statistics in partially premixed turbulent opposed jet flames. These flames were observed to be very sensitive to excessive seeding of particles. Since flames close to extinction were studied, very low seeding densities were required to prevent impact on the extinction behavior of the flame, and conventional PIV algorithms would have resulted in poor spatial resolution. An improved PIV algorithm was developed, in connection with a PTV procedure used in high-temperature regions of low seed density, and revealed high in-plane resolution up to 300 μm. The PIV/PTV algorithm slightly under-resolved the Kolmogorov scales for the present cases, whereas Batchelor scales were fully resolved in-plane by the simultaneous OH PLIF. In the data processing, transient OH contours obtained from single-shots were used to define flame-fixed coordinates. Conditional velocities, out-of-plane vorticity, 2D dilatation, and both axial and radial strain were processed from the data. The conditional statistics show that vorticity is preferably generated close to the reaction zone, particularly at off-centerline positions. Hence, flow-chemistry interactions could be identified directly in the region of the reaction zone. This finding was also supported by qualitative high speed Mie scattering/chemiluminescence imaging that permitted temporally resolved visualization of the formation of eddies just upstream of the luminous flame areas.     

Numerical investigation of pulverized coal particle group combustion using tabulated chemistry

The ignition and combustion of coal particle groups are investigated numerically in a laminar flow reactor. The Flamelet Generated Manifold method is extended to account for the complex mixture of gases being released during devolatilization, which is calculated with a competing two-step model. A second mixture fraction is introduced to include the mixing with the second methane fuel stream. The interactions of the gas phase with particles are modeled within a fully coupled Euler-Lagrange framework. To investigate the influence of particle groups on ignition and combustion, successively increasing densities of particle streams have been analyzed. The ignition delay time is increased significantly by higher particle densities. This delay is validated successfully with the available measurements. Moreover, the shape of the volatile flame was found to be strongly influenced by the particle number density inside the flame. A transition from spherical flames around single particles to a conical flame around the particle cloud could be found in numerical results as well as in experiments. As the primary mechanism for the substantial ignition delay and the formation of the flame, the increased heat transfer from the gas-phase to the particle group, resulting in lower gas-phase temperatures, was identified.     

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.     

A computational study of soot formation and flame structure of coflow laminar methane/air diffusion flames under microgravity and normal gravity

A numerical study is conducted of methane–air coflow diffusion flames at microgravity (μg) and normal gravity (1g), and comparisons are made with experimental data in the literature. The model employed uses a detailed gas phase chemical kinetic mechanism that includes PAH formation and growth, and is coupled to a sectional soot particle dynamics model. The model is able to accurately predict the trends observed experimentally with reduction of gravity without any tuning of the model for different flames. The microgravity sooting flames were found to have lower temperatures and higher volume fraction than their normal gravity counterparts. In the absence of gravity, the flame radii increase due to elimination of buoyance forces and reduction of flow velocity, which is consistent with experimental observations. Soot formation along the wings is seen to be surface growth dominated, while PAH condensation plays a more major role on centreline soot formation. Surface growth and PAH growth increase in microgravity primarily due to increases in the residence time inside the flame. The rate of increase of surface growth is more significant compared to PAH growth, which causes soot distribution to shift from the centreline of the flame to the wings in microgravity.     

Particle formation in opposed-flow diffusion flames of ethylene: An experimental and numerical study

An experimental and numerical study on particles inception and growth is performed in opposed-flow diffusion flames of ethylene and air characterized by different sooting tendencies. Spectrally resolved UV-visible laser induced fluorescence, laser induced incandescence and laser light scattering measurements are used to characterize different classes of combustion-generated compounds. A detailed kinetic model accounting for both gas-phase and particle formation is used. Comparison between experimental results and numerical predictions gives a qualitative view of the mechanism of particle formation in opposed-flow flames.Particle inception is the result of both chemical growth and coagulation of aromatic compounds. In the region close to the flame front where the temperature is relatively high and radicals are abundant, the particle inception is due to a chemical growth mechanism by which aromatic molecules add aromatic radicals leading to the formation of biphenyl-like structures. The growth process continues as high-molecular mass aromatics are moved away from the flame zone towards the stagnation plane by the addition of acetylene and other aromatics forming particles of increasing sizes. Graphitization of these particles and thermal annealing lead to the formation of soot particles. At relatively lower temperatures, found across the stagnation plane, particles growth still occurs and it is mainly due to a process of physical coagulation of PAHs.The experimental and numerical results obtained in this work demonstrate and explain the sensibility of inception and growth of particles to radical concentration and temperature in opposed-flow flame configurations.     

Flame studies of C2 hydrocarbons

The oxidation characteristics of C₂ hydrocarbons were revisited in flames established in the counterflow configuration. Laminar flame speeds of ethane/air, ethylene/air, and acetylene/oxygen/nitrogen mixtures as well as extinction strain rates of non-premixed ethane/air flames were measured using digital particle image velocimetry. The experiments were modeled using three different kinetic models. While the experimental and computed laminar flame speeds agreed closely for all C₂ hydrocarbons under fuel-lean conditions, notable discrepancies were identified under fuel-rich conditions. Using the computed flame structures, insight was provided into the controlling mechanisms that could be responsible for the observed discrepancies. More specifically, the uncertainties associated with the kinetics of the thermal decomposition of the ethyl radical were found to be a potential source of the observed discrepancies for ethane flames. It was shown also by using alternative rate constants for the ethyl radical decomposition, the rate of flame propagation and the extinction propensity are affected notably. Furthermore, the values of the branching ratio of acetylene consumption reactions involving atomic oxygen were found to have a significant effect on the propagation of rich acetylene flames.     

Numerical study of the effects of gravity on soot formation in laminar coflow methane/air diffusion flames under different air stream velocities

Numerical simulations of laminar coflow methane/air diffusion flames at atmospheric pressure and different gravity levels were conducted to gain a better understanding of the effects of gravity on soot formation by using relatively detailed gas-phase chemistry and complex thermal and transport properties coupled with a semi-empirical two-equation soot model. Thermal radiation was calculated using the discrete-ordinates method coupled with a non-grey model for the radiative properties of CO, CO₂, H₂O, and soot. Calculations were conducted for three coflow air velocities of 77.6, 30, and 5 cm/s to investigate how the coflowing air velocity affects the flame structure and soot formation at different levels of gravity. The coflow air velocity has a rather significant effect on the streamwise velocity and the fluid parcel residence time, especially at reduced gravity levels. The flame height and the visible flame height in general increase with decreasing the gravity level. The peak flame temperature decreases with decreasing either the coflow air stream velocity or the gravity level. The peak soot volume fraction of the flame at microgravity can either be greater or less than that of its normal gravity counterpart, depending on the coflow air velocity. At sufficiently high coflow air velocity, the peak soot volume fraction increases with decreasing the gravity level. When the coflow air velocity is low enough, soot formation is greatly suppressed at microgravity and extinguishment occurs in the upper portion of the flame with soot emission from the tip of the flame owing to incomplete oxidation. The numerical results provide further insights into the intimate coupling between flame size, residence time, thermal radiation, and soot formation at reduced gravity level. The importance of thermal radiation heat transfer and coflow air velocity to the flame structure and soot formation at microgravity is demonstrated for the first time.     

Structure of propagating edge diffusion flames in hydrocarbon fuel jets

Direct numerical simulations with a C₃-chemistry model have been performed to investigate the transient behavior and internal structure of flames propagating in an axisymmetric fuel jet of methane, ethane, ethylene, acetylene, or propane in normal earth gravity (1g) and zero gravity (0g). The fuel issued from a 3-mm-i.d. tube into quasi-quiescent air for a fixed mixing time of 0.3 s before it was ignited along the centerline where the fuel–air mixture was at stoichiometry. The edge of the flame formed a vigorously burning peak reactivity spot, i.e., reaction kernel, and propagated through a flammable mixture layer, leaving behind a trailing diffusion flame. The reaction kernel broadened laterally across the flammable mixture layer and possessed characteristics of premixed flames in the direction of propagation and unique flame structure in the transverse direction. The reaction kernel grew wings on both fuel and air sides to form a triple-flame-like structure, particularly for ethylene and acetylene, whereas for alkanes, the fuel-rich wing tended to merge with the main diffusion flame zone, particularly methane. The topology of edge diffusion flames depend on the properties of fuels, particularly the rich flammability limit, and the mechanistic oxidation pathways. The transit velocity of edge diffusion flames, determined from a time series of calculated temperature field, equaled to the measured laminar flame speed of the stoichiometric fuel–air mixtures, available in the literature, independent of the gravity level.     

Experimental low-stretch gaseous diffusion flames in buoyancy-induced flowfields

The present study experimentally investigates the structure and instabilities associated with extremely low-stretch (1 s⁻¹) gaseous diffusion flames. Ultra-low-stretch flames are established in normal gravity by bottom burning of a methane/nitrogen mixture discharged from a porous spherically symmetric burner of large radius of curvature. OH-PLIF and IR imaging techniques are used to characterize the reaction zone and the burner surface temperature, respectively. A flame stability diagram mapping the response of the ultra-low-stretch diffusion flame to varying fuel injection rate and nitrogen dilution is explored. In this diagram, two main boundaries are identified. These boundaries separate the stability diagram into three regions: sooting flame, non-sooting flame, and extinction. Two distinct extinction mechanisms are noted. For low fuel injection rates, flame extinction is caused by heat loss to the burner surface. For relatively high injection rates, at which the heat loss to burner surface is negligible, flame radiative heat loss is the dominant extinction mechanism. There also exists a critical inert dilution level beyond which the flame cannot be sustained. The existence of multi-dimensional flame phenomena near the extinction limits is also identified. Various multi-dimensional flame patterns are observed, and their evolutions are studied using direct chemiluminescence and OH-PLIF imaging. The results demonstrate the usefulness of the present burner configuration for the study of low-stretch gaseous diffusion flames.     

Evidence for the transition from the diffusion-limit in aluminum particle combustion

This work presents experimental evidence that the transition from gas-phase diffusion-limited combustion for aluminum particles begins to occur at a particle size of 10 μm at a pressure of 8.5 atm. Measurements of the particle temperature by AlO spectroscopy and three-color pyrometry indicate that the peak temperature surrounding a burning particle approaches the aluminum boiling temperature as particle size is decreased to 10 μm when oxygen is the oxidizer. This reduction indicates that reactions are occurring at or near the particle surface rather than in a detached diffusion flame. When CO₂ is the oxidizer, the combustion temperatures remain near the aluminum boiling temperature for particles as large as 40 μm, indicating that the flame is consistently near the surface throughout this size range. Burn time measurements of 10 and 2.8 μm powders indicate that burn time is roughly proportional to particle diameter to the first power. The burn rates of micron- and nano-particles also show strong pressure dependence. These measurements all indicate that the combustion has deviated from the vapor-phase diffusion limit, and that surface or near-surface processes are beginning to affect the rate of burning. Such processes would have to be included in combustion models in order to accurately predict burning characteristics for aluminum with diameter less than 10 μm.     

Soot particle size distribution measurements in a turbulent ethylene swirl flame

There is a need to better understand particle size distributions (PSDs) from turbulent flames from a theoretical, practical and even regulatory perspective. Experiments were conducted on a sooting turbulent non-premixed swirled ethylene flame with secondary (dilution) air injection to investigate exhaust and in-burner PSDs measured with a Scanning Mobility Particle Sizer (SMPS) and soot volume fractions (f_v) using extinction measurements. The focus was to understand the effect of systematically changing the amount and location of dilution air injection on the PSDs and f_v inside the burner and at the exhaust. The PSDs were also compared with planar Laser Induced Incandescence (LII) calibrated against the average f_v. LII provides some supplemental information on the relative soot amounts and spatial distribution among the various flow conditions that helps interpret the results. For the flame with no air dilution, f_v drops gradually along the centreline of the burner towards the exhaust and the PSD shows a shift from larger particles to smaller. However, with dilution air f_v reduces sharply where the dilution jets meet the burner axis. Downstream of the dilution jets f_v reduces gradually and the PSDs remain unchanged until the exhaust. At the exhaust, the flame with no air dilution shows significantly more particles with an f_v one to two orders of magnitude greater compared to the Cases with dilution. This dataset provides insights into soot spatial and particle size distributions within turbulent flames of relevance to gas turbine combustion with differing dilution parameters and the effect dilution has on the particle size. Additionally, this work measures f_v using both ex situ and in situ techniques, and highlights the difficulties associated with comparing results across the two. The results are useful for validating advanced models for turbulent combustion.     

Premixed turbulent flame front structure investigation by Rayleigh scattering in the thin reaction zone regime

Premixed turbulent flames of methane–air and propane–air stabilized on a bunsen type burner were studied using planar Rayleigh scattering and particle image velocimetry. The fuel–air equivalence ratio range was from lean 0.6 to stoichiometric for methane flames, and from 0.7 to stoichiometric for propane flames. The non-dimensional turbulence rms velocity, u′/S_L, covered a range from 3 to 24, corresponding to conditions of corrugated flamelets and thin reaction zones regimes. Flame front thickness increased slightly with increasing non-dimensional turbulence rms velocity in both methane and propane flames, although the flame thickening was more prominent in propane flames. The probability density function of curvature showed a Gaussian-like distribution at all turbulence intensities in both methane and propane flames, at all sections of the flame.The value of the term Dκ, the product of molecular diffusivity evaluated at reaction zone conditions and the flame front curvature, has been shown to be smaller than the magnitude of the laminar burning velocity. This finding questions the validity of extending the level set formulation, developed for corrugated flames region, into the thin reaction zone regime by increasing the local flame propagation by adding the term Dκ to laminar burning velocity.     

Combustion of bimodal nano/micron-sized aluminum particle dust in air

The combustion of bimodal nano/micron-sized aluminum particles with air is studied both analytically and experimentally in a well-characterized laminar particle-laden flow. Experimentally, an apparatus capable of producing Bunsen-type premixed flames was constructed to investigate the flame characteristics of bimodal-particle/air mixtures. The flame speed is positively affected by increasing the mass fraction of nano particles in the fuel formulation despite the lower flame luminosity and thicker flame zone. Theoretically, the flames are assumed to consist of several different regimes for fuel-lean mixture, including the preheat, flame, and post flame zones. The flame speed and temperature distribution are derived by solving the energy equation in each regime and matching the temperature and heat flux at the interfacial boundaries. The analysis allows for the investigation of the effects of particle composition and equivalence ratio on the burning characteristics of aluminum-particle/air mixtures. Reasonable agreement between theoretical results and experimental data was obtained in terms of flame speed. The flame structure of a bimodal particle dust cloud may display either an overlapping or a separated configuration, depending on the combustion properties of aluminum particles at different scales. At low percentages of nano particles in the fuel formulation, the flame exhibits a separated spatial structure with a wider flame regime. At higher nano-particle loadings, overlapping flame configurations are observed.     

Evaluation of a flamelet/progress variable approach for pulverized coal combustion in a turbulent mixing layer

A steady flamelet/progress variable (FPV) approach for pulverized coal flames is employed to simulate coal particle burning in a turbulent shear and mixing layer. The configuration consists of a carrier-gas stream of air laden with coal particles that mixes with an oxidizer stream of hot products from lean combustion. Carrier-phase DNS (CP-DNS) are performed, where the turbulent flow field is fully resolved, whereas the coal is represented by Lagrangian point particles. CP-DNS with direct chemistry integration is performed first and provides state-of-the-art validation data for FPV modeling. In a second step the control variables for FPV are extracted from the CP-DNS and used to test if the tabulated manifold can correctly describe the reacting flow (a priorianalysis). Finally a fully coupled a posteriori FPV simulation is performed, where only the FPV control variables are transported, and the chemical state is retrieved from the table and fed back to the flow solver. The a priori results show that the FPV approach is suitable for modeling the complex reacting multiphase flow considered here. The a posteriori data is similarly in good agreement with the reference CP-DNS, although stronger deviations than a priori can be observed. These discrepancies mainly appear in the upper flame (of the present DNS), where premixing and highly unsteady extinction and re-ignition effects play a role, which are difficult to capture by steady non-premixed FPV modeling. However, the present FPV model accurately captures the lower, more stable flame that burns in non-premixed mode.