Flame Soot Research Articles

Characteristics of turbulent flames in a confined and pressurised jet-in-hot-coflow combustor

Combustion in hot and low oxygen environments—such as those encountered in practical devices including inter-turbine burners and sequential gas turbines—is not yet fully understood at a fundamental level, particularly in terms of the effects of pressure. To meet this gap in understanding, a confined-and-pressurised jet-in-hot-coflow (CP-JHC) combustor has been developed to facilitate optical diagnostics of turbulent flames in hot and vitiated coflows for the studies of flame stabilisation, structure and soot formation at elevated pressures. The CP-JHC burner has been designed for steady operation at 10 bar with internal temperatures of up to 1975 K, with a water-cooled central jet issuing into a hot oxidant stream of combustion products from a non-premixed natural gas/H2 burner. This work describes the key features and operational capabilities of the CP-JHC burner and presents a selection of experimental results showing characteristics not previously available. Specifically, temperature measurements of the hot coflow are used to estimate the enthalpy deficit of the stream, revealing an increase in thermal efficiency with increasing heat input, and a decrease with increasing pressure. Chemiluminescence imaging of OH∗ and CH∗ is performed for turbulent jet flames to study the flame structure under various operating conditions, and true-colour imaging results are also included to highlight the change in soot formation under elevated pressures. The mean images indicate a change in stabilisation behaviour with changes in pressure and jet Reynolds number (Rejet), which is further investigated by a statistical analysis of the short-exposure CH∗ images. This analysis reveals that an increase in Rejet from 10,000 to 15,000 leads to an increase in the mean lift-off height (from the jet exit plane) from approximately 1.5 to 6 jet diameters at atmospheric pressure, while the flames at elevated pressures show significantly less variation and tend to stabilise at the jet exit for P > 3.5 bar(a). The experimental findings are complemented by numerical simulations of laminar opposed flow flames, providing additional insights into the fundamental chemical kinetics effects which influence these flames. In particular, a monotonic reduction in both the maximum and integrated OH∗ and CH∗ mass fractions is observed with increasing pressure. This reduction is particularly pronounced at lower pressures, with a reduction to 10% of the atmospheric-pressure value at 3 bar(a) for the integrated OH∗ mass fraction. Additionally, this behaviour is shown to be related to the combined effects of a shift in the formation pathways and the increased impact of collisional quenching.

The effects of 1-methylnaphthalene addition to n-dodecane on the formation of soot and polycyclic aromatic hydrocarbons in laminar coflow diffusion flames

1-Methylnaphthalene (1-MN) is a typical diaromatic component in petroleum-based fuels and has been widely chosen to represent aromatic fractions in surrogate fuels of diesel and jet fuels. In this study, experimental and modeling studies were performed to investigate the formation of typical polycyclic aromatic hydrocarbons (PAHs) and soot in coflow methane/air diffusion flames doped with 1-methylnaphthalene/n-dodecane mixtures, and explore chemical effects of 1-methylnaphthalen on key soot formation steps. The laser-induced incandescence (LII) and laser-induced fluorescence (LIF) techniques were used to obtained the soot volume fraction and relative concentration of typical PAHs along the flame centerline, respectively. A novel apparatus-independent indicator, yield aromatic index (YAI), was first proposed to quantify the formation tendency of a specific aromatic product in a flame. It can be found that the addition of 1-methylnaphthalene in the fuel mixtures has a significantly promoting effect on soot formation processes. The correlation between the mass fraction of 1-methylnaphthalene and sooting tendency shows a strong linear relationship. As to the PAH formation tendency, YAIA2R5 have the smaller deviations from corresponding YSIs than YAIA2&A3 and YAIA4, which indicating that A2R5 can be a type of important species leading to soot inception and have strong contribution to soot formation. Through the chemical kinetic analysis, A2R5 is proved to be a key coupling point of two A4 formation pathways, which start from n-dodecane and 1-methylnaphthalene, respectively. As a small amount of 1-methylnaphthalene is introduced into the fuel, the dominant approach to A2R5 rapidly shifts to a more efficient pathway, and is continually enhanced with increasing 1-methylnaphthalene at a moderate trend. The results reveal that 1-methylnaphthalene in the fuel can stride over the rate limiting step of the soot formation process of non-aromatic fuels, eventually leading to an obviously increasing sooting tendency. This study aims to provide useful information for the development of soot nucleation mechanisms and the control of soot formation processes.

Experimental investigation of soot formation in inverse diffusion flames of CO2 and N2 addition: Isolation of dilution and thermal effects

ABSTRACT This experimental study compares the flame structure, temperature, and soot formation characteristics of normal (NDFs) and inverse diffusion flames (IDFs), evaluates the effect of CO2 addition, and isolates the thermal and dilution effects of CO2 and N2 addition on soot formation in IDFs. A hyperspectral imager using the TR-GSVD algorithm measures IDFs with different CO2 addition (XD) in the oxidant, with N2 addition as the comparison. In contrast to NDFs, IDFs have an opened tip, and the visible flame height and flame width decrease as XD grows. IDFs have a higher peak temperature than NDFs, but their peak soot volume fraction is substantially lower. Compared with N2 addition at the same XD, CO2 addition narrows IDFs and makes the reaction zone visible, and the peak temperature of CO2 addition is 350 K lower than that of N2 addition. The suppression effect of CO2 on soot formation is more potent than N2, with a soot formation rate of 30% that of N2 addition and a soot loading of 20–60%. The activation energy of soot formation reaction with CO2 addition is higher than N2 addition. The isolating results reveal that the thermal effect contributes to the main suppression effect of CO2 addition on soot formation, while the dilution effect of N2 addition is stronger than its thermal effect.

Effect of wall parameters on impinging combustion and soot emission characteristics of heavy-duty diesel engine at low temperature

The effect of wall parameters on combustion and soot emission characteristics remains to be revealed so far, especially in the case of spray impingement at low temperatures. Therefore, the visualization experiments are carried out in a constant volume combustion chamber using the Mie scattering and direct photography techniques, and the two-color method was used to extract the flame temperature and soot volume. The results show that increased wall distance and wall angle contribute to fast and stable ignition, but result in more soot production. In addition, the lower the ambient temperature, the more prominent the above characteristics are. At Tamb = 820 K, as the wall distance increases from 40 mm to 60 mm, the liquid spray impingement changes to the vapor impingement, so the ignition delay shortens, and the flame area and natural luminance increase significantly. At lower Tamb = 770 K, a complete misfire is observed at Lw = 40 mm but the ignition remains stable at Lw = 60 mm. The variation of the ignition characteristic parameters with the wall angle is similar to that of the wall distance. Under Pinj = 40 MPa, as the wall angle increases from 0° to 70°, the time to reach luminance saturation advances from 0.60 ms to 0.27 ms. Under higher Pinj = 100 MPa, a complete misfire occurs at θ =0° but bright flames are observed at θ =30–70°. With the increase of wall distance, the mean flame temperature increases due to reduced wall cooling. Coupled with the expanded flame area and combustion duration, the high-temperature region (>1800K) of soot distribution and KL factor increase significantly, especially in the range of Lw = 40–50 mm.

Soot particle size distribution reconstruction in a turbulent sooting flame with the split-based extended quadrature method of moments

The Method of Moments (MOM) has largely been applied to investigate sooting laminar and turbulent flames. However, the classical MOM is not able to characterize a continuous particle size distribution (PSD). Without access to information on the PSD, it is difficult to accurately take into account particle oxidation, which is crucial for shrinking and eliminating soot particles. Recently, the Split-based Extended Quadrature Method of Moments (S-EQMOM) has been proposed as a numerically robust alternative to overcome this issue [Salenbauch et al., “A numerically robust method of moments with number density function reconstruction and its application to soot formation, growth, and oxidation,” J. Aerosol Sci. 128, 34–49 (2019)]. The main advantage is that a continuous particle number density function can be reconstructed by superimposing kernel density functions (KDFs). Moreover, the S-EQMOM primary nodes are determined individually for each KDF, improving the moment realizability. In this work, the S-EQMOM is combined with a large eddy simulation/presumed-probability density function flamelet/progress variable approach for predicting soot formation in the Delft Adelaide Flame III. The target flame features low/high sooting propensity/intermittency and comprehensive flow/scalar/soot data are available for model validation. Simulation results are compared with the experimental data for both the gas phase and the particulate phase. Good quantitative agreement has been obtained especially in terms of the soot volume fraction. The reconstructed PSD reveals predominantly unimodal/bimodal distributions in the first/downstream portion of this flame with particle diameters smaller than 100 nm. By investigating the instantaneous and statistical sooting behavior at the flame tip, it has been found that the experimentally observed soot intermittency is linked to mixture fraction fluctuations around its stoichiometric value that exhibits a bimodal probability density function.

Comprehensive optical diagnostics for flame behavior and soot emission response to a non-equilibrium plasma

This study reported comprehensive optical diagnostics for flame behavior and soot emission under directly coupling of the plasma with the flame at specific heights. The morphometric parameters of unstable flames under the direct plasma coupling were quantified. We also proposed an optical method to eliminate plasma luminescence from the field of view to extract flame intensity. At the same discharge height, with the increase of discharge frequency, the flame height decreased, while the flame horizontal extension distance and deflection angle increased. The relationships between flame morphologic and electrical parameters were obtained. The experimental results suggested a one-to-one correspondence between plasma action and flame deflection or shortening. When the plasma interacted with the flame, the overall temperature and soot emission of the flame decreased compared with that without plasma. At the same discharge height, the flame temperature and soot decreased further with the increase of discharge frequency. The soot emission changed more remarkably with the discharge frequency for higher discharge heights. With the increase of voltage, the flame temperature and soot increased at the lower discharge heights. The analysis of the experiment data demonstrated that the variation of soot emission was caused by the cooperation of multiple factors.

Relative errors in derived multi-wavelength intensive aerosol optical properties using cavity attenuated phase shift single-scattering albedo monitors, a nephelometer, and tricolour absorption photometer measurements

Abstract. Aerosol intensive optical properties, including Ångström exponents for aerosol light extinction (EAEs), scattering (SAEs) and absorption (AAEs) as well as and the single-scattering albedo (SSA), are indicators for aerosol size, chemical composition, radiative behaviour and particle sources. Derivation of these parameters requires the measurement of aerosol optical properties at multiple wavelengths, which usually involves the use of several instruments. Our study aims to quantify the uncertainties in the determination of these intensive properties using an optical closure approach. In our laboratory closure study, we measured the full set of optical properties for a range of light-absorbing particles with different properties externally mixed with ammonium sulfate to generate aerosols with controlled SSA values. The investigated absorbing particle types were fresh combustion soot emitted by an inverted flame soot generator (SOOT; fractal agglomerates), Aquadag (AQ; compact aggregates), Cabot black (BC; compact agglomerates) and an acrylic paint (magic black, shape unknown). The instruments used in this study were two cavity attenuated phase shift particle monitors for single-scattering albedo (CAPS PMSSA's; λ=450, 630 nm) for measuring light-extinction and light-scattering coefficients, one integrating nephelometer (λ=450, 550, 700 nm) for light-scattering coefficients, and one tricolour absorption photometer (TAP; λ=467, 528, 652 nm) for filter-based light-absorption coefficients. One key finding is that the coefficients of light absorption, scattering and extinction derived from combing the measurements of two independent instruments agree with measurements from single instruments; the slopes of regression lines are equal within reported uncertainties (i.e. closure is observed). Despite closure for measured absorption coefficients, we caution that the estimated uncertainties for absorption coefficients, propagated for the differential method (DM; absorption = extinction minus scattering), can exceed 100 % for atmospherically relevant SSA values (>0.9). This increasing estimated uncertainty with increasing SSA yields AAE values that may be too uncertain for measurements in the range of atmospheric aerosol loadings. We recommend using the DM for measuring AAE values when the SSA < 0.9. EAE- and SAE-derived values achieved closure during this study within stated uncertainties for extinction coefficients greater than 15 Mm−1. SSA values for 450 and 630 nm wavelengths internally agreed with each other within 10 % uncertainty for all instrument combinations and sampled aerosol types, which fulfils the defined goals for measurement uncertainty of 10 % proposed by Laj et al. (2020) for GCOS (Global Climate Observing System) applications.

Raman Spectroscopy of Nascent Soot Oxidation: Structural Analysis During Heating

The effect of oxidation on nascent soot particles is investigated in this work by means of Raman spectroscopy. Three different soot particle samples are produced in a lightly sooting ethylene/air laminar premixed flame and collected at different residence times. The samples are characterized by a different size of primary particles and a different degree of aging and hence graphitization, and they are representative of the early evolution of nascent soot in flames. Oxidation of particles is induced by exposing the samples to a high temperature oxidation treatment in air over a range of temperature 25–500°C. To this aim, a programmable heating microscope stage is used. Thermo-optical transmission (TOT) measurements are used to characterize the chemical composition of pristine particles in terms of organic and elemental carbon content, also providing the pyrolytic carbon fraction of the organic carbon. The TOT results show that the organic fraction is constant for the three conditions. On the other hand, the pyrolytic carbon fraction decreases and the elemental carbon increases when moving from the sample composed of just-nucleated particles to the sample mostly made of mature soot particles. Raman spectroscopy reveals that the thermal oxidation treatment performed on the sample of just-nucleated particles, with the highest organic carbon content, results in a reduction of the amorphous carbon component. Conversely, the sample of mature soot, with the highest elemental carbon content, shows an increase in the amorphous carbon phase after oxidation, which is attributed to fragmentation or the formation of point defects by O2 oxidation. Finally, the thermal oxidation procedure produces a strong reduction in the photoluminescence signal detected from Raman spectra.

Predicting simultaneously fields of soot temperature and volume fraction in laminar sooting flames from soot radiation measurements - a convolutional neural networks approach.

An original convolutional neural network, i.e. U-net approach, has been designed to retrieve simultaneously local soot temperature and volume fraction fields from line-of-sight measurements of soot radiation fields. A five-stage U-net architecture is established and detailed. Based on a set of N2 diluted ethylene non-premixed flames, the minimum batch size requirement for U-net model training is discussed and the U-net model prediction ability is validated for the first time by fields provided by the modulated absorption emission (MAE) technique documenting the N2 diluted flame. Additionally, the U-net model's flexibility and robustness to noise are also quantitatively studied by introducing 5% & 10% Gaussian random noises into training together with the testing data. Eventually, the U-net predictive results are directly contrasted with those of Bayesian optimized back propagation neural network (BPNN) in terms of testing score, prediction absolute error (AE), soot parameter field smoothness, and time cost.

Evaluation of in-cylinder endoscopic two-colour soot pyrometry of diesel combustion

Flame temperature and soot concentration imaging was performed using endoscopic two-colour (2C) soot pyrometry to investigate the characteristics of in-cylinder diesel engine combustion processes and provide validation data for engine simulation and design. To appropriately interpret the 2C image results, this paper focuses on the uncertainty and challenges of the technique, the line-of-sight nature of the measurement and presents comparable information for validation exercises. A line-of-sight flame light intensity model was created to explore how the temperature T and soot concentration KL measured by the 2C technique can relate to non-uniform flame temperature and soot distributions. It was found that T and KL measured from the 2C technique were likely to relate differently to the actual distribution depending on where in the flame the measurement was taken and on assumptions made about the flame spatial structure. Assessment has been made of the range of the maximum and minimum flame temperatures (assumed to correspond to reaction zone temperature and flame centreline respectively) that are consistent with measured temperature T and soot concentration KL. The analysis of uncertainties, flame temperature and soot distribution along the line-of-sight, and image averaging allows for better quantitative comparison of 2C soot pyrometry images to CFD simulation, which increases confidence in simulation-driven engine development.

Experimental investigation of the effect of hydrogen addition on the sooting limit and structure of methane/air laminar counterflow diffusion flames

The influence of hydrogen (H2) addition on the sooting limit and structure of methane/air laminar counterflow diffusion flames has been studied. Soot limits have been obtained using the laser light scattering technique for CH4/H2 mixtures with H2 concentration varying from 0–20% by volume in the fuel mixture for different strain rates. The resulting soot limit map shows a significant increase in the fuel concentration at the soot limit with increasing amounts of H2. To understand this trend, temperature and species concentration profiles have been measured and compared under the influence of H2 addition in (a) an incipiently sooting and (b) in a sooting CH4/air flame. Flame temperatures have been measured using a thin-wire S-type thermocouple and species profiles have been measured using the gas chromatography technique (GC). The results indicate a significant decrease in the amounts of higher hydrocarbons such as benzene and naphthalene (which are considered important soot precursors) with an increase in H2 concentration for the sooting flame. To explain this decrease in the concentration of higher hydrocarbons, pathway analysis has been performed to elucidate the influence of H2 on the formation and consumption of soot forming species.

Bio‐waste derived carbon nano‐onions as an efficient electrode material for symmetric and lead‐carbon hybrid ultracapacitors

Carbon and metal oxide nanocomposites have been extensively studied as electrode materials to develop energy and power-dense supercapacitors in recent years. Nevertheless, nano carbons with improved porosity and functional moieties are the most eco-friendly and cost-effective supercapacitor materials. In this work, carbon nano-onions (CNOs) synthesized by a single-step flame soot collection method, subsequently calcined at 600°C in an inert environment (CNO-600), are used as electrode material for the supercapacitors. CNO-600 s have a layer-by-layer nano onion structure with a ~25 nm particle size and a Brunauer–Emmett–Teller surface area of 147 m2 g−1. CNO-600 delivers 266 and 186 F g−1 of capacitance at 0.5 A g−1 for half cells and symmetric ultracapacitors, respectively. Ultracapacitors show capacitance retention of 91% with 20 000 GCD cycles in 1 M H2SO4 electrolyte. The stable capacitance of CNO-600 is due to easy intercalation/de-intercalation of electrolyte ions and electrons in the layer-by-layer structure of CNOs, contributing to pseudocapacitive charge storage with electric double layer capacitor behavior. The lead-carbon hybrid ultracapacitor fabricated using CNO-600 as anode material and PbO2 as cathode delivers a specific capacitance of 515 F g−1 at 1 A g−1 in 4.5 M H2SO4 electrolyte in the voltage range of 2.3 and 0.6 V. The substantial improvement of charge storage in CNO-based symmetric and lead-carbon hybrid system, demonstrate an excellent opportunity for the development of high-performance supercapacitors.

Experimental and numerical investigation of the transition from non sooting to sooting premixed n-butane flames, encompassing the nucleation flame conditions

In a small range of rich equivalence ratios, premixed flat flames, so-called nucleation flames, were shown to produce very small-size (2–4 nm) soot particles, which undergo negligible growth with the residence time. In such flames, the contribution of the soot nucleation step with respect to the soot growth process is larger than in standard sooting flames, making nucleation flames ideal target flames to better understand the inception process. In order to scrutinize the transition from non sooting to sooting flames, three premixed atmospheric n-butane/oxygen/nitrogen flames surrounding the nucleation flame conditions were investigated: the flame at ϕ=1.6 is a fuel-rich non-sooting flame, the flame at ϕ=1.75 is a nucleation flame and the flame at ϕ=1.95 is a lightly sooting flame. The soot volume faction (SVF) profiles were previously measured by laser-induced incandescence as well as the soot size distributions. In the present study, mole fractions of stable species up to benzene were measured by gas chromatography while those of naphthalene and pyrene were obtained by jet-cooled laser-induced fluorescence. It is found that acetylene, propyne, benzene, naphthalene and pyrene species show the highest sensitivity with the equivalence ratio, while a two orders of magnitude increase of SVF is observed. The chemical flame structure of these flames was modeled using three kinetic mechanisms of the literature to which a recently developed soot code, based on a sectional approach, was coupled. The chosen model is representative of the current state-of-the-art of models describing all steps of soot formation and growth and fully coupled with the gas phase. The ability of such a model to predict soot volume fraction with reasonable predictions of gas-phase species is validated here based on the new experimental database presented in this work. It also highlights the improvement required on particle inception modeling to correctly predict particle size distributions.

An investigation of thermal radiation from laminar diffusion flames in a tri-coflow burner with central oxygen

In natural gas combustion processes, oxygen-enriched combustion is often used to improve heat transfer and thermal efficiency. In this investigation, a triple-port burner is employed to investigate the effect of oxygen enrichment on thermal radiation when introducing oxygen into the center of a normal coflow diffusion flame, while maintaining an outer coflow of air. Two fuels are investigated: methane, being the primary constituent of natural gas and having a low propensity for soot formation, and ethylene, which acts as a reference fuel with a much higher propensity for soot formation. The flow rates of air in the outer annulus and fuel in the inner annulus are held constant, while the flow rate of oxygen in the central tube is systematically increased. Total radiation, which is converted to radiation loss fraction, is measured using a wide-angle radiometer. Soot volume fraction and soot temperature are measured using two-color ratio pyrometry with a digital camera.For low flow rates of central oxygen when an inner oxygen-fuel flame is apparent, the thermal radiation is increased due to an increase in soot concentration. At these low flow rates, thermal radiation is increased by 20% for methane and 26% for ethylene, as compared to a normal coflow flame without central oxygen. The increase in radiation from these flames results in a decreasing, or relatively constant soot temperature in the soot laden region as the increased soot concentration radiates heat from the flame, even though gas temperatures upstream near the central oxygen flame are quite high. For relatively high flow rates of central oxygen, radiation from the tri-coflow methane flame increases by up to 31% compared to a normal coflow flame, while radiation from the ethylene flame monotonically decreases. For both fuels, when oxygen flow rates are high, soot concentration decreases (due to a change in flame shape and enhanced oxidation rates) and soot temperature increases. Product gases are the dominant emitters of radiation in the methane flames studied. Soot is the dominant radiant emitter in the ethylene flames until high flow rates of central oxygen reduce the soot concentration, such that high temperature product gases take over as the dominant radiant emitters. Overall, low flow rates of central oxygen can increase thermal radiation from the coflow methane flame by 20% due to increased soot concentration, and high flow rates of central oxygen can increase thermal radiation by 31% due to increased gas temperatures. However, the methane flames with central oxygen still emit at least 41% less radiation than the coflow ethylene flame. These results indicate that when considering the effect of oxygen enrichment on thermal radiation, the change in overall flame (gas and soot) emissivity can be just as important as the change in temperature.

Modelling of soot formation and aggregation in turbulent flows with the LES-PBE-PDF approach and a conservative sectional method

The present paper presents a comprehensive approach for modelling soot formation in turbulent flows that incorporates a recently developed conservative finite volume sectional method for the solution of the population balance equation (PBE) into the Large Eddy Simulation - Probability Density Function (LES-PDF) framework for modelling turbulent reacting flows. The approach thus predicts the particle size distribution of soot and accounts for the complete set of aerosol dynamic processes (nucleation, surface growth, oxidation, condensation and aggregation) as well as for the interaction between turbulence, chemistry and soot. We employ a combination of gas-phase chemistry, soot kinetics and aerosol dynamics recently used by the authors in the context of a laminar co-flow diffusion flame and maintain the same kinetics without adjustments in order to focus on the modelling issues in turbulent sooting flame simulations. The results show that several features such as the location of the soot forming zones and the qualitative profiles of soot volume fraction and species concentrations can be predicted reasonably well, but there is a considerable underprediction in the magnitude of soot volume fraction. The possible reasons for this underprediction are discussed in the context of the aforementioned laminar flame simulation and the previous validation of the components of our methodology. The CPU time analysis shows that the solution of the PBE by the conservative sectional method and the associated transport of the discretised number densities account for less than 25% of the total CPU time, indicating that its incorporation in LES-PDF simulations of turbulent combustion is computationally feasible.

Laboratory studies of ice nucleation onto bare and internally mixed soot–sulfuric acid particles

Abstract. Soot particles are potential candidates for ice-nucleating particles in cirrus cloud formation, which is known to exert a net-warming effect on climate. Bare soot particles, generally hydrophobic and fractal ones, mainly exist near emission sources. Coated or internally mixed soot particles are more abundant in the atmosphere and have a higher probability of impacting cloud formation and climate. However, the ice nucleation ability of coated soot particles is not as well understood as that of freshly produced soot particles. In this laboratory study, two samples, a propane flame soot and a commercial carbon black, were used as atmospheric soot surrogates and coated with varying wt % of sulfuric acid (H2SO4). The ratio of coating material mass to the mass of bare soot particles was controlled and progressively increased from less than 5 wt % to over 100 wt %. Both bare and coated soot particle ice nucleation activities were investigated with a continuous-flow diffusion chamber operated at mixed-phase and cirrus cloud conditions. The mobility diameter and mass distribution of size-selected soot particles with/without H2SO4 coating were measured by a scanning mobility particle sizer and a centrifugal particle mass analyser running in parallel. The mixing state and morphology of soot particles were characterized by scanning electron microscopy and transmission electron microscopy. In addition, the evidence of the presence of H2SO4 on a coated soot particle surface is shown by energy-dispersive X-ray spectroscopy. Our study demonstrates that H2SO4 coatings suppress the ice nucleation activity of soot particles to varying degrees depending on the coating thickness, but in a non-linear fashion. Thin coatings causing pore filling in the soot aggregate inhibits pore condensation and freezing. Thick coatings promote particle ice activation via droplet homogeneous freezing. Overall, our findings reveal that H2SO4 coatings will suppress soot particle ice nucleation abilities in the cirrus cloud regime, having implications for the fate of soot particles with respect to cloud formation in the upper troposphere.

Numerical Simultaneous Determination of Non-Uniform Soot Temperature and Volume Fraction from Visible Flame Images

This paper presents a method to invert the two-dimensional distribution of a temperature and volume concentration of soot particles from color images. By using numerical simulation, the temperature field and particle volume-concentration field of a non-uniform soot flame are simultaneously reconstructed using the wide-response spectrum of a color CCD camera without adding monochromatic filters. The influence of number of cameras, error of camera position angle, measurement noise and different reconstruction algorithms on measurement accuracy are analyzed. The numerical-simulation results demonstrate that camera-position angle errors play a crucial role in the reconstruction accuracy. In addition, increasing the number of cameras can improve the reconstruction result accuracy. Compared with the least squares algorithm, the Tikhonov-regularization algorithm has a stronger anti-noise ability and can resist 39 dB of noise. The conclusions obtained in this paper are helpful to guide following experimental studies.

Monitoring flame soot maturity by variable temperature Raman spectroscopy

Flame-formed soot nanoparticles are known to possess different nanostructures as a function of a large variety of combustion operative parameters, including particle residence time in flames, flame stoichiometry, fuel chemical composition, temperature and pressure. This implies that important properties (e.g., soot oxidation reactivity, optical and electronic gap) may be different depending on the way soot particles are generated. Hence, it is beneficial to develop diagnostic methods that are sensitive to such differences among the various kinds of soot particles. In this work we investigate by off-line variable-temperature Raman spectroscopy two types of soot particles, namely just-nucleated and aged/mature particles, with a different size and maturity degree. The results obtained for soot particles have been compared and discussed with those found for other related carbon materials. As the Raman spectra are recorded at increasing sample temperature, from 300 to 525 K, both soots display a linear downshift of the position of the two main Raman modes (D and G bands). Just-nucleated soot particles exhibit the strongest temperature dependence of the position of the G band. Based on results from density functional theory calculations, interpreted by a simple empirical model, the observed temperature coefficient differences can be ascribed to differences in the nanostructural order of the two soot samples, which causes a different thermal expansion behavior.

Effect of CO2/H2O addition on laminar diffusion flame structure and soot formation of oxygen-enriched ethylene

Oxygen-enriched combustion technology has an important application prospect, in which Oxy-steam combustion is a new generation of potential carbon capture technology. In this paper, the effects of O2/CO2 and O2/H2O atmosphere on soot formation in laminar diffusion flame were studied. The flame image was taken by a color (CCD) camera in the visible band, the directional emission power in R and G bands was calibrated, and the two-dimensional distribution of temperature and soot volume fraction in the flame was reconstructed. The experimental results are compared with the numerical results, and the numerical results well predict the temperature of oxygen-enriched flame in O2/N2/CO2 atmosphere, but overestimate the soot volume fraction. The laminar diffusion flame of ethylene in two kinds of oxygen-rich atmosphere was numerically studied by using a step-by-step decoupling method to separate the density, transport, thermal and chemical effects of the diluent by introducing four virtual substances. The calculation results show that combustion in O2/H2O and O2/CO2 atmosphere reduces the flame peak temperature, but the effect on the flame centerline temperature distribution is different. The addition of H2O enhanced the concentration of OH through the reverse reaction rate of OH + H2=H + H2O, while the addition of CO2 decreased the concentration of OH.O2/CO2 combustion leads to the increase of flame height and radius, while in O2/H2O atmosphere, the flame height is shortened. Both CO2 and H2O have a good inhibitory effect on soot formation. CO2 in the oxidant affects soot nucleation and surface growth rate mainly by reducing flame temperature and H mole fraction, but not by promoting soot oxidation process. Water vapor also inhibits soot formation by increasing OH concentration through chemical effect.

Experimental studies on soot in MILD oxy-coal combustion flame: Sampling, microscopic characteristics, chemical compositions and formation mechanism

Based on a diffusion-flamelet-based Hencken burner, the effect of temperature on the volume fraction of soot was explored firstly. The temperature of MILD oxy-coal (MILD-OCC) flame was measured by temperature measuring device and the volume fraction of soot was obtained by the thermocouple deposition method. Then the mass concentration, microstructure, nanostructure parameters (the distribution of particle size, the length of crystallite, the curvature of crystallite, the layer spacing of crystallite) and chemical compositions of soot were studied. The soot particles generated from MILD-OCC flame were harvested by thermophoretic sampling system and capillary sampling system, and measured with the combination of field emission transmission electron microscopy (TEM) and gas chromatography-mass spectrometry analyzer (GC-MS). The results showed that as the height of MILD-OCC flame increased, the degree of agglomeration of soot particles increased. The surface growth and oxidation existed at the same time and were in a competitive relationship, which manifested in the mass concentration of soot, the average distribution of particle size and the content of aromatic compounds. With the rise of flame height, the average length of the crystallite increased while the average curvature of the crystallite and the average crystalline layer spacing showed a decreasing trend, which showed that the microstructure of soot became more mature and orderly. These results are valuable for further understanding the formation mechanism of soot.