Soot Particle Size Distribution Research Articles

The effect of sodium chloride on the charge state of soot particles in a laminar diffusion flame

This study investigates the effect of sodium chloride on the charge state of soot nanoparticles formed in a laminar diffusion flame by measuring the soot particle size distribution, average charge per particle, and charge fraction at various heights within the flame. The well-studied Santoro burner with methane as the fuel (at 0.35 L/min) and co-flow air (at 70 L/min) was used, which produced a stable laminar diffusion flame with flame height of 61 mm. Samples of soot nanoparticles were extracted via a 0.3 mm orifice in a 3-mm stainless steel tubular probe at various heights above the burner and were immediately diluted by a factor of a few thousand for aerosol measurement. The effect of sodium chloride on a methane flame was investigated by comparing the experimentally measured data for methane-only and methane-NaCl flames. The addition of NaCl particles to the laminar diffusion flame did not have a significant effect on the particles in the nucleation region of the flame. The majority of the incipient soot particles in both flames are uncharged, and their sizes are nearly the same, with diameters of approximately 5 nm or less. However, the size of soot particles differs by approximately 10 % to 25 % between methane-only and methane-NaCl flames in the coagulation-dominated region of the flame. The net charge on soot particles within the coagulation region of the methane-only flames is negative, while it is positive with NaCl addition. The fraction of charged particles and ion concentration decreases with NaCl addition within the coagulation region. The study indicates that the smaller particle size observed in methane-NaCl flames may be attributed to reduced coagulation via altered particle charge states. These factors could be the major contributor to the variations in soot formation between methane-only and methane-NaCl flames. Novelty and Significance StatementThis research addresses a notable knowledge gap concerning the influence of NaCl, a prevalent component of hydraulic fracturing fluids, on soot particle behaviour in flames. By explaining the impact of NaCl on soot formation and charge states, the findings contribute to a deeper understanding of combustion processes in environments influenced by hydraulic fracturing operations, thereby informing strategies for reducing emissions and improving environmental sustainability in energy production. Overall, this article represents a significant advancement in the field of combustion science, with implications for environmental stewardship in energy production.This study provides valuable insights into how the introduction of NaCl alters the electrostatic properties of soot particles. This investigation expands upon existing knowledge by shedding light on the intricate mechanisms underlying soot formation and evolution in the presence of NaCl, elucidating its potential implications for combustion processes involving fossil fuels and industrial flaring.

Soot-on-snow experiment: artificial deposition of light-absorbing particles onto snow surfaces in 2018

The absorption of shortwave irradiance in snow depends on the physical properties of snow (e.g., snow grain size and shape, liquid water content, etc.) and light-absorbing particles (LAP). Originating from natural and anthropogenic sources, LAP has been reported to accelerate snowmelt significantly in different regions globally. Yet, our process-level understanding of LAP after deposition onto snow remains rather limited. Here we investigate the impacts of artificial deposition of different LAP onto snow surfaces in an outdoor environment of northern Finland. Following LAP dry deposition into a custom-made tent standing on top of the snowpack, the albedo was followed along with the properties of snow in snow pit measurements throughout the spring season. The results showed that the albedo decay at the end of the season for the different spots were linked to the initial amount and type of LAP that were deposited onto the snowpack. Measured snow temperature profiles from LAP doped snow versus natural reference snow illustrated that the LAP affected snow had higher temperatures in the subsurface snow layers. Collected snow samples analyzed for size distribution of soot particles revealed no apparent agglomeration of soot particles during thaw-freezing events taking place during the experiment. Despite the relatively large perturbation of the experimentally deposited LAP, their impact on the season length was only up to 3 days. Additional experiments are, nevertheless, needed to better constrain the effects of LAP on snow albedo, melt rate, and other associated processes.

An optical soot sizing method without prior morphology parameters

Great concern has been focused on the particle size distribution (PSD) of soot as a crucial factor of the physical and chemical properties. Optical methods are widely used to analyze the PSD of soot due to their non-invasive and real-time measurement, where the morphology parameters are essential for retrieving the PSD from optical signals. However, these parameters are difficult to obtain in field measurement. In this work, we propose a new PSD sensing method for soot without prior knowledge of the morphology parameters based on the light-scattering angular spectrum using a hybrid inverse algorithm. The light scattering angular spectrum is the intensity distribution of scattering light at different observation angles for simultaneously characterizing the PSD and the morphological parameters, which are decoupled by a hybrid inverse algorithm consisting of Tikhonov regularization and adaptive weighted particle swarm optimization (AW-PSO). A compacted and lens-free prototype sensor is designed to verify our method. The calibration experiments by spherical aerosols show that our prototype sensor provides high-precision light scattering angular spectrum measurement with maximum relative error (RE) of 14.78 %. In the tests of soot, the maximum Kullback-Leibler Divergence (DKL) of PSD is 0.28 in comparison with the reference volume equivalent PSD. The sensing method proposed in this paper provides volume equivalent PSD measurement for soot without requirement of the morphology parameters, and our prototype sensor shows great potential for soot and other non-spherical aerosol analysis in routine field measurements outside the laboratory.

LES of a pressurized sooting aero-engine model burner using a computationally efficient discrete sectional method coupled to tabulated chemistry

This work is focused on the modeling and analysis of soot formation and oxidation in the pressurized ethylene-based model burner investigated at DLR. This burner features a dual swirler configuration for the primary air supply and includes secondary dilution jets inside the combustion chamber, showing reacting flow characteristics representative of the RQL combustor technology. Large-eddy simulations (LES) of the DLR burner are conduced here to assess a coupling approach between flamelet generated manifold (FGM) chemistry and discrete sectional method (DSM) based soot model with clustering method. First, a validation of the numerical results is conducted for the gas velocity and temperature fields, and good agreement is obtained for both mean and fluctuating quantities. The Soot Volume Fraction (SVF) computed from LES shows a satisfactory agreement with the experimental data in both SVF distribution and magnitude. The analysis also includes a numerical investigation of the soot production and the Particle Size Distributions (PSD). Finally, the configuration without secondary air is evaluated and an accurate prediction of the SVF field is also obtained. In this case, the absence of dilution air strongly influences the central region of the combustion chamber, and soot distribution and PSD are mainly affected by transport and dilution, not oxidation. It is finally concluded the proposed modeling framework is capable of predicting the soot field and particle size distributions inside the combustor for both operating conditions.

Experimental and numerical investigation on soot formation and evolution of particle size distribution in laminar counterflow ethylene flames

A detailed investigation of the process of soot formation in ethylene-fueled laminar counterflow diffusion flames is conducted using dedicated experiments and numerical simulations. Two different strategies based on the Discrete Sectional Method (DSM) and the Split-based Quadrature Method of Moments (S-EQMOM) are considered to model the evolution of soot particle size distributions, and their comparative assessment is carried out for soot formation prediction and particle growth. A consistent chemical reaction mechanism describing the oxidation of hydrocarbon fuels and the prediction of soot precursors with the growth of polycyclic aromatic hydrocarbons (PAHs) up to pyrene ( ▪ ) is examined. Experiments for various strain rates and fuel compositions are performed to assess the sensitivity of soot production to these two parameters. The results show that both modeling strategies captured well the qualitative trends of soot volume fraction under variations in strain rate and mixture composition, with slight over-prediction of the peak values. For both soot models, a higher sensitivity of soot formation is noticed by changes in mixture composition compared to those of strain rate variation. Additionally, the soot models demonstrated promising performance in capturing the experimentally observed evolution of the soot particle size distribution (PSD).

LES investigation of soot formation in a turbulent non-premixed jet flame with sectional method and FGM chemistry

This study proposes a detailed soot modeling framework for large-eddy simulation (LES) to accurately predict soot formation and particle size distributions (PSD) in turbulent reacting flows. The framework incorporates Flamelet Generated Manifold (FGM) chemistry and a soot model based on the discrete sectional method (DSM) to predict both qualitative and quantitative sooting behavior while keeping the computational cost affordable. Two elementary modeling strategies are considered in the LES formalism for describing soot formation rates. These strategies rely on an a-priori tabulation of soot formation rates and their run-time computation. The LES formalism is applied to the simulations of a well-characterized, non-premixed, turbulent jet flame. A comparative analysis of strategies employed for filtered soot source term treatment is conducted to investigate their impact on the prediction of soot quantities and the evolution of soot PSDs. The LES results for the gas phase and soot phase are compared against the available experimental data. A good prediction of soot evolution is achieved with the two methodologies. The tabulation of soot formation rates leads to a significant reduction in computational cost compared to the model based on their explicit runtime computation. The LES results reveal that the modeling of filtered soot source terms has a significant impact on the quantitative prediction of soot formation. The possible reasons for the observed differences in the soot prediction are discussed. The run-time computation-based model provides a more consistent treatment of the non-linear interactions between the gas and soot phases in soot source terms compared to the tabulated soot chemistry approach. On the other hand, the tabulated soot chemistry model is an interesting and efficient modeling approach for predicting soot formation in turbulent conditions. Overall, both approaches have their strengths and limitations, and the choice of approach may depend on the specific needs of the application.

A computationally efficient approach for soot modeling with discrete sectional method and FGM chemistry

A novel approach for the prediction of soot formation in combustion simulations within the framework of discrete sectional method (DSM) based univariate soot model and Flamelet Generated Manifold (FGM) chemistry, referred to as FGM-CDSM, is proposed in this study. The FGM-CDSM considers the clustering of soot sections derived from the original soot particle size distribution function (PSDF) to minimize the computational cost. Unlike conventional DSM, in FGM-CDSM, governing equations for soot mass fractions are solved for the clusters, by using a pre-computed lookup table with tabulated soot source terms from the flamelet manifold, while the original soot PSDF is re-constructed in a post-processing stage. The flamelets employed for the manifold are computed with detailed chemistry and the complete sectional soot model. A comparative assessment of FGM-CDSM is conducted in laminar diffusion flames for its accuracy and computational performance against the detailed kinetics-based classical sectional model. Numerical results reveal that the FGM-CDSM can favorably reproduce the global soot quantities and capture their dynamic response predicted by detailed kinetics with a good qualitative agreement. Furthermore, compared to detailed kinetics, FGM-CDSM is shown to substantially reduce the computational cost of the complete reacting flow simulation with soot particle transport. Primarily, the use of FGM reduces the overall calculation by about two orders of magnitude compared to detailed kinetics, which is advanced further with the clustering of sections at a low memory footprint. Therefore, the present work demonstrates the promising capabilities of FGM-CDSM in the context of computationally efficient soot calculations and provides an excellent framework for extending its application to the simulations of turbulent sooting flames.

On the impact of differential diffusion between soot and gas phase species in turbulent flames

The molecular diffusivities of larger PAHs and soot particles approach zero leading to differential diffusion with gas-phase species. The present work systematically quantifies the impact on soot moments, soot related statistical correlations and Particle Size Distributions (PSDs) using a fully coupled transported joint probability density function (JPDF) method featuring a 78-dimensional joint-scalar space, including enthalpy, gas phase species with the PSD discretised using 62 size classes via a mass and number density preserving sectional method. Differential diffusion of soot (DDS) is treated via a gradual decline of diffusivity among soot sections maintaining realisability and the expected exponential decay of variance. The solution of the flow field features a time-dependent second moment closure and an elliptic solver. The turbulent non-premixed Sandia C2H4 flame from the International Sooting Flame (ISF) data base was selected as a target along with the KAUST (C2H4/N2) variant of the same flame. Results show that reduced soot diffusion leads to a significant increase in the soot volume fraction RMS and that the correlation coefficient between soot volume fraction and temperature is further reduced in a particle-size-dependent manner. Similar observations are made for correlations between the soot volume fraction and the mass fractions of gas-phase species such as CO, OH, H and C2H2. The results suggest that computational methods that presume explicit (e.g. flame structure related) correlations between such scalars and with soot face leading order modeling challenges. It is also shown that the correlation between CO and soot increases due to oxidation of soot and that DDS leads to a modest downstream shift of PSDs towards larger particles.

Effects of Iron Addition on the Collision of Polycyclic Aromatic Hydrocarbon Clusters: A Molecular Dynamics Study

In this work, soot particle size distributions in iron-doped premixed ethylene flames are examined using scanning mobility particle sizer measurements. It is found that iron addition promotes the growth in soot particle size, and the enhanced particle coagulation is inferred to be an important reason. To support that, the influence of iron addition on the coagulation of polycyclic aromatic hydrocarbon (PAH) clusters, the analogue of incipient soot particles, is further investigated using molecular dynamics simulations. Based on the results of hundreds of binary head-on collision simulations, the collision between two coronene-Fe-coronene dimers is found to have a significantly higher coagulation efficiency than that between two coronene dimers. However, this enhancement effect weakens as the size of the PAH monomer increases. Although the coagulation efficiency can be increased by iron addition, the collision frequency is almost unaffected, as revealed from the binary off-central collision simulations. Moreover, the simulation results of coronene cluster growth via coagulation show that iron addition promotes coronene cluster growth, leading to larger cluster size, which may explain the larger soot particle size observed in iron-doped flames.

Evolution of the Soot-Particle Size Distribution Function in the Cylinder and Exhaust System of Piston Engines: Simulation

A computational tool for simulating the temporal evolution of the soot-particle size distribution function (SDF) in the internal combustion engine (ICE) and in the attached exhaust pipe is developed and tested against available experimental data on the soot-particle SDF at the outlet of the exhaust system. Firstly, a database of soot particle properties (particle mean diameter, dispersion, total particle number density vs. time for different fuels, fuel-to-air equivalence ratios, temperatures, pressures, and exhaust gas recirculation) is developed based on the thoroughly validated detailed model of soot formation under ICE conditions. The database is organized in the form of look-up tables. Secondly, the soot-particle SDF in the database is approximated using the log-normal SDF, which is directly used in the multidimensional calculations of the ICE operation process. Thirdly, the coagulation model of soot particles is developed, which includes three coagulation mechanisms: Brownian, turbulent–kinetic, and turbulent–diffusion. This model is applied for simulating the evolution of the soot-particle SDF in the exhaust pipe after opening the exhaust valve. Calculations show that the coagulation process of soot particles in the exhaust pipe has a significant effect on the mean size of particles at the outlet of the exhaust system (the mean particle diameter can increase by almost an order of magnitude), and the dominant mechanism of particle coagulation in the exhaust system of a diesel engine is the Brownian mechanism. The objective, approach, and obtained results are the novel features of the study.

Impacts of Cloud‐Processing on Ice Nucleation of Soot Particles Internally Mixed With Sulfate and Organics

AbstractSoot particles are one of the major aerosol components (in particle number concentration) in the troposphere and can impact cirrus formation. Depending on their physicochemical properties, soot particles can nucleate ice in the cirrus regime via pore condensation and freezing (PCF) at a lower ice saturation threshold than that of the homogeneous freezing of solution droplets. Soot aerosol undergoing multiple cloud cycles can change its porosity and surface wettability, thus modulating its PCF ability. In this study, organic‐rich and ‐lean size‐selected propane flame soot particles were coated with different thicknesses of sulfuric acid (H2SO4) and exposed to thermodynamic conditions under 228 K and relative humidity with respect to water 104% to simulate contrail formation. Ice‐activated soot particles from the mimicked contrail were sublimated before being tested for ice nucleation (IN) at T ≤ 233 K. Additionally, soot particle size and mass distribution as well as morphology were characterized. The results demonstrate that the increase in mesopore availability induced by cloud‐processing plays a key role in regulating soot IN. All cloud‐processed soot become more compacted, however, only if more PCF relevant mesopores are generated, can the compacted soot exhibit promoted IN. If a H2SO4 coating and/or enriched organics occupy the pore volume, inhibition of PCF is observed for the cloud‐processed soot. Notably, a thick H2SO4 coating enhances the PCF of 400 nm organic‐lean soot particles because the partially engulfed but collapsed soot‐core may have new mesopores produced by compaction. Therefore, the mesopore abundance plays the key role in evaluating aged soot IN ability.

Experimental investigation on the size-dependent maturity of soot particles in laminar premixed ethylene burner-stabilized stagnation flames

To understand soot maturation mechanism, we investigate the size-evolution of soot maturity in a series of laminar premixed burner-stabilized stagnation ethylene flames, with the maximum flame temperature Tf,max ranging from 1630 to 1869 K and the equivalence ratio φ ranging from 2.0 to 2.3. The soot particle size distribution is obtained by using the orifice sampling technique together with a scanning mobility particle sizer, while the maturity of soot is evaluated based on its oxidation characteristics and Raman spectra. The results show that at a fixed φ (say 2.2), soot particles grow bigger and become more mature concurrently in higher Tf,max flames (1809 and 1869 K). In contrast, although particle size increases obviously with time in lower Tf,max flames (1630 and 1724 K), soot maturity remains almost unchanged, indicating that particle growth is mainly controlled by particle coagulation or PAH condensation, instead of surface reactions in these flames. At a fixed Tf,max (say ∼ 1725 K), soot size growth is faster at higher φ as expected. However, when comparing soot particles of similar sizes, the particles from lower φ flames are more mature than those from higher φ flames, where the particle growth rate is too high to allow sufficient residence time for particle maturation.

Soot nanoparticle sizing in counterflow flames using in-situ particle sampling and differential mobility analysis verified with two-colour time-resolved laser-induced incandescence

The emphasis of this work is on the development of an intrusive particle sampling system to track the evolution of soot nanoparticles in ethylene counterflow diffusion flames. The overarching objective is to determine the mobility size distributions in a spatially resolved manner using the developed probe system coupled with differential mobility analysis, i.e., a scanning mobility particle sizer (SMPS). The probe system involves a tailor-made quartz probe, gas supply, pressure control periphery, and a traverse system enabling a precise positioning along the flame axis. In preliminary experiments, the dilution ratio of the quartz probe as function of boundary conditions as well as particle losses during intrusive particle sampling are studied. To demonstrate the capability of the developed particle sampling system, results from ethylene counterflow diffusion flames with different fuel mass fractions and strain rates are presented and compared with results derived by non-intrusive laser-based diagnostics, i.e., two-colour time-resolved laser induced incandescence (2C-TiRe-LII). Results of these experiments indicate that the particle sampling system is capable of tracking the development of particle size distributions – independent of the distribution function, i.e., mono-, bi- or multimodal shape – in counterflow flames. Likewise, the agreement between soot volume fractions and particle size distributions measured via intrusive particle sampling coupled with differential mobility analysis and non-intrusive laser-based 2C-TiRe-LII is excellent at varying the fuel mass fractions and strain rates of the ethylene counterflow flames.

Soot particle size distributions in turbulent opposed jet flames with premixed propene–air reactants

Emissions of soot are strongly dependent on turbulence-chemistry interactions due to the relatively slow formation and oxidation processes. Studies of laminar flames have shown that both flow conditions and the chemistry of the parent fuel have a significant impact on measured particle size distributions (PSDs). The current study determines the impact of flow on the development of PSDs in premixed turbulent flames through a variation in the total rate of strain using an opposed jet configuration with fractal grid generated turbulence. The impact of fuel chemistry is investigated under such conditions through the use of propene–air flames with results compared to the corresponding ethene–air flames quantified in earlier studies. Samples were extracted using a quartz probe featuring aerodynamic quenching and dual port dilution at the probe tip and in the transfer-line. Spatially resolved PSD data is obtained along the stagnation point streamline using a scanning mobility particle sizer equipped with nano- and long-DMA columns to show the evolution through the turbulent flame brush. Results confirm that PSDs of soot in premixed turbulent flames are exceptionally sensitive to both the chemistry of the parent fuel and the flow field. The reduced residence times in the current turbulent flows lead to maximum median and mean mobility diameters below 10 nm with higher rates of strain promoting unimodal PSD shapes. It is further shown that the chemistry of the parent fuel has a strong influence on PSDs with propene causing a two order of magnitude increase in smaller particles compared to the corresponding ethene flame.

Flamelet LES of a turbulent pulverized solid fuel flame using a detailed phenomenological soot model

In this work, large-eddy simulation (LES) is conducted for a turbulent pulverized coal flame with a detailed phenomenological model to characterize the soot evolution and a flamelet model to describe the detailed gas phase kinetics. In particular, a quadrature-based moment method (QBMM) is adopted to describe the soot statistics with the physicochemical processes of soot particle nucleation, condensation, coagulation, chemical surface growth and oxidization being considered. The simulation results are compared to the experimental data, including the direct photograph images, particle velocities, laser induced fluorescence (LIF) for polycyclic aromatic hydrocarbons (PAHs), laser induced incandescence (LII) for soot, scanning electron microscope (SEM) with the thermophoretic sampling (TS), and the time-resolved LII (TiRe-LII) for spatial soot particle size distribution. The comparisons show that the ignition position and the mean velocity of the coal particles can be accurately predicted with the proposed flamelet/QBMM/LES method, and an overall good agreement is also obtained when comparing against the PAHs-LIF, soot-LII and SEM images. The importance of the contributions of the different physicochemical processes to the soot particle volume growth is quantified by analyzing the corresponding moment source terms. It is found that for the pulverized coal flame studied, the chemical surface growth is the most important contribution to the soot volume growth at different locations along the streamwise direction. Although the nucleation does not make a significant contribution to soot volume growth, it determines the number density of the primary soot particles formed in the main flow region.

Investigation of soot formation in [formula omitted]-dodecane spray flames using LES and a discrete sectional method

Considering stricter regulations on soot emissions, the detailed soot modeling approaches facilitating prediction of soot particle size distributions (PSD) are increasingly in demand. In this context, the transient evolution of soot is numerically investigated for two high-pressure turbulent sprays from the Engine Combustion Network (ECN), namely, Spray C (SC) and Spray D (SD). The 900−K ambient temperature (Tam) sprays are studied. This is because the two cases tend to produce a similar amount of soot at Tam=900K, despite the significantly different spray development. To predict the soot formation with information on PSD, a discrete sectional method is applied within the large-eddy simulation (LES) framework. The applied modeling strategy favorably captures the experimentally observed similar soot mass for SC and SD in the characteristic field-of-view (FOV) frustum. Moreover, the transient dynamics of soot within the FOV frustum is well captured, and the onset of soot is well predicted. It is observed that for SC and SD, soot formation is more prominent in fuel-rich (2<ϕ<4) and high-temperature (T>1500K) regions. Despite the stronger fuel dilution in the downstream area of the spray, soot is predominantly present in the head of the spray during the whole combustion progress, corresponding to larger particle sizes and higher soot number density. Although the spray development of SC and SD are different, the FOV approach bridges the two cases. The unique correlation between soot mass and FOV volume recognized in experiments was found to hold for the complete quasi-steady sooting region. Moreover, PSD analysis suggests very similar soot size and number density with respect to the FOV volume. This is attributed to the similar LOL for SC and SD in the normalized coordinates, and the same FOV volume corresponding to similar locations in the normalized coordinates.

Soot Size Determination In A Swirl Stratified Premixed Ethylene-Air Flame By A Sampling Probe And Elastic Light Scattering

An experimental study was performed to measure the size and number density distributions of soot particles produced in turbulent, stratified (high spatial equivalence ratio gradient), swirled (rotating flow) premixed ethylene-air flames at atmospheric pressure. Soot particle size and number density measurements are initially performed using a Scanning Mobility Particle Sizer (SMPS). For this purpose, two-stage sampling and dilution device designed for hot gas analysis was used. The dilution rate of the sampling apparatus was evaluated to ensure a most representative probing. In a second step, the ex-situ measurements were replaced by single-shot measurements recorded with a high cadency planar multi-angle light scattering (2D-MALS) laser diagnostic technique, based on the relationship between aggregate size and light scattering angle. In a third step, results obtained by the SMPS as well as by the optical diagnostic were compared. Because a direct confrontation of the obtained results obtained is not feasible due to difference in nature of both techniques, a two-step post-processing methodology as developed. For this purpose, the median electric mobility diameters measured by SMPS were converted into diameters of gyration by means of a semi-empirical conversion tool. Moreover, a time average data processing was applied to the soot size distributions recorded by 2D-MALS, considering that SMPS measurements performed over a relatively large acquisition time converge to a single value. Results obtained in stratified swirled premixed flames by SMPS exhibit an overall good agreement with the optical measurements. This good similarity between the results provides a remarkably high degree of confidence in the quality of the measurements for both measurement systems investigated. Furthermore, the results suggest that a comparison of soot aggregate size and number density measurements between a sampling probe and a light scattering technique is still possible in turbulent flames at atmospheric pressure. While the current work has focused on the performances of SMPS and the 2D-MALS approach on a one-to-one basis, future work will also address the application of these diagnostics to high-pressure two-phase flames for which measurements are made in confined environments.

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.

Simulation of the Formation and Growth of Soot Aerosol Particles in a Premixed Combustion Process Using a Soot Aerosol Dynamics Model

Recently, an aerosol dynamics model—the Soot Aggregate Moment Model (SAMM)—that can efficiently trace the size distribution and morphology of soot particles was developed. In order to examine the applicability of SAMM in association with open-source CFD and combustion chemistry solvers, the formation and growth of soot particles in a premixed ethylene/air combustion were simulated by connecting SAMM with OpenSMOKE++ in this study. The simulation results were compared with available measurements and with the results of a previous study conducted using SAMM connected with an in-house CFD code and the CHEMKIN combustion chemistry package. Both CHEMKIN and OpenSMOKE++ underestimated C2H2 concentration compared to previous measurements, with deviation from the measured data being smaller for OpenSMOKE++. The chemical mechanism adopted in the CHEMKIN package was found to underestimate pyrene concentration by a factor of several tens. OpenSMOKE++ predicted much higher soot precursor concentrations than CHEMKIN, leading to a higher nucleation rate and a faster surface growth in the latter part of the reactor. This resulted in a reasonable soot production rate without introducing an artificial condensation enhancement factor. The overestimation of low-molecular-weight polycyclic aromatic hydrocarbons in the latter part of the reactor and the neglect of sintering led to an overprediction of soot production and primary particle number. This result indicates that accounting only for obliteration without sintering in SAMM could not simulate the merging of primary particles sufficiently. This indication merits further investigation.

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.