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Soot and Radiation Measurements in Microgravity Jet Diffusion Flames

The subject of soot formation and radiation heat transfer in microgravity jet diffusion flames is important not only for the understanding of fundamental transport processes involved but also for providing findings relevant to spacecraft fire safety and soot emissions and radiant heat loads of combustors used in air-breathing propulsion systems. Our objectives are to measure and model soot volume fraction, temperature, and radiative heat fluxes in microgravity jet diffusion flames. For this four-year project, we have successfully completed three tasks, which have resulted in new research methodologies and original results. First is the implementation of a thermophoretic soot sampling technique for measuring particle size and aggregate morphology in drop-tower and other reduced gravity experiments. In those laminar flames studied, we found that microgravity soot aggregates typically consist of more primary particles and primary particles are larger in size than those under normal gravity. Comparisons based on data obtained from limited samples show that the soot aggregate's fractal dimension varies within +/- 20% of its typical value of 1.75, with no clear trends between normal and reduced gravity conditions. Second is the development and implementation of a new imaging absorption technique. By properly expanding and spatially-filtering the laser beam to image the flame absorption on a CCD camera and applying numerical smoothing procedures, this technique is capable of measuring instantaneous full-field soot volume fractions. Results from this technique have shown the significant differences in local soot volume fraction, smoking point, and flame shape between normal and reduced gravity flames. We observed that some laminar flames become open-tipped and smoking under microgravity. The third task we completed is the development of a computer program which integrates and couples flame structure, soot formation, and flame radiation analyses together. We found good agreements between model predictions and experimental data for laminar and turbulent flames under both normal and reduced gravity. We have also tested in the laboratory the techniques of rapid-insertion fine-wire thermocouples and emission pyrometry for temperature measurements. These techniques as well as laser Doppler velocimetry and spectral radiative intensity measurement have been proposed to provide valuable data and improve the modeling analyses.

Ku, Jerry C.↗

Laminar Soot Processes

Soot formation within hydrocarbon-fueled flames is an important unresolved problem of combustion science for several reasons: soot emissions are responsible for more deaths than any other combustion pollutant, thermal loads due to continuum radiation from soot limit the durability of combustors, thermal radiation from soot is mainly responsible for the growth and spread of unwanted fires, carbon monoxide associated with soot emissions is responsible for most fire deaths, and limited understanding of soot processes is a major impediment to the development of computational combustion. Thus, soot processes within laminar nonpremixed (diffusion) flames are being studied, emphasizing space-based experiments at microgravity. The study is limited to laminar flames due to their experimental and computational tractability, noting the relevance of these results to practical flames through laminar flamelet concepts. The microgravity environment is emphasized because buoyancy affects soot processes in laminar diffusion flames whereas effects of buoyancy are small for most practical flames. Results discussed here were obtained from experiments carried out on two flights of the Space Shuttle Columbia. After a brief discussion of experimental methods, results found thus far are described, including soot concentration measurements, laminar flame shapes, laminar smoke points and flame structure. The present discussion is brief.

Lin, K. -C.↗

Fuel Preheat Effects on Soot-Field Structure in Laminar Gas Jet Diffusion Flames Burning in 0-g and 1-g

An experimental investigation conducted at the 2.2-s drop tower of the NASA Lewis Research Center is presented to quantify the influence of moderate fuel preheat on soot-field structure within 0-g laminar gas jet diffusion flames. Parallel work in 1-g is also presented to delineate the effect of elevated fuel temperatures on soot-field structure in buoyant flames. The experimental methodology implements jet diffusion flames of nitrogen-diluted acetylene fuel burning in quiescent air at atmospheric pressure. Fuel preheat of approximately 100 K in the 0-g laminar jet diffusion flames is found to reduce soot loadings in the annular region, but causes an increase in soot volume fractions at the centerline. In addition, fuel preheat reduces the radial extent of the soot field in 0-g. In 1-g, the same fuel preheat levels have a more moderated influence on soot loadings in the annular region, but are also seen to enhance soot concentrations near the axis low in the flame. The increased soot loadings near the flame centerline, as caused by fuel preheat, are consistent with the hypothesis that preheat levels of approximately 100 K enhance fuel pyrolysis rates. The results show that the growth stage of particles transported along the soot annulus is shortened both in 1-g and 0-g when elevated fuel temperatures are used.

Konsur, Bogdan↗

Soot Formation in Laminar Premixed Methane/Oxygen Flames at Atmospheric Pressure

Flame structure and soot formation were studied within soot-containing laminar premixed mc1hane/oxygen flames at atmospheric pressure. The following measurements were made: soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, soot structure by thermophoretic sampling and transmission electron microscope (TEM), major gas species concentrations by sampling and gas chromatography, and gas velocities by laser velocimetry. Present measurements of gas species concentrations were in reasonably good agreement with earlier measurements due to Ramer et al. as well as predictions based on the detailed mechanisms of Frenklach and co-workers and Leung and Lindstedt: the predictions also suggest that H atom concentrations are in local thermodynamic equilibrium throughout the soot formation region. Using this information, it was found that measured soot surface growth rates could be correlated successfully by predictions based on the hydrogen-abstraction/carbon-addition (HACA) mechanisms of both Frenklach and co-workers and Colket and Hall, extending an earlier assessment of these mechanisms for premixed ethylene/air flames to conditions having larger H/C ratios and acetylene concentrations. Measured primary soot particle nucleation rates were somewhat lower than the earlier observations for laminar premixed ethylene/air flames and were significantly lower than corresponding rates in laminar diffusion flames. for reasons that still must be explained.

Xu, F.↗

Soot Oxidation in Laminar Hydrocarbon/Air Diffusion Flames at Atmospheric Pressure

Soot oxidation was studied experimentally in laminar hydrocarbon/air diffusion flames at atmospheric pressure. Measurements were carried out along the axes of round jets burning in coflowing air considering acetylene, ethylene, proplyene and propane as fuels. Measurements were limited to the initial stages of soot oxidation (carbon consumption less than 70%) where soot oxidation mainly occurs at the surface of primary soot particles. The following properties were measured as a function of distance above the burner exit: soot concentrations by deconvoluted laser extinction, soot temperatures by deconvoluted multiline emission, soot structure by thermophoretic sampling and analysis using Transmission Electron Microscopy (TEM), concentrations of stable major gas species (N2, H2O, H2, 02, CO, CO2, CH4, C2H2, C2H4, C2H6, C3H6, and C3H8) by sampling and gas chromatography, concentrations of some radical species (H, OH, O) by the deconvoluted Li/LiOH atomic absorption technique and flow velocities by laser velocimetry. It was found that soot surface oxidation rates are not particularly affected by fuel type for laminar diffusion flames and are described reasonably well by the OH surface oxidation mechanism with a collision efficiency of 0.10, (standard deviation of 0.07) with no significant effect of fuel type in this behavior; these findings are in good agreement with the classical laminar premixed flame measurements of Neoh et al. Finally, direct rates of surface oxidation by O2 were small compared to OH oxidation for present conditions, based on estimated O2 oxidation rates due to Nagle and Strickland-Constable, because soot oxidation was completed near the flame sheet where O2 concentrations were less than 1.2% by volume.

Xu, F.↗

Soot Aerosol from Aircraft: Is there Enough to Cause Middle-Latitude Lower Stratospheric Ozone

Soot aerosol from aircraft has been implicated to cause long-term ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. equals 5%,per decade. During the 1996 SUCCESS field campaign, we sampling aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EIH2SO4=4.8E-2 and 5.7E- 1. g/kgFUEL for 75 and 675 ppm fuel-sulfur, respectively) and soot (EIsoot=7.5E-4 g/kgFUEL). The corresponding fuel-sulfur to H2SO4 conversion efficiency was 25 % and 30%,respctively. Applying the H2SO4 emission index to the 1990 fuel by the world's commercial fleets of 1.3E11 kg, a conversion efficiency of 30% would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4, if the fuels averaged 500 ppmm.The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E5 kg. Thus, soot amounts to only one half of one percent of the aerosol generated by aircraft. The fractal nature of soot may increase its actual surface area by about a factor of 10. The findings, however, of (1) stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year; and (2) a trend in stratospheric soot loading of approx.6% per year since 1981, similar to the annual increase of aircraft operations since that time, implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II extinction, against the "noise" due to volcanic eruptions, The current single scatter albedo of the stratospheric aerosol is omega = 0.993+/-0.004.

Pueschel, R. F.↗

Soot Formation in Laminar Premixed Methane/Oxygen Flames at Atmospheric Pressure

Flame structure and soot formation were studied within soot-containing laminar premixed methanefoxygen flames at atmospheric pressure. The following measurements were made: soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, soot structure by thermophoretic sampling and transmission electron microscope (TEM), major gas species concentrations by sampling and gas chromatography, and gas velocities by laser velocimetry. Present measurements of gas species concentrations were in reasonably good agreement with earlier measurements due to Ramer et al. as well as predictions based on the detailed mechanisms of Frenklach and co-workers and Leung and Lindstedt; the predictions also suggest that H atom concentrations are in local thermodynamic equilibrium throughout the soot formation region. Using this information, it was found that measured soot surface growth rates could be correlated successfully by predictions based on the hydrogenabstraction/carbon-addition (HACA) mechanisms of both Frenklach and co-workers and Colket and Hall, extending an earlier assessment of these mechanisms for premixed ethylene/air flames to conditions having larger H/C ratios and acetylene concentrations. Measured primary soot particle nucleation rates were somewhat lower than the earlier observations for laminar premixed ethylene/air flames and were significantly lower than corresponding rates in laminar diffusion flames, for reasons that still must be explained.

Xu, F.↗

Soot Oxidation in Hydrocarbon/Air Diffusion Flames at Atmospheric Pressure

Soot oxidation was studied experimentally in laminar hydrocarbon/air diffusion flames at atmospheric pressure. Measurements were carried out along the axes of round jets burning in coflowing air considering acetylene, ethylene, propylene and propane as fuels. Measurements were limited to the initial stages of soot oxidation (carbon consumption less than 70%) where soot oxidation mainly occurs at the surface of primary soot particles. The following properties were measured as a function of distance above the burner exit: soot concentrations by deconvoluted laser extinction, soot temperatures by deconvoluted multiline emission, soot structure by thermophoretic sampling and analysis using Transmission Electron Microscopy (TEM), concentrations of stable major gas species (N2, H2O, H2, O2, CO, CO2, CH4, C2H2,C2H4, C2H6, C3H6, and C3H8) by sampling and gas chromatography, concentrations of some radical species (H, OH, O) by the deconvoluted Li/LiOH atomic absorption technique and flow velocities by laser velocimetry. It was found that soot surface oxidation rates are not particularly affected by fuel type for laminar diffusion flames and are described reasonably well by the OH surface oxidation mechanism with a collision efficiency of 0.10, (standard deviation of 0.07) with no significant effect of fuel type in this behavior; these findings are in good agreement with the classical laminar premixed flame measurements of Neoh et al. Finally, direct rates of surface oxidation by O2 were small compared to OH oxidation for present conditions, based on estimated O2 oxidation rates due to Nagle and Strickland-Constable (1962), because soot oxidation was completed near the flame sheet where O2 concentrations were less than 1.2% by volume.

Xu, F.↗

Resolving Mixtures of Soot Characterized by SP-AMS Spectra Using a Latent Dirichlet Allocation Model

Soot produced by detonation or combustion events exhibits different chemical properties depending on the fuel, device construction, and environmental conditions in which the event occurs. These properties can be useful for defining relevant signatures for probabilistically identifying the different types of events that occurred, based on the soot that is produced from these events. However, it is rare to observe samples of soot from a detonation or combustion that are not contaminated by outside particles. In this paper, we present a method for resolving mixtures of soot to determine the contributions of sources that may be present in samples of recovered soot. We use Latent Dirichlet Allocation to describe the generative process for a sample of recovered soot, and use Variational Bayesian Inference to learn about the parameters associated with the generative model. We demonstrate the utility of this method by considering real samples of mixtures of soot under various frameworks to show that the model is able to identify the different components present in a sample of soot as well as their mixing proportions.

54 ENVIRONMENTAL SCIENCES↗

Soot and PAH formation in high pressure spray pyrolysis of gasoline and diesel fuels

Time-resolved soot and PAH formation from gasoline and diesel spray pyrolysis are visualized and quantified using diffuse back illumination (DBI) and laser induced fluorescence (LIF) at 355 nm, respectively, in a constant-volume vessel at 60 bar from 1400 to 1700 K for up to 30 ms. The delay, maximum formation rate, and yield of soot and PAHs are compared across fuels and temperatures and correlated with the yield sooting indices on either the mass or mole basis. The delays generally decrease with increasing temperature, and the formation rates of both PAHs and soot generally increase with temperature. The apparent PAH-LIF yield may decrease with temperature due to PAH growth and conversion into larger species, signal trapping, and thermal quneching. Soot yield generally increases with temperature. The mass-based YSI correlates reasonably well with soot delay, but YSI does not correlate well with soot yield. Here, the mass-based YSI is a more appropriate predictor of sooting propensity than the mole-based YSI.

42 ENGINEERING↗

Analysis of soot formation from aviation fuels in laminar counterflow flames

Combustion emissions from aviation contribute to the formation of condensation trail (contrail) that can lead to the formation of anthropogenic cirrus clouds. Ice particles that form contrails are observed to have a linear correlation with soot particle number density. Synthetic aviation fuels (SAFs) offer a promising route to mitigate the production of soot particles while also increasing energy security. Although studies have focused on combustion and spray behavior, the detailed investigation of soot formation processes for different jet fuels and their impact on models for computational fluid dynamics (CFD) applications is not well understood. Moreover, experimental measurements of soot for canonical flames using Synthetic aviation fuels (SAF) for model validation remain scarce. To address this, we use employed the Lawrence Livermore National Laboratory (LLNL) detailed soot model based on the discrete sectional method. Additionally, we develop two reduced chemical mechanisms for Jet-A and Alcohol-to-Jet (C1) that are suitable for turbulent flame simulations and couple them with the Hybrid Method of Moments (HMOM). The detailed and reduced model frameworks are validated against experimental measurements of soot volume fraction (ƒ ν ) from a counterflow burner experiment previously reported in the literature. Given the good agreement between modeling results and experimental measurements for the (1) spatial distribution of ƒ ν and (2) the non-linear variation of peak ƒ ν with strain rate, we further investigate the modeled sub-processes (nucleation, condensation, surface growth, and oxidation) using the LLNL model to analyze the assumptions in the reduced model framework. Furthermore, the results indicate a significant contribution from resonant radicals to the surface growth of soot particles, which are not accounted for in the current implementation of HMOM and could help reconcile soot predictions by the reduced model with observations.

Counterflow↗

Resonance-stabilized radical clustering bridges the gap between gaseous precursors and soot in the inception stage

Carbonaceous particles are widespread in combustion, atmospheric, extraterrestrial, and nanomaterials environments. Resonance-stabilized radicals (RSRs) are commonly identified in fuel combustion and pyrolysis processes and play an essential role in carbonaceous particle formation. Despite their importance, comprehensive experimental and mechanistic understanding of particle inception through RSR reactions is lacking. This work investigated particle size distribution, chemical composition, and thermal behavior of soot particles generated by the flow reactor pyrolysis reactions of typical RSRs, in particular, 1-indenyl, 1-methylnaphthyl, and 2-methylnaphthyl radicals, and by the pyrolysis of hydrocarbons with a variety of structures. Particle size distributions show soot particles with mobility diameters in an incipient-particle range of 1.3 to 1.6 nm. Laser desorption/ionization mass spectrometry results suggest that soot products consist of much larger covalently bound clusters (CBCs) than those observed in the gas phase. Under our experimental conditions, the CBCs exhibit a phase transition for particles with calculated molecular diameters of around 1.5 nm. Evaporation experiments and thermogravimetric analysis of the soot products reveal distinct thermal characteristics for small and large CBCs. These results implicate CBCs as bridges between gas-phase species and soot particles. The present work provides a soot-inception mechanism called RSR clustering (RSRC) that is characterized by the reactive clustering of RSRs. The RSRC mechanism contrasts with conventional soot formation models that attribute soot inception primarily to the aggregation of large-size polycyclic aromatic hydrocarbons.

carbonaceous particle↗

High temperature and pressure regime soot: Physical, optical and chemical signatures from high explosive detonations

Submicron particles are formed during the detonation and deflagration of carbon-rich energetic materials known as high explosives (HE) that can be lofted and transported long distances in the atmosphere. Particles include refractory species like soot, a.k.a. black carbon (BC), and have impacts to climate and human health at local, regional, and global scales. Here, we contrast detonation soot aerosol physical, optical and chemical properties that are formed more efficiently in terms of emission factors and ratios with traditional combustion sources from biomass burning and fossil fuels. We utilize ambient aerosol techniques for the first time to identify soot from two well-known HE's (1) Comp B-3: 40% trinitrotoluene (TNT) and 60% 1,3,5-trinitro-1,3,5-triazinane (RDX) and (2) PBX 9501: 95% 1,3,5,7-tetranitro-1,3,5,7-tetrazoctane (HMX) with 2.5% Estane and a 2.5% mixture of bis(2,2-dinitropropyl)-acetal (BDNPA) and bis(2,2-dinitropropyl)-formal (BDNPF). Size distributions, optical and chemical properties are presented. Aggregate soot had small mobility diameters (<100 nm) and unique optical and chemical signatures depending on the explosive composite composition, detonation atmosphere (e.g., air, argon) and pressure. Single-scattering albedos (SSA) from 0.3 to 0.8 and absorption Angstrom exponents (AAE) from 0.5 to 2.0 measured across 405–870 nm wavelengths depended on the explosive composite composition and detonation conditions. Comp B-3 detonation soot was similar to other combustion soot sources, whereas PBX 9501 soot had high scattering relative to absorption. Carbonaceous chemical signatures included the presence of fullerenes that were distinct from ambient and laboratory-generated soot surrogates and the detection of trace metals, including aluminum, copper, iron, and zinc.

36 MATERIALS SCIENCE↗

Measurements and Modeling of Soot Formation and Radiation in Microgravity Jet Diffusion Flames

This is a computational and experimental study for soot formation and radiative heat transfer in jet diffusion flames under normal gravity (1-g) and microgravity (0-g) conditions. Instantaneous soot volume fraction maps are measured using a full-field imaging absorption technique developed by the authors. A compact, self-contained drop rig is used for microgravity experiments in the 2.2-second drop tower facility at NASA Lewis Research Center. On modeling, we have coupled flame structure and soot formation models with detailed radiation transfer calculations. Favre-averaged boundary layer equations with a k-e-g turbulence model are used to predict the flow field, and a conserved scalar approach with an assumed Beta-pdf are used to predict gaseous species mole fraction. Scalar transport equations are used to describe soot volume fraction and number density distributions, with formation and oxidation terms modeled by one-step rate equations and thermophoretic effects included. An energy equation is included to couple flame structure and radiation analyses through iterations, neglecting turbulence-radiation interactions. The YIX solution for a finite cylindrical enclosure is used for radiative heat transfer calculations. The spectral absorption coefficient for soot aggregates is calculated from the Rayleigh solution using complex refractive index data from a Drude- Lorentz model. The exponential-wide-band model is used to calculate the spectral absorption coefficient for H20 and C02. It is shown that when compared to results from true spectral integration, the Rosseland mean absorption coefficient can provide reasonably accurate predictions for the type of flames studied. The soot formation model proposed by Moss, Syed, and Stewart seems to produce better fits to experimental data and more physically sound than the simpler model by Khan et al. Predicted soot volume fraction and temperature results agree well with published data for a normal gravity co-flow laminar flames and turbulent jet flames. Predicted soot volume fraction results also agree with our data for 1-g and 0-g laminar jet names as well as 1-g turbulent jet flames.

Ku, Jerry C.↗

The Impact of Buoyancy and Flame Structure on Soot, Radiation and NOx Emissions from a Turbulent Diffusion Flame

It is hypothesized that the spatial structure of a turbulent diffusion flame plays an important role in determining the emissions of radiative energy, soot and NO, from a combustor. This structure, manifested in the two point statistics, is influenced by buoyancy. Radiation, soot and NOx emissions are the cumulative result of processes that occur throughout a flame. For example, radiation fluxes along a line of sight can be found from summing up the contributions from sources in individual pockets of hot soot that emit, and from sinks in cold soot that absorb. Soot and NOx are both the results of slow chemistry and are not equilibrium products. The time that is available for production and burnout is crucial in determining the eventual emissions of these pollutants. Turbulence models generally rely on a single point closure of the appropriate time averaged equations. Hence, spatial information is lost and needs to be modeled using solution variables such as turbulence kinetic energy and dissipation rate, often with the assumption of isotropy. However, buoyancy can affect the physical structure of turbulent flames and can change the spatial extent of soot bearing regions. Theoretical comparisons with models are best done in the limit of infinite Froude number because the inclusion of buoyancy in flow models introduces significant uncertainties. Hence, LII measurements of soot, measurements of radiation fluxes from soot, Particle Imaging Velocimetry (PIV) of the flow field and measurements of post flame NOX will be carried out on the NASA Lewis 2.2 sec drop tower and eventually on the parabolic flight aircraft. The drop rig will be a modified version of a unit that has been successfully used at Lewis in the past.

Kennedy, I. M.↗

Carbon Nanostructure: Its Evolution During its Impact Upon Soot Growth and Oxidation

The proposed work is a ground-based study to define and quantify soot nanostructural changes in response to growth conditions, thermal and oxidative treatments and to quantify their impact upon further oxidation and growth of highly ordered carbon materials. Experimental data relating soot oxidation rates to multiple oxidizing species concentrations will directly test for additive or synergistic soot oxidation rates. Such validation is central for assessing the applicability of individual soot oxidation rates and designing oxidative strategies for controlling soot loadings in and emissions from turbulent combustion processes. Through these experiments, new insights into soot nanostructure evolution during and its impact upon oxidation by O2 and OH will be realized. It is expected that the results of this effort will spawn new research directions in future microgravity and 1g environments. Issues raised by positive or even negative demonstration of the hypotheses of this proposal have direct bearing on modelling and controlling soot formation and its destruction in nearly every combustion process producing soot.

Source record↗

Soot Formation in Laminar Premixed Ethylene/Air Flames at Atmospheric Pressure

Soot formation was studied within laminar premixed ethylene/air flames (C/O ratios of 0.78-0.98) stabilized on a flat-flame burner operating at atmospheric pressure. Measurements included soot volume fractions by both laser extinction and gravimetric methods, temperatures by multiline emission, soot structure by thermophoretic sampling and transmission electron microscopy, major gas species concentrations by sampling and gas chromatography, concentrations of condensable hydrocarbons by gravimetric sampling. and velocities by laser velocimetry. These data were used to find soot surface growth rates and primary soot particle nucleation rates along the axes of the flames. Present measurements of soot surface growth rates were correlated successfully by predictions based on typical hydrogen-abstraction/carbon-addition (HACA) mechanisms of Frenklach and co-workers and Colket and Hall. These results suavest that reduced soot surface growth rates with increasing residence time seen in the present and other similar flames were mainly caused by reduced rates of surface activation due to reduced H atom concentrations as temperatures decrease as a result of radiative heat losses. Primary soot particle nucleation rates exhibited variations with temperature and acetylene concentrations that were similar to recent observations for diffusion flames; however, nucleation rates in the premixed flames were significantly lower than in, the diffusion flames for reasons that still must be explained. Finally, predictions of yields of major gas species based on mechanisms from both Frenklach and co-workers and Leung and Lindstedt were in good agreement with present measurements and suggest that H atom concentrations (relevant to HACA mechanisms) approximate estimates based on local thermodynamic equilibrium in the present flames.

Xu, F.↗

Sooting Limits Of Diffusion Flames With Oxygen-Enriched Air And Diluted Fuel

Oxygen-enhanced combustion permits certain benefits and flexibility that are not otherwise available in the design of practical combustors, as discussed by Baukal. The cost of pure and enriched oxygen has declined to the point that oxygen-enhanced combustion is preferable to combustion in air for many applications. Carbon sequestration is greatly facilitated by oxygen enrichment because nitrogen can be eliminated from the product stream. For example, when natural gas (or natural gas diluted with CO2) is burned in pure oxygen, the only significant products are water and CO2. Oxygen-enhanced combustion also has important implications for soot formation, as explored in this work. We propose that soot inception in nonpremixed flames requires a region where C/O ratio, temperature, and residence time are above certain critical values. Soot does not form at low temperatures, with the threshold in nonpremixed flames ranging from about 1250-1650 K, a temperature referred to here as the critical temperature for soot inception, Tc. Soot inception also can be suppressed when residence time is short (equivalently, when the strain rate in counterflow flames is high). Soot induction times of 0.8-15 ms were reported by Tesner and Shurupov for acetylene/nitrogen mixtures at 1473 K. Burner stabilized spherical microgravity flames are employed in this work for two main reasons. First, this configuration offers unrestricted control over convection direction. Second, in steady state these flames are strain-free and thus can yield intrinsic sooting limits in diffusion flames, similar to the way past work in premixed flames has provided intrinsic values of C/O ratio associated with soot inception limits.

Sunderland, P. B.↗