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Soot propensity is studied numerically for an initially binary size, axisymmetric cluster of evaporating drops by defining it as the propensity for nucleation reations to occur; the study does not address physical or chemical processes ensuing after soot nucleation.
Radiometric data were obtained over a range of parametric test conditions at three positions along the length of an experimental combustor segment corresponding to the primary, intermediate, and dilution zones. The concentration of soot entrained in the combustion gases was calculated by a technique using spectral radiance measurements. Tests were conducted primarily with Jet A fuel, although limited data were taken with two fuels having higher aromatic content, diesel oil number 2 and a blend of 40 percent tetralin in Jet A fuel. Radiometric observation of the combustion gases indicated that the maximum total radiance peaked at the intermediate zone, which was located immediately upstream of the dilution holes. Soot concentrations calculated from optical measurements in the dilution zone compared favorably with those obtained by in situ gas sampling at the exhaust. The total radiance increased with the higher aromatic content fuels.
The practicability of using a classical light-scattering technique, involving comparison of angular scattering intensity patterns with theoretically determined Mie and Rayleight patterns, to detect discrete soot particles (diameter less than 50 nm) in premixed propane/air and propane/oxygen-helium flames is considered. The experimental apparatus employed in this investigation included a laser light source, a flat-flame burner, specially coated optics, a cooled photomultiplier detector, and a lock-in voltmeter readout. Although large, agglomerated soot particles were detected and sized, it was not possible to detect small, discrete particles. The limiting factor appears to be background scattering by the system's optics.
An investigation of hardware configurations which attempt to minimize carbon and soot-production without sacrificing performance in small gas turbine combustors was conducted. Four fuel injectors, employing either airblast atomization, pressure atomization, or fuel vaporization techniques were combined with nozzle air swirlers and injector sheaths. Eight configurations were screened at sea-level takeoff and idle test conditions. Selected configurations were focused upon in an attempt to quantify the influence of combustor pressure, inlet temperature, primary zone operation, and combustor loading on soot and carbon formation. Cycle tests were also performed. It was found that smoke emission levels depended on the combustor fluid mechanics, the atomization quality of the injector and the fuel hydrogen content.
An analytical program was conducted to compute the soot and NOx emissions from a combustor and the radiation heat transfer to the combustor walls. The program involved the formulation of an emission and radiation model and the incorporation of this model into the Garrett 3-D Combustor Perfomance Computer Program. Computations were performed for the idle, cruise, and take-off conditions of a JT8D can combustor. The predicted soot and NOx emissions and the radiation heat transfer to the combustor walls agree reasonably well with the limited experimental data available.
An experimental program on the catalytic oxidation of iso-octane demonstrated the feasibility of the two-stage combustion system for reducing particulate emissions. With a fuel-rich (phi = 4.8 to 7.8) catalytic combustion preburner as the first stage the combustion process was soot free at reactor outlet temperatures of 1200 K or less. Although soot was not measured directly, its absence was indicated. Reaction products collected at two positions downstream of the catalyst bed were analyzed on a gas chromatograph. Comparison of these products indicated that pyrolysis of the larger molecules continued along the drift tube and that benzene formation was a gas-phase reaction. The effective hydrogen-carbon ratio calculated from the reaction products increased by 20 to 68 percent over the range of equivalence ratios tested. The catalytic partial oxidation process also yielded a large number of smaller-containing molecules. The fraction of fuel carbon in compounds having two or fewer carbon atoms ranged from 30 percent at 1100 K to 80 percent at 1200 K.
Temperature and velocity profiles are presented for cyclohexane, n-heptane, and iso-octane free, laminar, boundary layer, sooting, diffusion flames. Temperatures are measured with 3 mil Pt/Pt-13 percent Rh thermocouples. Corrected gas temperatures are derived by performing an energy balance of convection to and radiation from the thermocouple bead incorporating the variation of air conductivity and platinum emissivity with temperature. Velocities are measured using laser doppler velocimetry techniques. Profiles are compared with previously reported analytic temperature and velocity fields. Comparison of theoretical and experimental temperature profiles suggests improvement in the analytical treatment is needed, which accounts more accurately for the local soot radiation. The velocity profiles are in good agreement, with the departure of the theory from observation partially due to the small fluctuations inherent in these free flows.
The impact of thermodynamic parameters on the sensitivity of model predictions of soot formation by shock-tube pyrolysis of acetylene were assessed analytically. The pyrolysis process was treated as having three components: initiation, the initial pyrolysis stages; cyclization, formation of larger molecules and radicals and small aromatic molecules; and polymerization, further growth of aromatic rings. Rate equations are reviewed for each component. Thermodynamic effects were assessed by varying the C2H-H and C2H3-H bond energies and the Ct-(Ct) group additivity value. Any change in the C2H-H bond energy had a significant impact on the temperature and the maximum amount of the soot yield. The findings underscore the necessity of using accurate thermodynamic data for modeling high-temperature chemical kinetics.
Flame temperatures in nonsooting and sooting environments were successfully measured by radiometry for pre-mixed propane-oxygen laminar flames stabilized on a water-cooled, porous sintered-bronze burner. The measured temperatures in the nonsooting flames were compared with fine-wire thermocouple measurements. The results show excellent agreement below 1700 K, and when the thermocouple measurements were corrected for radiation effects, the agreement was good for even higher temperatures. The benefits of radiometry are: (1) the flow is not disturbed by an intruding probe, (2) calibration is easily done using a blackbody source, and (3) measurements can be made even with soot present. The theory involved in the radiometry measurements and the energy balance calculations used to correct the thermocouple temperature measurements are discussed.
The formation of carbon dust in the outflow from stars and the subsequent evolution of this so called stardust in the interstellar medium is reviewed. The chemical and physical processes that play a role in carbon stardust formation are very similar to those occurring in sooting flames. Based upon extensive laboratory studies of the latter, the structure and physical and chemical properties of carbon soot are reviewed and possible chemical pathways towards carbon stardust are discussed. Grain-grain collisions behind strong interstellar shocks provide the high pressures required to transform graphite and amorphous carbon grains into diamond. This process is examined and the properties of shock-synthesized diamonds are reviewed. Finally, the interrelationship between carbon stardust and carbonaceous meteorites is briefly discussed.
Soot enters the stratosphere either from the troposphere in deep thunderstorm convection, predominantly in the tropics, from midlatitude forest fires, and directly from aircraft flying above the tropopause. Particles emitted from jet aircraft are relatively ineffective as cloud droplet condensation nuclei (less than 1 percent) compared with those from forest fires (above 50 percent). Chemical and other modification during aging of the particles may influence these results in some circumstances; cloud nucleating properties can be used as a soot tracer. Such aerosols, as they grow to haze drops and ilute in increasing humidity, may form ice particles in the cold polar stratosphere or in tropical cumuli anvils at 18 to 20 km altitude at temperatures as low as -90 C. Ice may also form as particles are removed by descent through troposphere folds and enter midlatitude cirrus at levels below -40 C. In the stratosphere, ice particles may provide surfaces that catalyze heterogeneous chemical reactions; in the upper troposphere, the optical depths of cirrus clouds may be significantly increased.
Neither methane nor liquefied natural gas (LNG) produces soot when burned in turbine simulator with liquid oxygen under conditions like those in gas-generator section of rocket engine. Experiments conducted to determine if these fuels behave similarly to other hydrocarbon fuels, which give off soot coating turbomachinery and reducing performance.
The study of the burning of a single droplet is an ideal problem from which to gain fundamental understanding of diffusion flame characteristics. Droplet combustion is a complex physico-chemical process that involves a chemically-reacting two-phase flow with phase changes and yet simple experiments and analysis can be used to attain important insights into the burning rate, flame dynamics, kinetic extinction and disruption processes. It is a subject that has been actively studied for the past 40 years with most of the fundamental experiments being performed under reduced-gravity conditions for direct comparisons with theoretical/computational analyses that invoke spherical symmetry assumptions. In the earlier studies, the effects of sooting on the overall burning characteristics were not considered. However, recent microgravity investigations performed at the NASA-LeRC droptowers (Droplet Combustion Experiment) and others indicate that effects of soot and sootcloud formation may be significant during the lifetime of the droplet and therefore must be included in the analysis.
A four-channel laser transmissometer has been used to probe the soot content of the exhaust plume of the X-34 60k-lb thrust Fastrac rocket engine at NASA's Marshall Space Flight Center. The transmission measurements were made at an axial location approximately equal 1.65 nozzle diameters from the exit plane and are interpreted in terms of homogeneous radial zones to yield extinction coefficients from 0.5-8.4 per meter. The corresponding soot mass density, spatially averaged over the plume cross section, is, for Rayleigh particles, approximately equal 0.7 microgram/cc, and alternative particle distributions are briefly considered. Absolute plume radiance at the laser wavelength (515 nm) is estimated from the data at approximately equal 2,200 K equivalent blackbody temperature, and temporal correlations in emission from several spatial locations are noted.
A four-channel laser transmissometer has been used to probe the soot content of the exhaust plume of the X-34 60k-lb thrust Fastrac rocket engine at NASA's Marshall Space Flight Center. The transmission measurements were made at an axial location about equal 1.65 nozzle diameters from the exit plane and are interpreted in terms of homogeneous radial zones to yield extinction coefficients from 0.5-8.4 per meter. The corresponding soot mass density, spatially averaged over the plume cross section, is, for Rayleigh particles, approximately equal to 0.7 micrograms/cubic cm and alternative particle distributions are briefly considered. Absolute plume radiance at the laser wavelength (515 nm) is estimated from the data at approximately equal to 2.200 K equivalent blackbody temperature, and temporal correlations in emission from several spatial locations are noted.
This paper summarizes recent studies of the effects of stoichiometric mixture fraction (structure) and hydrodynamics on soot particle inception and flame extinction in diffusion flames. Microgravity experiments are uniquely suited for these studies because, unlike normal gravity experiments, they allow structural and hydrodynamic effects to be independently studied. As part of this recent flight definition program, microgravity studies have been performed in the 2.2 second drop tower. Normal gravity counterflow studies also have been employed and analytical and numerical models have been developed. A goal of this program is to develop sufficient understanding of the effects of flame structure that flames can be "designed" to specifications - consequently, the program name Flame Design. In other words, if a soot-free, strong, low temperature flame is required, can one produce such a flame by designing its structure? Certainly, as in any design, there will be constraints imposed by the properties of the available "materials." For hydrocarbon combustion, the base materials are fuel and air. Additives could be considered, but for this work only fuel, oxygen and nitrogen are considered. Also, the structure of these flames is "designed" by varying the stoichiometric mixture fraction. Following this line of reasoning, the studies described are aimed at developing the understanding of flame structure that is needed to allow for optimum design.
Hypotheses of global wildfires following the Cretaceous-Tertiary (KT) boundary impact are supported by high concentrations of elemental carbon (3.6 mg cm-3) and soot (1.8 mg cm-2) in DSDP Site 465, which was located several thousand kilometers from potential continental sources at 65 Ma. Soot is not preserved at four other central Pacific KT localities, but this is attributed to loss during oxic diagenesis. We find no evidence for wildfires related to major impacts in the late Eocene or to Ir anomalies and extinctions in the late Cenomanian.
Studies of soot oxidation have ranged from in situ flame studies to shock tubes to flow reactors. Each of these systems possesses particular advantages and limitations related to temperature, time and chemical environments. Despite the aforementioned differences, these soot oxidation investigations share three striking features. First and foremost is the wide variation in the rates of oxidation. Reported oxidation rates vary by factors of +6 to - 20 relative to the Nagle Strickland-Constable (NSC) rate for graphite oxidation [3]. Rate variations are not surprising, as the temperatures, residence times, types of oxidants and methods of oxidation differ from study to study. Nevertheless, a valid explanation for rate differences of this magnitude has yet to be presented.