Non-premixed oxy-fuel combustion of natural gas is used in industrial applications where high-intensity heat is required, such as glass manufacturing and metal forging and shaping. In these applications, the high flame temperatures achieved by oxy-fuel combustion increase radiative heat transfer to the surfaces of interest and soot formation within the flame is desired for further augmentation of radiation. However, the high cost of cryogenic air separation has limited the penetration of oxy-fuel combustion technologies. New approaches to air separation are being developed that may reduce oxygen production costs, but only for intermediate levels of oxygen enrichment of air. To determine the influence of oxygen enrichment on soot formation and radiation, we developed a non-premixed coannular burner in which oxygen concentrations and oxidizer flow rates can be independently varied, to distinguish the effects of turbulent mixing intensity from oxygen enrichment on soot formation and flame radiation. Local radiation intensities, soot concentrations, and soot temperatures have been measured using a thin-film thermopile, planar laser-induced incandescence (LII), and two-color imaging pyrometry, respectively. The measurements show that soot formation increases as the oxygen concentration decreases from 100% to 50%, helping to moderate a decrease in overall flame radiation. An increase in turbulence intensity has a marked effect on flame height, soot formation and thermal radiation, leading to decreases in all of these. The soot temperature decreases with a decrease in the oxygen concentration and increases with an increase in turbulent mixing intensity. Altogether, the results suggest that properly designed oxygen-enriched burners that enhance soot formation for intermediate levels of oxygen purity may be able to achieve thermal radiation intensities as high as 85% of traditional oxy-fuel burners utilizing high-purity oxygen.
Truly quantifying soot concentrations within turbulent flames is a difficult prospect. Laser extinction measurements are constrained by spatial resolution limitations and by uncertainty in the local soot extinction coefficient. Laser-induced incandescence (LII) measurements rely on calibration against extinction and thereby are plagued by uncertainty in the extinction coefficient. In addition, the LII measurements are subject to signal trapping in flames with significant soot concentrations and/or flame widths. In the study reported here, a turbulent ethylene non-premixed jet flame (jet exit Reynolds number of 20,000) is investigated by a combination of LII and full-flame HeNe laser (633 nm) extinction measurements. The LII measurements have been calibrated against extinction measurements in a laminar ethylene flame. An extinction coefficient previously measured in laminar ethylene flames is used as the basis of the calibration. The time-Averaged LII data in the turbulent flame has been corrected for signal trapping, which is shown to be significant in this flame, and then the line-of-sight extinction for a theoretical 633 nm light source has been calculated acrob the LII-determined soot concentration field. Comparison of the LII-based extinction with that actual measured along the flame centerline is favorable, showing an average deviation of approximately 10%. This lends credence to the measured values of soot concentrations in the flame and also gives a good indication of the level of uncertainty in the measured soot concentrations, subject to the additional uncertainty in the previously measured extinction coefficient, estimated to be ±15%.
Oxy-fuel combustion is a well-known approach to improve the heat transfer associated with stationary energy processes. Its overall penetration into industrial and power markets is constrained by the high cost of existing air separation technologies for generating oxygen. Cryogenic air separation is the most widely used technology for generating oxygen but is complex and expensive. Pressure swing adsorption is a competing technology that uses activated carbon, zeolites and polymer membranes for gas separations. However, it is expensive and limited to moderate purity O₂ . MOFs are cutting edge materials for gas separations at ambient pressure and room temperature, potentially revolutionizing the PSA process and providing dramatic process efficiency improvements through oxy-fuel combustion. This LDRD combined (1) MOF synthesis, (2) gas sorption testing, (3) MD simulations and crystallography of gas siting in pores for structure-property relationship, (4) combustion testing and (5) technoeconomic analysis to aid in real-world implementation.
Future energy systems based on gasification of coal or biomass for co-production of electrical power and fuels may require gas turbine operation on unusual gaseous fuel mixtures. In addition, global climate change concerns may dictate the generation of a CO2 product stream for end-use or sequestration, with potential impacts on the oxidizer used in the gas turbine. In this study the operation at atmospheric pressure of a small, optically accessible swirl-stabilized premixed combustor, burning fuels ranging from pure methane to conventional and H2-rich and H2-lean syngas mixtures is investigated. Both air and CO2-diluted oxygen are used as oxidizers. CO and NOx emissions for these flames have been determined from the lean blowout limit to slightly rich conditions (1.03). In practice, CO2-diluted oxygen systems will likely be operated close to stoichiometric conditions to minimize oxygen consumption while achieving acceptable NOx performance. The presence of hydrogen in the syngas fuel mixtures results in more compact, higher temperature flames, resulting in increased flame stability and higher NOx emissions. Consistent with previous experience, the stoichiometry of lean blowout decreases with increasing H2 content in the syngas. Similarly, the lean stoichiometry at which CO emissions become significant decreases with increasing H2 content. For the mixtures investigated, CO emissions near the stoichiometric point do not become significant until 0.95. At this stoichiometric limit, CO emissions rise more rapidly for combustion in O2-CO2 mixtures than for combustion in air.
Future energy systems based on gasification of coal or biomass for co-production of electrical power and gaseous or liquid fuels may require gas turbine operation on unusual fuel mixtures. In addition, global climate change concerns may dictate the production of a CO2 product stream for end-use or sequestration, with potential impacts on the oxidizer used in the gas turbine. In this study the operation at atmospheric pressure of a small, optically accessible swirl-stabilized premixed combustor, burning fuels ranging from pure methane to conventional and H2-rich and H2-lean syngas mixtures is investigated. Both air and CO2-diluted oxygen are used as the oxidizers. CO and NOx emissions for these flames have been determined over the full range of stoichiometrics from the lean blow-off limit to slightly rich conditions (φ ∼ 1.03). The presence of hydrogen in the syngas fuel mixtures results in more compact, higher temperature flames, resulting in increased flame stability and higher NOx emissions. The lean blowoff limit and the lean stoichiometry at which CO emissions become significant both decrease with increasing H2 content in the syngas. For the investigated mixtures, CO emissions near the stoichiometric point do not become significant until (φ > 0.95. At this stoichiometric limit, where dilute-oxygen power systems would preferably operate, CO emissions rise more rapidly for combustion in O2-CO2 mixtures than for combustion in air.
Flame heights of co-flowing cylindrical ethylene-air and methane-air laminar inverse diffusion flames were measured. The luminous flame height was found to be greater than the height of the reaction zone determined by planar laser-induced fluorescence (PLIF) of hydroxyl radicals (OH) because of luminous soot above the reaction zone. However, the location of the peak luminous signals along the centerline agreed very well with the OH flame height. Flame height predictions using Roper's analysis for circular port burners agreed with measured reaction zone heights when using values for the characteristic diffusion coefficient and/or diffusion temperature somewhat different from those recommended by Roper. The fact that Roper's analysis applies to inverse diffusion flames is evidence that inverse diffusion flames are similar in structure to normal diffusion flames.
The dimensionless extinction coefficient (K{sub e}) of soot must be known to quantify laser extinction measurements of soot concentration and to predict optical attenuation through smoke clouds. Previous investigations have measured K{sub e} for post-flame soot emitted from laminar and turbulent diffusion flames and smoking laminar premixed flames. This paper presents the first measurements of soot K{sub e} from within laminar diffusion flames, using a small extractive probe to withdraw the soot from the flame. To measure K{sub e}, two laser sources (635 nm and 1310 nm) were coupled to a transmission cell, followed by gravimetric sampling. Coannular diffusion flames of methane, ethylene and nitrogen-diluted kerosene burning in air were studied, together with slot flames of methane and ethylene. K{sub e} was measured at the radial location of maximum soot volume fraction at several heights for each flame. Results for K{sub e} at both 635 nm and 1310 nm for ethylene and kerosene coannular flames were in the range of 9-10, consistent with the results from previous studies of post-flame soot. The ethylene slot flame and the methane flames have lower K{sub e} values, in some cases as low as 2.0. These lower values of K{sub e} are found to result from the contributions of (a) the condensation of PAH species during the sampling of soot, (b) the wavelength-dependent absorptivity of soot precursor particles, and, in the case of methane, (c) the negligible contribution of soot scattering to the extinction coefficient. RDG calculations of soot scattering, in combination with the measured K{sub e} values, imply that the soot refractive index is in the vicinity of 1.75-1.03i at 635 nm.
Fires pose the dominant risk to the safety and security of nuclear weapons, nuclear transport containers, and DOE and DoD facilities. The thermal hazard from these fires primarily results from radiant emission from high-temperature flame soot. Therefore, it is necessary to understand the local transport and chemical phenomena that determine the distributions of soot concentration, optical properties, and temperature in order to develop and validate constitutive models for large-scale, high-fidelity fire simulations. This report summarizes the findings of a Laboratory Directed Research and Development (LDRD) project devoted to obtaining the critical experimental information needed to develop such constitutive models. A combination of laser diagnostics and extractive measurement techniques have been employed in both steady and pulsed laminar diffusion flames of methane, ethylene, and JP-8 surrogate burning in air. For methane and ethylene, both slot and coannular flame geometries were investigated, as well as normal and inverse diffusion flame geometries. For the JP-8 surrogate, coannular normal diffusion flames were investigated. Soot concentrations, polycyclic aromatic hydrocarbon (PAH) laser-induced fluorescence (LIF) signals, hydroxyl radical (OH) LIF, acetylene and water vapor concentrations, soot zone temperatures, and the velocity field were all successfully measured in both steady and unsteady versions of these various flames. In addition, measurements were made of the soot microstructure, soot dimensionless extinction coefficient (&), and the local radiant heat flux. Taken together, these measurements comprise a unique, extensive database for future development and validation of models of soot formation, transport, and radiation.
The structure of laminar inverse diffusion flames (IDF) of methane and ethylene in air was studied using a cylindrical co-flowing burner. IDF were similar to normal diffusion flames, except that the relative positions of the fuel and oxidizer were reversed. Radiation from soot surrounding the IDF masked the reaction zone in visible images. As a result, flame heights determined from visible images were overestimated. The height of the reaction zone as indicated by OH LIF was a more relevant measure of height. The concentration and position of PAH and soot were observed using LIF and laser-induced incandescence (LII). PAH LIF and soot LII indicated that PAH and soot are present on the fuel side of the flame, and that soot is located closer to the reaction zone than PAH. Ethylene flames produced significantly higher PAH LIF and soot LII signals than methane flames, which was consistent with the sooting propensity of ethylene. The soot and PAH were present on the fuel side of the reaction zone, but the soot was closer to the reaction zone than the PAH. This is an abstract of a paper presented at the 30th International Symposium on combustion (Chicago, IL 7/25-30/2004).