Effect of high CO2 concentration on char formation through mineral reaction during biomass pyrolysis

O₂/CO₂ combustion has attracted considerable attention as a promising technology for CO₂ capture. Using biomass for fuel is considered carbon neutral, and O₂/CO₂ biomass combustion can mitigate the deleterious environmental effect of greenhouse. In this study, the effect of CO₂, the main component gas in O₂/CO₂ combustion, on the pyrolysis characteristics of biomass is investigated. Cellulose, lignin, and metal-depleted lignin pyrolysis experiments were performed using a thermobalance. Information on the surface chemistry of the chars was obtained by Fourier transform infrared (FTIR) spectroscopy to investigate changes in the surface chemistry during pyrolysis under different surrounding gasses. When the temperature increased to 1073 K at heating rate of 1 K s^?1, the char yield of lignin in the presence of CO₂ increased by about 10% compared with that under Ar. However, for cellulose and metal-depleted lignin, no significant difference appeared between pyrolysis under CO₂ and that under Ar. FT-IR showed that a strong peak corresponding to carbonate ions appeared in the char derived from lignin under CO₂. Therefore, salts such as Na₂CO₃ or K₂CO₃ formed during the lignin pyrolysis under CO₂. At around 1650–1770 cm^?1, a significant difference appeared in the FTIR spectra of chars formed under CO₂ and those formed under Ar. C=O groups not associated with an aromatic ring were found only in chars formed under CO₂. It was suggested that these salts affected the char formation reaction, in that the char formed during lignin pyrolysis under CO₂ had unique chemical bands that did not appear in the lignin-derived char prepared under Ar.     

Particle imaging of ignition and devolatilization of pulverized coal during oxy-fuel combustion

Oxy-fuel combustion of coal is a promising technology for cost-effective power production with carbon capture and sequestration that has ancillary benefits of emission reductions and lower flue gas cleanup costs. To fully understand the results of pilot-scale tests of oxy-fuel combustion and to accurately predict scale-up performance through CFD modeling, fundamental data are needed concerning coal and coal char combustion properties under these unconventional conditions. In the work reported here, the ignition and devolatilization characteristics of both a high-volatile bituminous coal and a Powder River Basin subbituminous coal were analyzed in detail through single-particle imaging at a gas temperature of 1700 K over a range of 12–36 vol % O₂ in both N₂ and CO₂ diluent gases. The bituminous coal images show large, hot soot cloud radiation whose size and shape vary with oxygen concentration and, to a lesser extent, with the use of N₂ versus CO₂ diluent gas. Subbituminous coal images show cooler, smaller emission signals during devolatilization that have the same characteristic size as the coal particles introduced into the flow (nominally 100 μm). The measurements also demonstrate that the use of CO₂ diluent retards the onset of ignition and increases the duration of devolatilization, once initiated. For a given diluent gas, a higher oxygen concentration yields shorter ignition delay and devolatilization times. The effect of CO₂ on coal particle ignition is explained by its higher molar specific heat and its tendency to reduce the local radical pool. The effect of O₂ on coal particle ignition results from its effect on the local mixture reactivity. CO₂ decreases the rate of devolatilization because of the lower mass diffusivity of volatiles in CO₂ mixtures, whereas higher O₂ concentrations increase the mass flux of oxygen to the volatiles flame and thereby increase the rate of devolatilization.     

A mechanistic char oxidation model consistent with observed CO2/CO production ratios

Reliable prediction of char conversion, heat release, and particle temperature during heterogeneous char oxidation relies upon quantitative calculation of the CO₂/CO production ratio. This ratio depends strongly on the surface temperature, but also on the local partial pressure of oxygen and thus becomes more important in simulations of oxy-fuel or pressurized combustion systems. Existing semi-empirical intrinsic kinetic models of char combustion have been calibrated against the temperature-dependence of the CO₂/CO production ratio, but have neglected the effect of the local oxygen concentration. In this study we employ steady-state analysis to demonstrate the limitations of the existing 3-step semi-global kinetics models and to show the necessity of using a 5-step model to adequately capture the temperature- and oxygen-dependence of the CO₂/CO production ratio. A suitable 5-step heterogeneous reaction mechanism is developed and its rate parameters fit to match CO₂/CO production data, global reaction orders, and activation energies reported in the literature. The model predictions are interrogated for a broad range of conditions characteristic of pressurized, oxy-fuel, and conventional high-temperature char combustion, for which essentially no experimental information on the CO₂/CO production ratio is available. The results suggest that the CO₂/CO production ratio may be considerably lower than that estimated with existing power-law correlations for oxygen partial pressures less than 10 kPa and surface temperatures higher than 1600 K. To assist with implementation of the mechanistic CO₂/CO production ratio results, an analytical procedure for calculating the CO₂/CO production ratio is presented.     

Comparing reaction orders of anthracite chars with bituminous coal chars at high temperature oxidation conditions

The influence of concentration of oxygen on the oxidation rates of 5 anthracite chars is investigated at gas temperatures ranging from 1223 K to 1673 K. Reaction orders and kinetic parameters are determined with a multivariable optimization method in which modeled burnout profiles are fitted to experimental burnout profiles from a 4 m isothermal plug flow reactor operating at industrially realistic heating rates, i.e., 10⁴–10⁵ K/s. The determined reaction orders are compared to reaction orders of 10 bituminous coal chars investigated at similar conditions in a previous study. The results show that the optimized reaction order of the anthracite chars is zero, while the reaction order of the bituminous coal char is one. The difference in the reaction orders cannot be explained by using the two semi-global oxidation reactions: C(O) + O₂ → CO/CO₂ and C(O) → CO. However, by also considering 2C(O) → CO₂ + C as a possible reaction step, the reaction order difference between the anthracite chars and the bituminous coal chars can be explained. In addition, a first attempt to apply the same multivariable optimization method to determine the reaction order for a biomass char is presented.     

A comparative study of FESEM and EDX analyses of Datong coal in N2 and CO2 environments

Field emission scanning electron microscopy, energy-dispersive X-ray spectroscopy and Brunauer Emmett Teller surface area analyses of char produced in CO₂ and N₂ environments in a thermo-gravimetric analyzer, using thermo-plus II software, were investigated under different parametric conditions. These conditions include temperature, flow rate variations etc. for the implementation of oxy-fuel combustion technology. It was observed that, at high temperatures and low flow rates, the mass loss rate of coal in CO₂ was higher than in that of a N₂ environment. This may be due to one additional step of coal gasification i.e. char gasification by CO₂ at higher temperature. More importantly, during the reaction with CO₂ the formations of perfectly hexagonal nanorods at the particular temperature of 773 K were observed. However, the amount of these nanorods decreases and the dimensions i.e. size and shape change (smaller aspect ratio) with the increase of flow rate and temperature as well. The formation of these nanorods are attracted much because of their peculiar properties and potential applications in functional nano-devices and environmentally clean energy purposes i.e. CO₂ capturing.     

Mechanism on the contribution of coal/char fragmentation to fly ash formation during pulverized coal combustion

In this paper, the correlations between coal/char fragmentation and fly ash formation during pulverized coal combustion are investigated. We observed an explosion-like fragmentation of Zhundong coal in the early devolatilization stage by means of high-speed photography in the Hencken flat-flame burner. While high ash-fusion (HAF) bituminous and coal-derived char samples only undergo gentle perimeter fragmentation in the char burning stage. Simultaneously, combustion experiments of two kinds of coals were conducted in a 25?kW down-fired combustor. The particle size distributions (PSDs) of both fine particulates (PM_1-10) and bulk fly ash (PM₁₀₊) were measured by Electrical Low Pressure Impactor (ELPI) and Malvern Mastersizer 2000, respectively. The results show that the mass PSD of residual fly ash (PM₁₊) from Zhundong coal exhibits a bi-modal shape with two peaks located at 14?µm and 102?µm, whereas that from HAF coal only possesses a single peak at 74?µm. A hybrid model accounting for multiple-route ash formation processes is developed to predict the PSD of fly ash during coal combustion. By incorporating coal/char fragmentation sub-models, the simulation can quantitatively reproduce the measured PM₁₊ PSDs for different kinds of coals. The sensitivity analysis further reveals that the bi-modal mass distribution of PM₁₊ intrinsically results from the coal fragmentation during devolatilization.     

Measurements and modelling of oxy-fuel coal combustion

Oxy-fuel combustion is one of the most promising technologies to isolate efficiently and economically CO₂ emissions in coal combustion for the ready carbon sequestration. The high proportions of both H₂O and CO₂ in the furnace have complex impacts on flame characteristics (ignition, burnout, and heat transfer), pollutant emissions (NO_x, SO_x, and particulate matter), and operational concerns (ash deposition, fouling/slagging). In contrast to the existing literature, this review focuses on fundamental studies on both diagnostics and modelling aspects of bench- or lab-scale oxy-fuel combustion and, particularly, gives attention to the correlations among combustion characteristics, pollutant formation, and operational ash concerns. First, the influences of temperature and species concentrations (e.g., O₂, H₂O) on coal ignition, volatile combustion and char burning processes, for air- and oxy-firing, are comparatively evaluated and modelled, on the basis of data from optically-accessible set-ups including flat-flame burner, drop-tube furnace, and down-fired furnace. Then, the correlations of combustion-generated particulate/NO_x emissions with changes of combustion characteristics in both air and oxy-fuel firing modes are summarized. Additionally, ash deposition propensity, as well as its relation to the formation of fine particulates (i.e. PM_0.2, PM₁ and PM₁₀), for both modes are overviewed. Finally, future research topics are discussed. Fundamental oxy-fuel combustion research may provide an ideal alternative for validating CFD simulations toward industrial applications.     

The structure and extinction of nonpremixed methane/nitrous oxide and ethane/nitrous oxide flames

Knowledge of combustion of hydrocarbon fuels with nitrogen-containing oxidizers is a first step in understanding key aspects of combustion of hypergolic and gun propellants. Here an experimental and kinetic-modeling study is carried out to elucidate aspects of nonpremixed combustion of methane (CH₄) and nitrous oxide (N₂O), and ethane (C₂H₆) and N₂O. Experiments are conducted, at a pressure of 1 atm, on flames stabilized between two opposing streams. One stream is a mixture of oxygen (O₂), nitrogen (N₂), and N₂O, and the other a mixture of CH₄ and N₂ or C₂H₆ and N₂. Critical conditions for extinction are measured. Kinetic-modeling studies are performed with the San Diego Mechanism. Experimental data and results of kinetic-modeling show that N₂O inhibits the flame by promoting extinction. Analysis of the flame structure shows that H radicals are produced in the overall chain-branching step 3H₂ + O₂ ? 2H₂O + 2H, in which molecular hydrogen is consumed. Hydrogen is also consumed in the overall step N₂O + H₂ ? N₂ + H₂O where stable products are formed. Inhibition of the flames by N₂O is attributed to competition between these two overall steps.     

Optimization of gas pressures ratio in a fast-axial-flow CO2 laser with genetic algorithm

In this paper, the laser output power of a fast-axial flow CO₂ laser was optimized with gas pressures ratio of CO₂:N₂:He using a genetic algorithm technique. The power of laser was increased from 500 W (un-optimized case) to 2200 W (simulated case), also experimentally the power has achieved the value of 700 W (optimized case).     

Measurements of H2O2 in low temperature dimethyl ether oxidation

H₂O₂ is one of the most important species in dimethyl ether (DME) oxidation, acting not only as a marker for low temperature kinetic activity but also responsible for the “hot ignition” transition. This study reports, for the first time, direct measurements of H₂O₂ and CH₃OCHO, among other intermediate species concentrations in helium-diluted DME oxidation in an atmospheric pressure flow reactor from 490 to 750 K, using molecular beam electron-ionization mass spectrometry (MBMS). H₂O₂ measurements were directly calibrated, while a number of other species were quantified by both MBMS and micro gas chromatography to achieve cross-validation of the measurements. Experimental results were compared to two different DME kinetic models with an updated rate coefficient for the H + DME reaction, under both zero-dimensional and two-dimensional physical model assumptions. The results confirm that low and intermediate temperature DME oxidation produces significant amounts of H₂O₂. Peroxide, as well as O₂, DME, CO_, and CH₃OCHO profiles are reasonably well predicted, though profile predictions for H₂/CO₂ and CH₂O are poor above and below ～625 K, respectively. The effect of the collisional efficiencies for the H + O₂ + M = HO₂ + M reaction on DME oxidation was investigated by replacing 20% He with 20% CO₂. Observed changes in measured H₂O₂ concentrations agree well with model predictions. The new experimental characterizations of important intermediate species including H₂O₂, CH₂O and CH₃OCHO, and a path flux analysis of the oxidation pathways of DME support that kinetic parameters for decomposition reactions of HOCH₂OCO and HCOOH directly to CO₂ may be responsible for model under-prediction of CO₂. The H abstraction reactions for DME and/or CH₂O and the unimolecular decomposition of HOCH₂O merit further scrutiny towards improving the prediction of H₂ formation.     

The influence of some processing conditions on host crystal structure and phosphorescence properties of SrAl2O4:Eu2+, Dy3+ nanoparticle pigments synthesized by combustion technique

The spectroscopic and host phase properties of SrAl₂O₄:Eu²⁺, Dy³⁺ phosphors with a series of different initiating combustion temperature, urea concentration as a fuel and critical pH of precursor solution are investigated. The SrAl₂O₄:Eu²⁺, Dy³⁺ nanoparticle pigments were obtained by exothermic combustion process within less than 5 min. The sample that ignited at initiating combustion temperature of 600 °C exhibits highest intensity emission peak at 517 nm in which the SrAl₂O₄ host phase has the maximum fraction of monoclinic SrAl₂O₄ phase. The excitation spectra consist of 240 and 254 nm broad peaks. The experimental results show that the optimum ratio of urea is 2.5 times higher than theoretical quantities for best emission condition of SrAl₂O₄:Eu²⁺, Dy³⁺ phosphor particles. The critical pH was obtained about 5.2. The crystallite size of these pigments is about 40 nm before thermal treatment and 62 nm after thermal treatment, respectively.     

N2 emission-channel change in NO reduction over stepped Pd(211) by angle-resolved desorption

A sharp change in the N₂ emission channel from N₂O(a) → N₂(g) + O(a) to N(a) + N(a) → N₂(g) has been found at around 500 K in a steady-state NO + D₂ reaction over stepped Pd(211) = [(S)3(111) × (100)] by means of angle-resolved desorption. The desorbing N₂ is highly collimated at around 30° off normal toward the step-down direction below about 500 K due to the intermediate N₂O decomposition, whereas, above 500 K, the near normally directed desorption due to the recombination of N(a) is relatively enhanced. The N₂O decomposition channel is promoted when the reaction is carried out with hydrogen (deuterium) and the channel change is accelerated by quick changes of the amounts of surface hydrogen and oxygen (or NO(a)) into the opposite directions, and enhanced nitrogen removal as ammonia on the resultant hydrogen-rich surface. In the steady-state NO + CO reaction, the N₂ emission channel gradually changes above 500 K toward recombination. A model for the off-normal N₂ emission is briefly described.     

Submillimeter-wave measurements of N2 and O2 pressure broadening for HO2 radical generated by Hg-photosensitized reaction

The N₂ and O₂ pressure broadening coefficients of the pure rotational transitions at 625.66 GHz (N_KaKc=10_1?9–10_0?10, J=10.5–10.5) and 649.70 GHz (N_KaKc=10_2?9–9_2?8, J=9.5–8.5) in the vibronic ground state X²A′ of the perhydroxyl (HO₂) radical have been determined by precise laboratory measurements. For the production of HO₂, the mercury-photosensitized reaction of the H₂ and O₂ precursors was used to provide an optimum condition for measurement of the pressure broadening coefficient. The Superconducting Submillimeter-wave Limb Emission Sounder (SMILES) was designed to monitor the volume mixing ratio of trace gases including HO₂ in the Earth's upper atmosphere using these transitions. The precise measurement of pressure broadening coefficient γ in terms of the half width at half maximum is required in order to retrieve the atmospheric volume mixing ratio. In this work, γ coefficients of the 625.66 GHz transition were determined for N₂ and O₂ at room temperature as γ(N₂)=4.085±0.049 MHz/Torr and γ(O₂)=2.578±0.047 MHz/Torr with 3σ uncertainty. Similarly, the coefficients of the 649.70 GHz transition were determined as γ(N₂)=3.489±0.094 MHz/Torr and γ(O₂)=2.615±0.099 MHz/Torr. The air broadening coefficients for the 625.66 GHz and 649.70 GHz lines were estimated at γ(air)=3.769±0.067 MHz and 3.298±0.099 MHz respectively, where the uncertainty includes possible systematic errors. The newly determined coefficients are compared with previous results and we discuss the advantage of the mercury-photosensitized reaction for HO₂ generation. In comparison with those of other singlet molecules, the pressure broadening coefficients of the HO₂ radical are not much affected by the existence of an unpaired electron.     

Growth of SnO2 nanoparticles via thermal evaporation method

Tin oxide (SnO₂) nanoparticles were fabricated by evaporation of Sn powers at 1000 °C in air pressure. The as-deposited SnO₂ particles were single crystal structure, which were mostly spherical shape, the diameter of particles was ranging from 200 to 600 nm. The photoluminescence (PL) spectrum showed that a sharp emission peak at around 393 nm with the excitation wavelength at 325 nm, which suggested possible applications in nanoscaled optoelectronic devices. It was also found that the holding time affects the morphology of the products. The formation mechanism of SnO₂ particles was discussed.     

In-situ formation of SiC nanocrystals by high temperature annealing of SiO2/Si under CO: A photoemission study

We have studied CO interaction with SiO₂/Si system at high temperature (~ 1100 °C) and 350 mbar by core-level photoemission. Even for short annealing time (5 min) the signal from Si2p and C1s core levels shows a clear change upon CO treatment. Shifted components are attributed to formation of SiC. This is confirmed by TEM imaging which further shows that the silicon carbide is in the form of nano-crystals of the 3C polytype. Photoemission spectroscopy moreover reveals the formation of silicon oxicarbide which could not be evidenced by other methods. Combining these results with previous Nuclear Resonance Profiling study gives a deeper insight into the mechanisms involved in the nanocrystals growth and especially for the reaction equation leading to SiC formation. We show that CO diffuses as a molecule through the silica layer and reacts with the silicon substrate according the following reaction: 4 CO + 4 Si → SiO₂ + 2SiC + SiO₂C₂.     

A DNS study on temporally evolving jet flames of pulverized coal/biomass co-firing with different blending ratios

Biomass co-firing within the existing pulverized coal boiler is thought as a practical near-term way of biomass utilization, while its detailed combustion characteristics and pollutant formation have not yet been fully understood. In the present study, we report a Carrier-phase Direct Numerical Simulation study coupled with detailed mechanism to provide a deep insight into the coal/biomass co-firing (CBCF) jet flames under different blending ratios. It is found that compared with the pure coal flame, the CBCF could (i) prompt the volatiles ignition, produce higher H₂O and similar CO₂ mass fractions at blending ratios of 20% and 40%, and obviously reduce the gas temperature and CO₂ mass fraction at the blending ratio of 50%; (ii) prompt the coal devolatilization and char burnout at blending ratios of 20% and 40%, while the char burnout is reduced when blending ratio is 50% due to the local enrichment of large particles and lack of oxygen; (iii) reduce the thermal, prompt, NNH and N₂O-intermediate routes of NO formation, but show limited effect on the NO-reburning route of NO destruction, therefore, resulting in an obvious NO reduction.     

On the rate constants of OH + HO2 and HO2 + HO2: A comprehensive study of H2O2 thermal decomposition using multi-species laser absorption

Hydrogen peroxide (H₂O₂) and hydroperoxy (HO₂) reactions present in the H₂O₂ thermal decomposition system are important in combustion kinetics. H₂O₂ thermal decomposition has been studied behind reflected shock waves using H₂O and OH diagnostics in previous studies (Hong et al. (2009) [9] and Hong et al. (2010) [6,8]) to determine the rate constants of two major reactions: H₂O₂ + M → 2OH + M (k₁) and OH + H₂O₂ → H₂O + HO₂ (k₂). With the addition of a third diagnostic for HO₂ at 227 nm, the H₂O₂ thermal decomposition system can be comprehensively characterized for the first time. Specifically, the rate constants of two remaining major reactions in the system, OH + HO₂ → H₂O + O₂ (k₃) and HO₂ + HO₂ → H₂O₂ + O₂ (k₄) can be determined with high-fidelity.No strong temperature dependency was found between 1072 and 1283 K for the rate constant of OH + HO₂ → H₂O + O₂, which can be expressed by the combination of two Arrhenius forms: k₃ = 7.0 × 10¹² exp(550/T) + 4.5 × 10¹⁴ exp(?5500/T) [cm³ mol^?1 s^?1]. The rate constants of reaction HO₂ + HO₂ → H₂O₂ + O₂ determined agree very well with those reported by Kappel et al. (2002) [5]; the recommendation therefore remains unchanged: k₄ = 1.0 × 10¹⁴ exp(?5556/T) + 1.9 × 10¹¹⁺exp(709/T) [cm³ mol^?1 s^?1]. All the tests were performed near 1.7 atm.     

High-resolution transmission measurements of CO2 at high temperatures for industrial applications

High-resolution transmission spectra of CO₂ in the 2.7, 4.3 and 15 μm regions at temperatures up to 1773 K and at approximately atmospheric pressure (1.00±0.01 atm) are measured and compared with line-by-line calculations based on the HITEMP-1995, HITEMP-2010, CDSD-HITEMP and CDSD-4000 databases. The spectra have been recorded in a high-temperature flow gas cell and using a Fourier transform infrared (FTIR) spectrometer at a nominal resolution of 0.125 cm^?1. The volume fractions of CO₂ in the measurements were 1, 10 and 100%. The measurements have been validated by comparison with medium-resolution data obtained by Bharadwaj and Modest [6]. The deviations between the experimental spectra and the calculations at 1773 K and the vibrational energy exchange and thermal dissociation of CO₂ at high temperatures are discussed.     

Ground-based solar absorption studies for the Carbon Cycle science by Fourier Transform Spectroscopy (CC-FTS) mission

Carbon cycle science by Fourier transform spectroscopy (CC-FTS) is an advanced study for a future satellite mission. The goal of the mission is to obtain a better understanding of the carbon cycle in the Earth's atmosphere by monitoring total and partial columns of CO₂, CH₄, N₂O, and CO in the near infrared. CO₂, CH₄, and N₂O are important greenhouse gases, and CO is produced by incomplete combustion. The molecular O₂ column is also needed to obtain the effective optical path of the reflected sunlight and is used to normalize the column densities of the other gases. As part of this advanced study, ground-based Fourier transform spectra are used to evaluate the spectral region and resolution needed. Spectra in the 3950–7140 cm^?1 region with a spectral resolution of 0.0042 cm^?1 recorded at Kiruna (67.84°N, 20.41°E, and 419 m above sea level), Sweden, on 1 April 1998, were degraded to the resolutions of 0.01, 0.1, and 0.3 cm^?1. The effect of spectral resolution on the retrievals has been investigated with these four Kiruna spectra. To obtain further information on the spectral resolution, optical components and spectroscopic parameters required by the future mission, high-resolution solar absorption spectra between 2000 and 15000 cm^?1 were recorded using Fourier transform spectrometers at Kitt Peak (31.9°N, 111.6°W, and 2.1 km above sea level), Arizona, on 25 July 2005 and Waterloo (43.5°N, 80.6°W, and 0.3 km above sea level), Ontario, on 22 November 2006 with spectral resolutions of 0.01 and 0.1 cm^?1, respectively. Dry air volume mixing ratios (VMRs) of CO₂ and CH₄ were retrieved from these ground-based observations. The HITRAN 2004 spectroscopic parameters are used with the SFIT2 package for the spectral analysis. The measurement precisions for CO₂ and CH₄ total columns are better than 1.07% and 1.13%, respectively, for our observations. Based on these results, a Fourier transform spectrometer (maximum spectral resolution of 0.1 cm^?1 or 5 cm maximum optical path difference (MOPD)) operating between 2000 and 15000 cm^?1 is suggested as the primary instrument for the mission. Further progress in improving the atmospheric retrievals for CO₂, CH₄, and O₂ requires new laboratory measurements of the spectroscopic line parameters.     

Modeling midwave infrared muzzle flash spectra from unsuppressed and flash-suppressed large caliber munitions

Time-resolved infrared spectra of firings from a 152 mm howitzer were acquired over an 1800–6000 cm^?1 spectral range using a Fourier-transform spectrometer. The instrument collected primarily at 32 cm^?1 spectral and 100 Hz temporal resolutions. Munitions included unsuppressed and chemically flash suppressed propellants. Secondary combustion occurred with unsuppressed propellants resulting in flash emissions lasting ～100 ms and dominated by H₂O and CO₂ spectral structure. Non-combusting plume emissions were one-tenth as intense and approached background levels within 20–40 ms. A low-dimensional phenomenological model was used to reduce the data to temperatures, soot absorbances, and column densities of H₂O, CO₂, CH₄, and CO. The combusting plumes exhibit peak temperatures of ～1400 K, areas of greater than 32 m², low soot emissivity of ～0.04, with nearly all the CO converted to CO₂. The non-combusting plumes exhibit lower temperatures of ～1000 K, areas of ～5 m², soot emissivity of greater than 0.38 and CO as the primary product. Maximum fit residual relative to peak intensity are 14% and 8.9% for combusting and non-combusting plumes, respectively. The model was generalized to account for turbulence-induced variations in the muzzle plumes. Distributions of temperature and concentration in 1–2 spatial regions demonstrate a reduction in maximum residuals by 40%. A two-region model of combusting plumes provides a plausible interpretation as a ～1550 K, optically thick plume core and ～2550 K, thin, surface-layer flame-front. Temperature rate of change was used to characterize timescales and energy release for plume emissions. Heat of combustion was estimated to be ～5 MJ/kg.