A computational study of combustion and extinction of opposed-jet syngas diffusion flames

This paper reports a numerical study on the combustion and extinction characteristics of opposed-jet syngas diffusion flames. A model of one-dimensional counterflow syngas diffusion flames was constructed with constant strain rate formulations, which used detailed chemical kinetics and thermal and transport properties with flame radiation calculated by statistic narrowband radiation model. Detailed flame structures, species production rates and net reaction rates of key chemical reaction steps were analyzed. The effects of syngas compositions, dilution gases and pressures on the flame structures and extinction limits of H₂/CO synthetic mixture flames were discussed. Results indicate the flame structures and flame extinction are impacted by the compositions of syngas mixture significantly. From H₂-enriched syngas to CO-enriched syngas fuels, the dominant chain reactions are shifting from OH + H₂→H + H₂O for H₂O production to OH + CO→H + CO₂ for CO₂ production through the key chain-branching reaction of H + O₂→O + OH. Flame temperature increases with increasing hydrogen content and pressure, but the flame thickness is decreased with pressure. Besides, the study of the dilution effects from CO₂, N₂, and H₂O, showed the maximum flame temperature is decreased the most with CO₂ as the dilution gas, while CO-enriched syngas flames with H₂O dilution has highest maximum flame temperature when extinction occurs due to the competitions of chemical effect and radiation effect. Finally, extinction limits were obtained with minimum hydrogen percentage as the index at different pressures, which provides a fundamental understanding of syngas combustion and applications.     

Chemical effects of added CO2 on the extinction characteristics of H2/CO/CO2 syngas diffusion flames

Chemical effects of added CO₂ on flame extinction characteristics are numerically studied in H₂/CO syngas diffusion flames diluted with CO₂. The two representative syngas flames of 80% H₂ + 20% CO and 20% H₂ + 80% CO are inspected according to the composition of fuel mixture diluted with CO₂ and global strain rate. Particular concerns are focused on impact of chemical effects of added CO₂ on flame extinction characteristics through the comparison of the flame characteristics between well-burning flames far from extinction limit and flames at extinction. It is seen that chemical effects of added CO₂ reduce critical CO₂ mole fraction at flame extinction and thus extinguish the flame at higher flame temperature irrespective of global strain rate. This is attributed by the suppression of the reaction rate of the principal chain branching reaction through the augmented consumption of H-atom from the reaction CO₂ + H→CO + OH. As a result the overall reaction rate decreases. These chemical effects of added CO₂ are similar in both well-burning flames far from extinction limit and flames at extinction. There is a mismatching in the behaviors between critical CO₂ mole fraction and maximum flame temperature at extinction. This anomalous phenomenon is also discussed in detail.     

Flame characteristics in H2/CO synthetic gas diffusion flames diluted with CO2: Effects of radiative heat loss and mixture composition

Numerical study is conducted to understand the impact of fuel composition and flame radiation in flame structure and their oxidation process in H₂/CO synthetic gas diffusion flame with and without CO₂ dilution. The models of Sun et al. and David et al., which have been well known to be best-fitted for H₂/CO synthetic mixture flames, are evaluated for H₂/CO synthetic mixture flames diluted with CO₂. Effects of radiative heat loss to flame characteristics are also examined in terms of syngas mixture composition. Importantly contributing reaction steps to heat release rate are compared for the synthetic gas mixture flames of high contents of H₂ and CO, individually, with and without CO₂ dilution. The modification of the oxidation pathways is also addressed.     

Important role of chemical interaction on flame extinction in downstream interaction between stretched premixed H2-air and CO-air flames

Important role of chemical interaction in flame extinction is numerically investigated in downstream interaction among lean (rich) and lean (rich) premixed as well as partially premixed H₂- and CO-air flames. The strain rate varies from 30 to 5917 s⁻¹ until interacting flames cannot be sustained anymore. Flame stability diagrams mapping lower and upper limit fuel concentrations for flame extinction as a function of strain rate are presented. Highly stretched interacting flames are survived only within two islands in the flame stability map where partially premixed mixture consists of rich H₂-air flame, extremely lean CO-air flame, and a diffusion flame. Further increase in strain rate finally converges to two points. It is found that hydrogen penetrated from H₂-air flame (even at lean flame condition) participates in CO oxidation vigorously due to the high diffusivity such that it modifies the slow main reaction route CO + O₂ → CO₂ + O into the fast cyclic reaction route involving CO + OH → CO₂ + H. These chemical interactions force even rich extinction boundaries with deficient reactant Lewis numbers larger than unity to be slanted at high strain rate. Appreciable amount of hydrogen in the side of lean H₂-air flame also oxidizes the CO penetrated from CO-air flame, and this reduces flame speed of the H₂-air flame, leading to flame extinction. At extremely high strain rates, interacting flames are survived only by a partially premixed flame such that it consists of a very rich H₂-air flame, an extremely lean CO-air flame, and a diffusion flame. In such a situation, both the weaker H₂- and CO-air flames are parasite on the stronger diffusion flame such that it can lead to flame extinction in the situation of weakening the stronger diffusion flame. Important role of chemical interaction in flame extinction is discussed in detail.     

Extinction of premixed H2/air flames: Chemical kinetics and molecular diffusion effects

Laminar flame speed has traditionally been used for the partial validation of flame kinetics. In most cases, however, its accurate determination requires extensive data processing and/or extrapolations, thus rendering the measurement of this fundamental flame property indirect. Additionally, the presence of flame front instabilities does not conform to the definition of laminar flame speed. This is the case for Le<1 flames, with the most notable example being ultralean H₂/air flames, which develop cellular structures at low strain rates so that determination of laminar flame speeds for such mixtures is not possible. Thus, this low-temperature regime of H₂ oxidation has not been validated systematically in flames. In the present investigation, an alternative/supplemental approach is proposed that includes the experimental determination of extinction strain rates for these flames, and these rates are compared with the predictions of direct numerical simulations. This approach is meaningful for two reasons: (1) Extinction strain rates can be measured directly, as opposed to laminar flame speeds, and (2) while the unstretched lean H₂/air flames are cellular, the stretched ones are not, thus making comparisons between experiment and simulations meaningful. Such comparisons revealed serious discrepancies between experiments and simulations for ultralean H₂/air flames by using four kinetic mechanisms. Additional studies were conducted for lean and near-stoichiometric H₂/air flames diluted with various amounts of N₂. Similarly to the ultralean flames, significant discrepancies between experimental and predicted extinction strain rates were also found. To identify the possible sources of such discrepancies, the effect of uncertainties on the diffusion coefficients was assessed and an improved treatment of diffusion coefficients was advanced and implemented. Under the conditions considered in this study, the sensitivity of diffusion coefficients to the extinction response was found to be significant and, for certain species, greater than that of the kinetic rate constants.     

Comparative study on the effect of CO2 and H2O dilution on laminar burning characteristics of CO/H2/air mixtures

A study on the effect of CO₂ and H₂O dilution on the laminar burning characteristics of CO/H₂/air mixtures was conducted at elevated pressures using spherically expanding flames and CHEMKIN package. Experimental conditions for the CO₂ and H₂O diluted CO/H₂/air/mixtures of hydrogen fraction in syngas from 0.2 to 0.8 are the pressures from 0.1 to 0.3 MPa, initial temperature of 373 K, with CO₂ or H₂O dilution ratios from 0 to 0.15. Laminar burning velocities of the CO₂ and H₂O diluted CO/H₂/air/mixtures were measured and calculated using the mechanism of Davis et al. and the mechanism of Li et al. Results show that the discrepancy exists between the measured values and the simulated ones using both Davis and Li mechanisms. The discrepancy shows different trends under CO₂ and H₂O dilution. Chemical kinetics analysis indicates that the elementary reaction corresponding to peak ROP of OH consumption for mixtures with CO/H₂ ratio of 20/80 changes from reaction R3 (OH + H₂ = H + H₂O) to R16 (HO₂+H = OH + OH) when CO₂ and H₂O are added. Sensitivity analysis was conducted to find out the dominant reaction when CO₂ and H₂O are added. Laminar burning velocities and kinetics analysis indicate that CO₂ has a stronger chemical effect than H₂O. The intrinsic flame instability is promoted at atmospheric pressure and is suppressed at elevated pressure for the CO₂ and H₂O diluted mixtures. This phenomenon was interpreted with the parameters of the effective Lewis number, thermal expansion ratio, flame thickness and linear theory.     

NO formation of opposed-jet syngas diffusion flames: Strain rate and dilution effects

The NO formation characteristics and reaction pathways of opposed-jet H₂/CO syngas diffusion flames were analyzed with a revised OPPDIF program which coupled a narrowband radiation model with detailed chemical kinetics in this work. The effects of strain rates ranging from 0.1 to 1000 s^?1 and diluents including CO₂, H₂O and N₂ on NO production rates were investigated for three typical syngas compositions. The numerical results demonstrated that NO is produced primary through NNH-intermediate route and thermal route at high strain rates, where the reaction of NH + O = NO + H (R51) also become more active. Near the strain rate of 10 s^?1, the flame temperature is the highest and thermal route is the dominant NO formation route, but NO would be consumed by reburn route where NO is converted to NH through HNO, especially for H₂-rich syngas. At low strain rates, radiative heat loss results in a lower flame temperature and further reduce NO formation, while the reaction of N + CO₂ = NO + CO (R140) become more important, especially for CO-rich syngas. With the diluents, NO production rates decreased with increasing dilution percentages. When the flame temperature is very high as the thermal route is dominant near strain rate of 10 s^?1, CO₂ dilution makes flame temperature and NO production rate the lowest. Toward both lower and higher strain rates, adding H₂O is more effective in reducing NO because R140 and NNH-intermediate route are suppressed the most by H₂O dilution respectively.     

Numerical investigation of diluent influence on flame extinction limits and emission characteristic of lean-premixed H2-CO (syngas) flames

In recent years, research efforts have been channeled to explore the use of environmentally-friendly clean fuel in lean-premixed combustion so that it is vital to understand fundamental knowledge of combustion and emissions characteristics for an advanced gas turbine combustor design. The current study investigates the extinction limits and emission formations of dry syngas (50% H₂-50% CO), moist syngas (40% H₂-40% CO-20% H₂O), and impure syngas containing 5% CH₄. A counterflow flame configuration was numerically investigated to understand extinction and emission characteristics at the lean-premixed combustion condition by varying dilution levels (N₂, CO₂ and H₂O) at different pressures and syngas compositions. By increasing dilution and varying syngas composition and maintaining a constant strain rate in the flame, numerical simulation showed among diluents considered: CO₂ diluted flame has the same extinction limit in moist syngas as in dry syngas but a higher extinction temperature; H₂O presence in the fuel mixture decreases the extinction limit of N₂ diluted flame but still increases the flame extinction temperature; impure syngas with CH₄ extends the flame extinction limit but has no effect on flame temperature in CO₂ diluted flame; for diluted moist syngas, extinction limit is increased at higher pressure with the larger extinction temperature; for different compositions of syngas, higher CO concentration leads to higher NO emission. This study enables to provide insight into reaction mechanisms involved in flame extinction and emission through the addition of diluents at ambient and high pressure.     

Effects of Lewis number and preferential diffusion on flame characteristics in 80%H2/20%CO syngas counterflow diffusion flames diluted with He and Ar

Numerical study is conducted to grasp flame characteristics in H₂/CO syngas counterflow diffusion flames diluted with He and Ar. An effective fuel Lewis number, applicable to premixed burning regime and even to moderately stretched diffusion flames, is suggested through the comparison among fuel Lewis number, effective Lewis number, and effective fuel Lewis number. Flame characteristics with and without the suppression of the diffusivities of H, H₂, and He are compared in order to clarify the important role of preferential diffusion effects through them. It is found that the scarcity of H and He in reaction zone increases flame temperature whereas that of H₂ deteriorates flame temperature. Impact of preferential diffusion of H, H₂, and He in flame characteristics is also addressed to reaction pathways for the purpose of displaying chemical effects.     

Computed NOx emission characteristics of opposed-jet syngas diffusion flames

This paper reported a numerical study on the NO_x emission characteristics of opposed-jet syngas diffusion flames. A narrowband radiation model was coupled to the OPPDIF program, which used detailed chemical kinetics and thermal and transport properties to enable the study of 1-D counterflow syngas diffusion flames with flame radiation. The effects of syngas composition, pressure and dilution gases on the NO_x emission of H₂/CO synthetic mixture flames were examined. The analyses of detailed flame structures, chemical kinetics, and nitrogen reaction pathways indicate NO_x are formed through Zeldovich (or thermal), NNH and N₂O routes both in the hydrogen-lean and hydrogen-rich syngas flames at normal pressure. Zeldovich route is the main NO formation route. Therefore, the hydrogen-rich syngas flames produce more NO due to higher flame temperatures compared to that for hydrogen-lean syngas flames. Although NNH and N₂O routes also are the primary NO formation paths, a large amount of N₂ will be reformed from NNH and N₂O species. For hydrogen-rich syngas flames, the NO formation from NNH and N₂O routes are lesser, where NO can be dissipated through the reactions of NH + NO → N₂ + OH and NH + NO → N₂O + H more actively. At a rather low pressure (0.01 atm), NNH-intermediate route is the only formation path of NO. Increasing pressure then enhances NO formation reactions, especially through Zeldovich mechanisms. However, at higher pressures (5–10 atm), NO is then converted back to N₂ through reversed N₂O route for hydrogen-lean syngas flames, and through NNH as well for hydrogen-rich syngas flames. In addition, the dilution effects from CO₂, H₂O, and N₂ on NO emissions for H₂/CO syngas flames were studied. The hydrogen-lean syngas flames with H₂O dilution have the lowest NO production rate among them, due to a reduced reaction rate of NNH + O → NH + NO. But for hydrogen-rich syngas flames with CO₂ dilution, the flame temperatures decrease significantly, which leads to a reduction of NO formation from Zeldovich route.     

Effect of radiation emission and reabsorption on flame temperature and NO formation in H2/CO/air counterflow diffusion flames

The radiation effect on flame temperature and NO emission of H₂-lean (0.2H₂ + 0.8CO) and H₂-rich (0.8H₂ + 0.2CO) syngas/air counterflow diffusion flames was numerically investigated using OPPDIF code incorporated with the optical thin model, statistical narrow band model and adiabatic condition. Firstly, the coupled effect of strain rate and radiation was studied. Disparate tendencies of NO emission with an increasing strain rate between H₂-lean and H₂-rich syngas flames were found at very small strain rate, and the effect of radiation reabsorption on NO formation can be neglected when the strain rate was greater than 100 s^?1 for both H₂-lean and H₂-rich syngas flames. Because the radiation effect is vital to flames with small strain rate, its impact on flame temperature and NO emission was investigated in detail at a strain rate of 10 s^?1. The results indicated that NO formation is more sensitive to radiation reabsorption than flame temperature, especially for the H₂-rich syngas flame. The underlying mechanism was discovered by using reaction pathway analysis. Furthermore, the radiation effect under CO₂ dilution of the syngas fuel was examined. It was demonstrated that the radiation effect on flame temperature became more prominent with the increase of CO₂ concentration for both H₂-lean and H₂-rich syngas. The radiation effect on NO emission increased first and then decreased with an increasing CO₂ content for H₂-lean syngas, whereas for H₂-rich syngas the radiation effect is monotonic.     

Lower flammability limit of H2/CO/air mixtures with N2 and CO2 dilution at elevated temperatures

The lower flammability limits of H₂/CO/air mixtures with N₂ and CO₂ dilution were systematic experimentally studied over a wide range of H₂ blending ratios (0–100 vol%) with N₂ (0–67 vol%) and CO₂ (0–67 vol%) dilution in the fuels under various elevated initial temperatures (298 K–473 K) and atmospheric pressure. The experimentation was conducted via an 8 L stainless steel cylindrical explosion vessel and using the metal wire fusing as the ignition source. The corresponding cases were also calculated using Kondo's correlation proposed based on a limiting flame temperature concept. To gain an insightful understanding of the effect of chemical kinetics at different H₂ fractions and CO₂ dilution ratios, sensitivity analysis and H mole fractions were carried out using Chemkin-Pro. The experimental results showed that the lower flammability limits decreased with the increase of H₂ fractions especially when the H₂ content was low (x_H2 ≤ 0.25). Attributable to the accelerated oxidation of CO by the greater generation of OH from H₂/O₂ reaction, Le Chatelier's Rule tended to relatively over-estimate the lower flammability limits of H₂/CO mixtures with a small amount of H₂. Because of the larger heat capacity, and the inhibition effect on the oxidation of CO and the generation of H radicals, CO₂ presented a stronger dilution effect on lower flammability limit than N₂. Moreover, the lower flammability limits for all measured syngas mixtures displayed great linear temperature dependence. A comparison between the experimental data and calculation results showed that, Kondo's correlation provided the satisfactorily accuracy predictions on the lower flammability limits of diluted syngas mixtures with lower H₂ fractions (x_H2 ≤ 0.5). However, when the H₂ fractions were high and the mixture was highly CO₂ diluted, Kondo's correlation over-estimated the lower flammability limits and the prediction error would reach to 30%. The considerably distinctions were not only attributed to the inadaptable assumption against to the growing and lower behaviour of H₂ flame temperature at lower flammability limit, but also caused by the preferential diffusion of H₂, as well as the variation of the chemical effects under high H₂ content and high CO₂ dilution conditions.     

Effect of CO2/N2/CH4 dilution on NO formation in laminar coflow syngas diffusion flames

The effect of CO₂/N_2/CH₄ dilution on NO formation in laminar coflow H₂/CO syngas diffusion flames was experimentally and numerically investigated. The results reveal that the NO emission index increases with H₂/CO mole ratio. In all cases, CO₂/N₂/CH₄ dilution can reduce the peak temperature of syngas flame and have the ability to reduce peak flame temperature is decreased in the following order: CO₂>N₂>CH₄. CO₂/N₂ dilution reduces the NO formation in syngas flame while CH₄ dilution promotes the NO formation. Besides, the dilution of CO₂/N₂/CH₄ can reduce the peak mole fraction of OH and its variations with H₂/CO mole ratio and dilution ratio show the same trend as the peak flame temperature variations. The height of the flame with CO₂ and N₂ dilution increases with dilution ratio. The flame with CH₄ dilution becomes higher and wider with the increase of dilution ratio.     

Investigation of dilution effects on partially premixed swirling syngas flames using a LES-LEM approach

The dilution effects of CO₂ and H₂O on partially premixed swirling syngas flames are investigated with the large eddy simulation (LES) method. The linear-eddy model (LEM) is employed to directly resolve the unclosed molecular diffusion, scalar mixing and chemical reaction processes occurring at subgrid scale level using their specific length and time scales instead of modelling, which makes the LES-LEM approach quite attractive for hydrogen fuel combustion as the obviously different diffusion and reaction characteristics of H₂ and H compared to other species in the syngas mixture. Firstly, adding CO₂ into the fuel stream can significantly decrease the flame temperature during the partially premixed combustion. The concentration of H and OH radicals decreases upon CO₂ dilution and thus the chemical reaction processes are modified. Compared with CO₂, H₂O is less effective in changing the temperature field because of the chemical effects of H₂O. The simultaneous addition of H₂O and CO₂ as dilution gases with volume ratio 1:1 into the fuel stream is also conducted to identify the effects of H₂O and CO₂ on partially premixed combustion dynamics by comparing with single H₂O and CO₂ cases. The obtained results are expected to provide helpful information for the design and operation of gas turbine combustion systems with syngas fuels.     

Effect of flame stretch in downstream Interaction between premixed syngas-air flames

The effect of strain rate in downstream interactions between lean (rich) and lean (rich) premixed syngas flames with the fuel composition of 50% H₂ and 50% CO is numerically investigated by varying the strain rate in the range of 5∼500 s⁻¹. The flame stability maps for several strain rates are presented and main concerns are focused on the downstream interactions on the lean and rich extinction boundaries. The fuel composition of 50% H₂ and 50% CO with effective Lewis numbers larger than unity for both lean and rich extinction boundaries is chosen for grasping the important role of hydrogen with the deficient reactant Lewis numbers much smaller than unity. The results show that the lean extinction boundaries have the slanted shape, thereby leading to strong interactions; meanwhile the rich extinction boundaries at appropriately low strain rates are of square, indicating weak interactions. However, at highly strained interacting rich flames, the rich extinction boundaries show a slanted shape, thereby leading to strong interactions even for Lewis numbers much larger than unity. In such situations, thermal and chemical interactions are explained in detail. It is found that, in interacting flames, the excessive heat loss of the stronger flame partly to the weaker flame and mostly to the ambience is the mechanism of flame extinction.     

Computed extinction limits and flame structures of H2/O2 counterflow diffusion flames with CO2 dilution

A narrowband radiation model is coupled to the OPPDIF program, which uses detailed chemical kinetics and thermal and transport properties to enable the study of one-dimensional counterflow H₂/O₂ diffusion flames with CO₂ as dilution gas over the entire range of flammable strain rates. The effects of carbon dioxide dilution, ambient pressure and inlet temperature of opposed jets on the extinction limits and flame structures are compared and discussed. The extinction limits are presented using maximum flame temperature and strain rate as coordinates. Both high-stretch blowoff and the low-stretch quenching limits are computed. When the CO₂ dilution percentage is higher, the flame is thinner and flame temperature is lower. The combustible range of strain rates is decreased with increasing CO₂ percentage due to the effects of CO₂ dilution, which is categorized as dilute effect, chemical effect and radiation effect. In addition, the flame temperature of low-stretch diffusion flame with radiation loss is substantially lower than that computed with the non-radiation model. This large temperature drop results from the combined effect of flame radiation and chemical kinetics. The extinction limits and flame temperature are increasing with increasing atmospheric pressure and temperature, but the flame thickness is decreased with the pressure. At higher pressure and temperature, the extinction limits are extended more on the high-stretch blowoff limits, indicating the influence of the ambient pressure and temperature on the chemical reaction.     

Extinction studies of near-limit lean premixed syngas/air flames

Extinction studies of weakly-stretched near-limit lean premixed syngas/air flames were conducted in a twin-flame counterflow configuration. Experiments showed that buoyancy-induced natural convection at normal gravity strongly disturbed these flames. In order to validate the simulation, accurate extinction data was obtained at micro-gravity. Experimental data obtained from the 3.6 s micro-gravity drop tower showed that the extinction equivalence ratio increased with the increasing global stretch rate and decreased with the increasing H₂ mole fraction in the fuel. Numerical simulation was conducted with CHEMKIN software using GRI 3.0 and USC-Mech II mechanisms. The predicted extinction limit trend was in agreement with the micro-gravity experimental data. Sensitivity analyses showed that the competition between the main branching reaction H + O₂ ⇔ O + OH and the main termination reaction H + O₂ + M ⇔ HO₂ + M in the H₂/O₂ chemistry determined the extinction limits of the flames. The dominant species for syngas/air flame extinction was the H radical. The key exothermal reaction changed from OH + CO ⇔ H + CO₂ to OH + H₂ ⇔ H + H₂O with the increasing H₂ mole fraction in the fuel. Also, the mass diffusion played a more important role than chemical kinetics in the flame extinction. When the H₂ mass diffusion was suppressed, the reaction zone was pushed to the stagnation plane and the flame became weaker; while H mass diffusion is suppressed, the reaction zone slightly shifted towards the upstream and the flame was slightly strengthened.     

Preferential diffusion effects on flame characteristics in H2/CO syngas diffusion flames diluted with CO2

Numerical study is conducted to clarify preferential diffusion effects of H₂ and H on flame characteristics in synthetic diffusion flames of the compositions of 80% H₂/20% CO and 20% H₂/80% CO as representatively H₂-enriched and CO-enriched H₂/CO flames. Impacts of CO₂ addition to the flames are also examined through the variation of added CO₂ mole fraction from 0 to 0.5. A comparison was made by employing a mixture-averaged diffusivity and the suppression of the diffusivities of H and H₂. It is found that preferential diffusion effects on maximum flame temperature cannot be explained by the well-known behavior between maximum flame temperature and scalar dissipation rate but by chemical processes. The concrete evidence is also presented through the examination of the behavior of maximum H mole fraction and the behavior of importantly-contributing reaction steps to overall heat release rate.     

A mechanistic evaluation of Soret diffusion in heptane/air flames

The influence of Soret diffusion on the structure and response of n-heptane/air flames is investigated numerically with detailed reaction mechanism and transport. Unstretched freely-propagating planar premixed flames as well as stretched counterflow premixed and diffusion flames are studied, with emphasis on the separate and combined Soret effects of heptane and its oppositely-directed decomposition species H₂ and H, as well as those of the major species O₂, N₂, CO₂ and H₂O. Results show that, in the unstretched case for which the flame temperature remains at its adiabatic value, Soret diffusion primarily affects the chemical kinetics embedded in the flame structure and the net effect is small; while in the stretched cases, its impact is mainly through those of heptane and the secondary fuel H₂ in modifying the flame temperature, with substantial effects, while H₂ and H also affect the chemical kinetics especially when the active reaction zone is localized. The dilution/enrichment of the reactant concentrations in the flame through the Soret diffusion of the major species O₂, N₂, CO₂ and H₂O further exert finite effects on the flame burning intensity.     

A detailed numerical study of NOx kinetics in low calorific value H2/CO syngas flames

The present study provides an extensive and detailed numerical analysis of NO_x chemical kinetics in low calorific value H₂/CO syngas flames utilizing predictions by five chemical kinetic mechanisms available out of which four deal with H₂/CO while the fifth mechanism (GRI 3.0) additionally accounts for hydrocarbon chemistry. Comparison of predicted axial NO profiles in premixed flat flames with measurements at 1 bar, 3.05 bar and 9.15 bar shows considerably large quantitative differences among the various mechanisms. However, at each pressure, the quantitative reaction path diagrams show similar NO formation pathways for most of the mechanisms. Interestingly, in counterflow diffusion flames, the quantitative reaction path diagrams and sensitivity analyses using the various mechanisms reveal major differences in the NO formation pathways and reaction rates of important reactions. The NNH and N₂O intermediate pathways are found to be the major contributors for NO formation in all the reaction mechanisms except GRI 3.0 in syngas diffusion flames. The GRI 3.0 mechanism is observed to predict prompt NO pathway as the major contributing pathway to NO formation. This is attributed to prediction of a large concentration of CH radical by the GRI 3.0 as opposed to a relatively negligible value predicted by all other mechanisms. Also, the back-conversion of NNH into N₂O at lower pressures (2–4 bar) was uniquely observed for one of the five mechanisms. The net reaction rates and peak flame temperatures are used to correlate and explain the differences observed in the peak [NO] at different pressures. This study identifies key reactions needing assessment and also highlights the need for experimental data in syngas diffusion flames in order to assess and optimize H₂/CO and nitrogen chemistry.