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1.
This paper reported a numerical study on the NOx 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 NOx emission of H2/CO synthetic mixture flames were examined. The analyses of detailed flame structures, chemical kinetics, and nitrogen reaction pathways indicate NOx 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.  相似文献   

2.
The present study has numerically investigated the Moderate or Intense Low oxygen Dilution (MILD) combustion regime, combustion processes and NO formation characteristics of the highly CO-rich syngas counterflow nonpremixed flames. To realistically predict the flame properties of the highly CO-rich syngas, the chemistry is represented by the modified GRI 3.0 mechanism. Computations are performed to precisely analyze the flame structure, NO formation rate, and EINO of each NO sub-mechanism. Numerical results reveal that the hydrogen enrichment and oxygen augmentation substantially influence the NO emission characteristics and the dominant NO production route in the CO-rich syngas nonpremixed flames under MILD and high temperature combustion regimes. It is found that the most dominant NO production routes are the NNH path for the lowest oxygen level (3%) and the thermal mechanism for the highest O2 condition (21%). For the intermediate oxygen level (9%), the most dominant NO production routes are the NNH route for the hydrogen fraction up to 5%, the CO2 path for the hydrogen fraction range from 5% to 10% and the thermal mechanism for the hydrogen fraction higher than 10%, respectively. To evaluate the contribution of the specific reaction on EINO the sensitivity coefficients are precisely analyzed for NO formation processes with the dominance of NNH/CO2/Thermal mechanism under the highly CO-rich syngas flames.  相似文献   

3.
This paper used the opposed-flow flame model and GRI 3.0 mechanism to investigate NO emission characteristics of H2-rich and H2-lean syngas under diffusion and premixed conditions, respectively, and analyzed influences of adding H2O, CO2 and N2 on NO formation from the standpoint of thermodynamics and reaction kinetics. For diffusion flames, thermal route is the dominant pathway to produce NO, and adding N2, H2O and CO2 shows a decreasing manner in lowering NO emission. The phenomenon above is more obvious for H2-rich syngas because it has higher flame temperature. For premixed flames, adding CO2 causes higher NO concentration than adding H2O, because adding CO2 produces more O radical, which promotes formation of NO through NNH + O = NH + NO, NH + O = NO + H and reversed N + NO = N2 + O. And in burnout gas, thermal route is the dominant way for NO formation. Under this paper's conditions, adding N2 increases the formation source of NO as well as decreases the flame temperature, and it reduces the NO formation as a whole. In addition, for H2-lean syngas and H2-rich syngas with CO2 as the diluent, N + CO2 = NO + CO plays as an important role in thermal route of NO formation.  相似文献   

4.
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.  相似文献   

5.
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.  相似文献   

6.
Extensive computations were made to determine the flammability limits of opposed-jet H2/CO syngas diffusion flames from high stretched blowoff to low stretched quenching. Results from the U-shape extinction boundaries indicate the minimum hydrogen concentrations for H2/CO syngas to be combustible are larger towards both ends of high strain and low strain rates. The most flammable strain rate is near one s−1 where syngas diffusion flames exist with minimum 0.002% hydrogen content. The critical oxygen percentage (or limiting oxygen index) below which no diffusion flames could exist for any strain rate was found to be 4.7% for the equal-molar syngas fuels (H2/CO = 1), and the critical oxygen percentage is lower for syngas mixture with higher hydrogen content. The flammability maps were also constructed with strain rates and pressures or dilution gases percentages as the coordinates. By adding dilution gases such as CO2, H2O, and N2 to make the syngas non-flammable, besides the inert effect from the diluents, the chemical effect of H2O contributes to higher flame temperature, while the radiation effect of H2O and CO2 plays an important role in the flame extinction at low strain rates.  相似文献   

7.
The NO mechanism under the moderate or intense low-oxygen dilution (MILD) combustion of syngas has not been systematically examined. This paper investigates the NO mechanism in the syngas MILD regime under the dilution of N2, CO2, and H2O through counterflow combustion simulation. The syngas reaction mechanism and the counterflow combustion simulation are comprehensively validated under different CO/H2 ratios and strain rates. The effects of oxygen volume fraction, CO/H2 ratio, pressure, strain rate, and dilution atmosphere are systematically investigated. For all the MILD cases, the contribution of the prompt and NO-reburning routes to the overall NO emission is less than 0.1% due to the lack of CH4 in fuel. At atmospheric pressure, the thermal route only accounts for less than 20% of the total NO emission because of the low reaction temperature. Moreover, at atmospheric pressure, the contribution of the NNH route to NO emission is always larger than 55% in the N2 atmosphere. The N2O-intermediate route is enhanced in CO2 and H2O atmospheres due to the increased third-body effects of CO2 and H2O through the reaction N2 + O (+M) ? N2O (+M). Especially in the H2O atmosphere, the N2O-intermediate route contributes to 60% NO at most. NO production is reduced with increasing CO/H2 ratio or pressure, mainly due to decreased NO formation from the NNH route. Importantly, a high reaction temperature and low NO emission are simultaneously achieved at high pressure. To minimize NO emission, the reactions should be operated at high values of CO/H2 ratios (i.e., >4) and pressures (e.g., P > 10 atm), low oxygen volume fractions (e.g., XO2 < 15%), and using H2O as a diluent. This study provides a new fundamental understanding of the NO mechanism of syngas MILD combustion in N2, CO2, and H2O atmospheres.  相似文献   

8.
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.  相似文献   

9.
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.  相似文献   

10.
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.  相似文献   

11.
Co-firing NH3 with H2/CO/syngas (SYN) is a promising method to overcome the low reactivity of NH3/air flame. Hence, this study aims to systematically investigate the laminar premixed combustion characteristics of NH3/air flame with various H2/CO/SYN addition loadings (0–40%) using chemical kinetics simulation. The numerical results were obtained based on the Han mechanism which can provide accurate predictions of laminar burning velocities. Results showed that H2 has the greatest effects on increasing laminar burning velocities and net heat release rates of NH3/air flame, followed by SYN and CO. CO has the most significant effects on improving NH3/air adiabatic flame temperatures. The H2/CO/SYN additions can accelerate NH3 decomposition rates and promote the generation of H and NH2 radicals. Furthermore, there is an evident positive linear correlation between the laminar burning velocities and the peak mole fraction of H + NH2 radicals. The reaction NH2 + NH <=> N2H2 + H and NH2 + NO <=> NNH + OH have remarkable positive effects on NH3 combustion. The mole fraction of OH × NH2 radicals positively affects the net heat release rates. Finally, it was discovered that H radicals play an important role in the generation of NO. The H2/CO/SYN additions can reduce the hydrodynamic and diffusional-thermal instabilities of NH3/air flame. The NH3 reaction pathways for NH3–H2/CO/SYN-air flames can be categorized mainly into NH3–NH2–NH–N–N2, NH3–NH2–HNO–NO(?N2O)–N2 and NH3–NH2(?N2H2)–NNH–N2. CO has the greatest influence on the proportions of three NH3 reaction routes.  相似文献   

12.
A laboratory-scale laminar counterflow burner was used to investigate NO formation in high pressure premixed CH4/H2/air flames. New experimental results on NO measurements by LIF were obtained at high pressure in CH4/H2/air flames with H2 content fixed at 20% in the fuel at pressures ranging from 0.1 to 0.7 MPa and an equivalence ratio progressively decreased from 0.74 to 0.6. The effects of hydrogen addition, equivalence ratio and pressure are discussed. These results are satisfactorily compared to the simulations using two detailed mechanisms: GDFkin®3.0_NOmecha2.0 and the mechanism from Klippenstein et al., which are the most recent high-pressure NOx formation mechanisms available in the literature. A kinetic analysis based on Rate of Production/Rate of Consumption and sensitivity analyses of NO is then presented to identify the main pathways that lead to the formation and consumption of NO. In addition, the effect of hydrogen addition on NO formation pathways is described and analysed.  相似文献   

13.
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.  相似文献   

14.
The effect of CO2/N2/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.  相似文献   

15.
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.  相似文献   

16.
Biomass derived gases produced via gasification, pyrolysis, and fermentation are carbon neutral alternative fuels that can be used in gas turbines, furnaces, and piston engines. To make use of these environmentally friendly but energy density low fuels the combustion characteristics of these fuels have to be fully understood. In this study the structure and laminar burning velocity of biomass derived gas flames are investigated using detailed chemical kinetic simulations. The studied gaseous fuels are the air-blown gasification gas, co-firing of gasification gas with methane, pyrolysis gases, landfill gases, and syngas, a mixture of carbon monoxide and hydrogen. The simulated burning velocities of reference fuel mixtures using two widely used chemical kinetic mechanisms, GRI Mech 3.0 and the San Diego mechanism, are compared with the experimental data to explore the uncertainties and scattering of the simulation data. The different chemical kinetic mechanisms are shown to give a reasonable agreement with each other and with experimental data, with a discrepancy within 7% over most of the conditions. The results show that the structures of typical landfill gas flames and co-firing of methane/gasification gas flames share essential similarity with methane flames. The reaction zones of these flames consist of a thin inner layer and a relatively thick CO/H2 oxidation layer. In the inner layer hydrocarbon fuel (methane) is converted through chain reactions to intermediates such as CH3, CH2O, CO, H2, etc. The structures of gasification gas flames, pyrolysis gas flames, syngas flames share similarity with the oxidization layer of the methane/air flames. Overall, the chemical reactions of all biomass derived gas flames occur in thin zones of the order of less than 1 mm. The thickness of all BDG gas flames is inversely proportional to their respective laminar burning velocity. The laminar burning velocities of landfill gases are found to increase linearly with the mole fraction of methane in the mixtures, whereas for gasification gas, syngas and pyrolysis gas where hydrogen is present, the laminar burning velocities scale linearly with the mole fraction of hydrogen.  相似文献   

17.
This study investigated the water-gas shift reaction in a bench-scale membrane reactor (M-WGS), where three supported Pd membranes of 44 cm in length and ca. 6 μm in thickness were used, reaching a total membrane surface area of 580.6 cm2. The WGS reaction was studied with the syngas mixture: 4.0% CO, 19.2% CO2, 15.4% H2O, 1.2% CH4 and 60.1% H2, under high temperature/pressure conditions: T = 673 K, pfeed = 20–35 bar(a), pperm = 15 bar(a), mimicking CO2 capture with co-production of H2 in a natural gas fired power plant. High reaction pressure and high permeation of Pd membranes allowed for near complete CO conversion and H2 recovery. Both the membranes and the membrane reactor demonstrated a long-term stability under the investigated conditions, indicating the potential of M-WGS to substitute conventional systems.  相似文献   

18.
Turbulent nonpremixed H2/N2 and H2/CO syngas flames were simulated using 3D large eddy simulations coupled with a laminar flamelet combustion model. Four different syngas fuel mixtures varying from H2-rich to CO-rich including N2 have been modelled. The computations solved the Large Eddy Simulation governing equations on a structured non-uniform Cartesian grid using the finite volume method, where the Smagorinsky eddy viscosity model with the localised dynamic procedure is used to model the sub-grid scale turbulence. Non-premixed combustion has been incorporated using the steady laminar flamelet model. Both instantaneous and time-averaged quantities are analysed and data were also compared to experimental data for one of the four H2-rich flames. Results show significant differences in both unsteady and steady flame temperature and major combustion products depending on the ratio of H2/N2 and H2/CO in syngas fuel mixture.  相似文献   

19.
A nickel-silica core@shell catalyst was applied for a methane tri-reforming process in a fixed-bed reactor. To determine the optimal condition of the tri-reforming process for production of syngas appropriate for methanol synthesis the effect of reaction temperature (550–750 °C), CH4:H2O molar ratio (1:0–3.0) and CH4:O2 molar ratio (1:0–0.5) in the feedstock was investigated. CH4 conversion rate and H2/CO ratio in the produced syngas were influenced by the feedstock composition. Increasing the amount of steam above the proportion of CH4:H2O 1:0.5 reduced the H2:CO molar ratio in produced syngas to ∼1.5. Increasing oxygen partial pressure improved methane conversion to 90% at 750 °C. At low ∼550 °C reaction temperature the tri-reforming process was not effective with low hydrogen production (H2 yield ∼20%) and very low <5% CO2 conversion. Increasing reaction temperature increased hydrogen yield to ∼85% at 750 °C. From all the tested reaction conditions the optimal for tri-reforming over the 11%Ni@SiO2 catalyst was: feed composition with molar ratio CH4:CO2:H2O:O2:He 1:0.5:0.5:0.1:0.4 at T = 750 °C. The results were explained in the context of characterisation of the catalysts used. The obtained results showed that the tri-reforming process can be applied for production of syngas with composition suitable for methanol synthesis.  相似文献   

20.
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.  相似文献   

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