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1.
Co-firing methane (CH4) and ammonia (NH3) has attracted growing concerns as a feasible greenhouse gas reduction strategy in gas turbine-based power generation, which raises the need to better understand the interaction of methane and nitric oxide (NO) under flame conditions. In this work, laminar flame propagation of CH4/NO mixtures at initial pressure (Pu) of 1 atm, initial temperature (Tu) of 298 K and equivalence ratios of 0.4–1.8 was experimentally investigated using a constant-volume combustion vessel. Laminar burning velocities (LBVs) and Markstein lengths were experimentally determined. A kinetic model of CH4/NO combustion was developed with rate constants of several important reactions updated, presenting reasonable predictions on the measured LBVs of CH4/NO mixtures. The modeling analyses reveal that the reduction of NO can proceed through two mechanisms, i.e. the hydrocarbon NO reduction mechanism and non-hydrocarbon NO reduction mechanism. Among the two mechanisms, the non-hydrocarbon NO reduction mechanism which includes reactions NO+H = N+OH, NO+O = N + O2 and NO+N = N2+O has a higher contribution to NO reduction at the equivalence ratio of 0.6, while the hydrocarbon NO reduction mechanism with hydrocyanic acid (HCN) as the key intermediate plays a more important role at the equivalence ratio of 1.8. NO+H = N+OH and CH3+NOHCN+H2O are found to be the two most sensitive reactions to promote the flame propagation, while the LBVs measured in this work are demonstrated to provide strong constraint for these reactions. Furthermore, previous CH4/O2/NO oxidation data measured in flow reactor and rapid compression machine were also simulated, which provides extended validation of the present model over wider conditions.  相似文献   

2.
A premixed nitromethane/oxygen/argon flame at low pressure (4.67 kPa) has been investigated using tunable vacuum ultraviolet (VUV) photoionization and molecular-beam mass spectrometry. About 30 flame species including hydrocarbons, oxygenated and nitrogenous intermediates have been identified by measurements of photoionization efficiency spectra. Mole fraction profiles of the flame species have been determined by scanning burner position at some selected photon energies. The results indicate that N2 and NO are the major nitrogenous products in the nitromethane flame. Compared with previous studies on nitromethane combustion, a number of unreported intermediates, including C3H4, C4H6, C4H8, C2H2O, C2H4O, CH3CN, H2CNHO, C3H3N and C3H7N, are observed in this work. Based on our experimental results and previous modeling studies, a detailed oxidation mechanism including 69 species and 314 reactions has been developed to simulate the flame structure. Despite some small discrepancies, the predictions by the modeling study are in reasonable agreement with the experimental results.  相似文献   

3.
Counterflow diffusion flame experiments and modeling results are presented for a fuel mixture consisting of N2, C2H2, and C2H4 flowing against decomposition products from a solid AP pellet. The flame zone simulates the diffusion flame structure that is expected to exist between reaction products from AP crystals and a hydrocarbon binder. Quantitative species and temperature profiles have been measured for one strain rate, given by a separation of 5 mm, between the fuel exit and the AP surface. Species measured include C2H2, C2H4, N2, CN, NH, OH, CH, C2, NO, NO2, O2, CO2, H2, CO, HCl, H2O, and soot volume fraction. Temperature was measured using a combination of a thermocouple at the fuel exit and other selected locations, spontaneous Raman scattering measurements throughout the flame, NO vibrational populations, and OH rotational population distributions. The burning rate of the AP was also measured for this flame’s strain rate. The measured eighteen scalars are compared with predictions from a detailed gas-phase kinetics model consisting of 105 species and 660 reactions. Model predictions are found to be in good agreement with experiment and illustrate the type of kinetic features that may be expected to occur in propellants when AP particles burn with the decomposition products of a polymeric binder.  相似文献   

4.
The combustion characteristics for the turbulent diffusion flames using the unsteady flamelet concept have been numerically investigated. The Favre-averaged Navier–Stokes equations are solved by a finite volume method of SIMPLE type that incorporates the laminar flamelet concept with a modified k ? ε turbulence model. The NO formation is estimated by solving the Eulerian particle transport equations in a postprocessing mode. Two test problems are considered: CH4/H2/N2 jet flame and CH4/H2 stabilised bluff body flame. The temperature and species profiles are well captured by the flamelet model. Two different chemical mechanisms (GRI 2.11 and 3.0) give nearly identical results for temperature and species except NO. The GRI 3.0 gives significantly higher NO levels compared to the GRI 2.11. This is mainly attributed to the difference in NO formation by the prompt mechanism. The NO formation is sensitive to the number of flamelet particles. The NO levels for two test flames do not change when the flamelet particle number exceeds six.  相似文献   

5.
6.
The chemical and thermal structures of flame of composite pseudo-propellants based on cyclic nitramines (HMX, RDX) and azide polymers (GAP and BAMO–AMMO copolymer) were investigated at a pressure of 1.0 MPa by molecular beam mass spectrometry and a microthermocouple technique. Eleven species H2, H2O, HCN, CO, CO2, N2, N2O, CH2O, NO, NO2, and nitramine vapor (RDXv or HMXv), were identified, and their concentration profiles were measured in HMX/GAP and RDX/GAP pseudo-propellant flames at a pressure of 1 MPa. Two main zones of chemical reactions in the flame of nitramine/GAP pseudo-propellants were found. In the first, narrow, zone 0.1 mm wide (adjacent to the burning surface), complete consumption of nitramine vapor and NO2 with the formation of NO, HCN, CO, H2, and N2 occurs. In the second, wider high-temperature zone, oxidation of HCN and CH2O by NO and N2O with the subsequent formation of CO, H2, and N2 takes place. The leading reactions in the high-temperature zone of flame of nitramine/GAP pseudo-propellants are the same as in the case of pure nitramines. In the case of nitramine/BAMO–AMMO pseudo-propellants a presence of carbonaceous particles on the burning surface did not allow us to analyze the zone adjacent to the burning surface, therefore only one flame zone was found. Temperature profiles in the combustion wave of nitramine/azide polymer pseudo-propellants were measured at 1 MPa. The data obtained can be used to develop and validate a self-sustain combustion model for pseudo-propellants based on nitramines and azide polymers.  相似文献   

7.
Absolute CN and CH radical concentrations were determined in situ during the combustion of a graphite substrate in premixed, laminar, low-pressure, H2/O2 flames for two different equivalence ratios, = 1.0 and = 1.5. For CN measurements, a small amount of NO (1.8%) was added. The concentration of CN was measured by cavity ring-down spectroscopy (CRDS) probing the absorption of the P1,2 (13) in the B–X (0, 0) band at 388.1 nm, and the concentration of CH was measured by linear unsaturated laser-induced fluorescence (LIF) exciting the fluorescence of the R1 (4) in the B–X (0, 0) band at 387.4 nm. Temperature measurements were done based on LIF excitation spectra of OH in the A–X (0, 0) band. It was found that the graphite substrate reduces the flame temperature in the vicinity of its surface. The CN concentrations were found to be three times higher for the rich flame than for the stoichiometric flame. CH concentrations were slightly higher for the stoichiometric flame than for the rich flame. The observed CH/CN concentration ratio is substantially lower compared to NO-doped low-pressure CH4/O2 flames. The obtained quantitative information can serve as a first calibration point for detailed numerical simulations of the burning solid graphite, which are based on the concept of surface elementary reactions.  相似文献   

8.
With the growing attention on ammonia (NH3) combustion, understanding NH3 and nitric oxide (NO) interaction at temperatures higher than DeNOx temperature region or even flame temperature becomes a new research need. In this work, the outwardly propagation spherical flame method was used to investigate the laminar flame propagation of NH3/NO/N2 mixtures and constrain the uncertainties of the specific kinetics. The present experiments were conducted at initial pressure of 1 atm, temperature of 298 K and equivalence ratios from 1.1 to 1.9. A kinetic model of NH3/NO combustion was updated from our previous work. Compared with several previous models, the present model can reasonably reproduce the laminar burning velocity data measured in this work and speciation data in literature. Based on model analyses, the interaction of NH3 and NO was thoroughly investigated. As both the oxidizer and a carrier of nitrogen element, NO frequently reacts with different decomposition products of NH3 including NH2, NH and NNH, and converts nitrogen element to the final product N2. It is found that the laminar burning velocity experiment of NH3/NO/N2 mixtures using the outwardly propagating spherical flame method can provide highly sensitive validation targets for the kinetics in NH3 and NO interaction.  相似文献   

9.
The effect of CO addition on extinction and NO x formation in lean premixed counterflow CH4/air flames was investigated by numerical simulation. Detailed chemistry and complex thermal and transport properties were employed. A method that gradually switched off the initial reactions of NO formation from different routes was used to analyse the variation of NO formation mechanism. The results indicate that the addition of certain amount of CO increases the strain extinction limits and reduces the radiation extinction limits. As a result, the lean flammability limit of CH4/air premixed flame is extended to leaner side by the addition of CO. The formation of NO in a flame is increased with the addition of CO at a constant equivalence ratio. For an ultra-lean flame, the increase in the formation of NO is mainly because of the increase in the contribution from the NNH intermediate route, while for a near stoichiometric flame, this increase is mainly attributable to the rise in the contribution from the thermal route. With the fraction of added CO being gradually increased, the formation of NO2 in a flame first decreases and then increases at a given equivalence ratio. The addition of CO reduces the formation N2O in an ultra-lean flame, while affects little on the formation of N2O in a near stoichiometric flame.  相似文献   

10.
The numerical modelling of alkali metal reacting dynamics in turbulent pulverised-coal combustion is discussed using tabulated sodium chemistry in large eddy simulation (LES). A lookup table is constructed from a detailed sodium chemistry mechanism including five sodium species, i.e. Na, NaO, NaO2, NaOH and Na2O2H2, and 24 elementary reactions. This sodium chemistry table contains four coordinates, i.e. the equivalence ratio, the mass fraction of the sodium element, the gas-phase temperature, and a progress variable. The table is first validated against the detailed sodium chemistry mechanism by zero-dimensional simulations. Then, LES of a turbulent pulverised-coal jet flame is performed and major coal-flame parameters compared against experiments. The chemical percolation devolatilisation (CPD) model and the partially stirred reactor (PaSR) model are employed to predict coal pyrolysis and gas-phase combustion, respectively. The response of the five sodium species in the pulverised-coal jet flame is subsequently examined. Finally, a systematic global sensitivity analysis of the sodium lookup table is performed and the accuracy of the proposed tabulated sodium chemistry approach has been calibrated.  相似文献   

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