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1.
Compared to hydrocarbons, ammonia's low reactivity and higher NOx emissions limit its practical application. Consequently, its implementation in combustion systems requires a different combustor geometry, by adapting existing systems or developing new ones. This study investigates the flame stability, NO emissions, and flame structure of NH3/CH4/air premixed flames in a novel combustor comprising a double swirl burner. A lean premixed CH4/air mixture of equivalence ratio, Φout, was supplied to the outer swirl, while a NH3/CH4/Air mixture fed the inner swirl. The molar fraction of NH3 in the inner fuel blend, xNH3, was varied from 0 (pure CH4) to 1 (pure NH3) over far-lean to far-rich inner stream equivalence ratio, Φin. This new burner's stability map was established in terms of Φin versus xNH3 for different Φout. Then, NO emissions were measured versus Φin for various xNH3 and Φout. Finally, based on the NO emissions, eight flames were down-selected for in-flame measurements, which included temperature and OH-PLIF. The stability measurements revealed that increasing xNH3 modifies the stability map by increasing the lean blowout limits and narrowing the flashback region. At Φout ≥ 0.6, a stable flame was achieved for a pure inner NH3/air mixture. Low NO emissions were achieved in this burner configuration at xNH3=1 by either enriching or far-leaning Φin. Enriching Φin led to a steep decrease in NO concentrations. However, to achieve low NO concentrations, precise control of Φout was needed. At Φin=1.4, 220 ppm NO at Φout=0.7 versus 690 at Φout=0.6 was measured. Moreover, substantially enriching Φin>1.2 led to a slight decrease in measured NO. Generally, the OH-PLIF images revealed a conical OH-layer at the burner exit. Certain flame conditions created OH-pockets inside the conical structure or formed a V-shaped OH-layer far downstream. This change in flame structure was found to impact NO emissions strongly.  相似文献   

2.
The influence of wall heat loss on the emission characteristics of ammonia-air swirling flames has been investigated employing Planar Laser-Induced Fluorescence imaging of OH radicals and Fourier Transform Infrared spectrometry of the exhaust gases in combustors with insulated and uninsulated walls over a range of equivalence ratios, ?, and pressures up to 0.5 MPa. Strong influence of wall heat loss on the flames led to quenching of the flame front near the combustor wall at 0.1 MPa, resulting in large unburned NH3 emissions, and inhibited the stabilization of flames in the outer recirculating zone (ORZ). A decrease in heat loss effects with an increase in pressure promoted extension of the fuel-rich stabilization limit owing to increased recirculation of H2 from NH3 decomposition in the ORZ. The influence of wall heat loss resulted in emission trends that contradict already reported trends in literature. NO emissions were found to be substantially low while unburned NH3 and N2O emissions were high at fuel-lean conditions during single-stage combustion, with values such as 55 ppmv of NO, 580 ppmv of N2O and 4457 ppmv of NH3 at ? = 0.8. In addition, the response of the flame to wall heat loss as pressure increased was more important than the effects of pressure on fuel-NO emission, thereby leading to an increase in NO emission with pressure. It was found that a reduction in wall heat loss or a sufficiently long fluid residence time in the primary combustion zone is necessary for efficient control of NH3 and N2O emissions in two-stage rich-lean ammonia combustors, the latter being more effective for N2O in addition to NO control. This study demonstrates that the influence of wall heat loss should not be ignored in emissions measurements in NH3-air combustion, and also advances the understanding of previous studies on ammonia micro gas turbines.  相似文献   

3.
Recent studies have demonstrated that ammonia could be one of the most promising hydrogen carrier candidates which can be used in large-scale power plants. However, it is challenging to burn ammonia in gas turbines due to its narrow flame stabilization limits. This study investigates the blow-off characteristics and flame macrostructure transition behavior of ammonia/air flame (i.e. NH3 flame) and ammonia/methane/air flame (i.e. 50%NH3 flame) in a swirl combustor. Methane/air flame (i.e. CH4 flame) is also demonstrated for comparative purposes. The flow field and instantaneous OH profile are measured with PIV and OH-PLIF technique, respectively. Large eddy simulation (LES) is conducted to extend understandings of the experimental findings. The results show that the NH3 flame possesses a poor lean flame stability limit which can be largely extended by adding CH4 in the fuel. Moreover, changing swirl number (S) shows no apparent effect on the lean blow-off limit (?b) for the NH3 flame. On the contrary, a clear extension on ?b is found for the 50%NH3 flame when increasing S. Four flame macrostructure modes can be identified when decreasing equivalence ratio (?). The transition from flame II to flame III (?t describes the transition equivalence ratio) can be considered as the early warning of blow-off for a swirl stabilized flame. It is found that for the NH3 flame, there is no clear flame macrostructure transition at small inlet velocities (U < 3.8 m/s), i.e., ?b?t, while the difference between ?b and ?t will be observed as the inlet velocity increases. However, for the 50%NH3 and CH4 flames, a clear flame macrostructure transition from flame II to flame III is observed even for a lower inlet velocity. The LES results show that the NH3 flame has a faster blow-off process compared to the CH4 flame, which is mainly attributed to the excessive stretch causing local extinction during the blow-off process.  相似文献   

4.
We investigate the effects of varying the degree of burner stabilization on Fenimore NO formation in fuel-rich low-pressure flat CH4/O2/N2 flames. Towards this end, axial profiles of flame temperature and OH, NO and CH mole fractions are measured using laser-induced fluorescence (LIF). The experiments are performed at equivalence ratios between 1.3 and 1.5. The flame temperature is seen to decrease by 200-300 K, with a concomitant decrease in OH mole fraction, upon reducing the total flow rate from 5 to 3 L/min, thus increasing stabilization. At equivalence ratios between 1.3 and 1.5, this decrease in flow rate lowers the maximum CH mole fraction by a factor of 2, and the NO mole fraction by ∼40% in all flames studied. Integrating the reaction rate for CH + N2 to estimate Fenimore NO formation, using the rate coefficient in GRI-Mech 3.0, and the measured temperatures and CH profiles show very good agreement with the measured NO mole fraction for ? = 1.3 and 1.4, supporting the current choice for this rate. This agreement also shows that the increase in residence time caused by increased stabilization is an important factor in the ultimate impact of the changes in CH mole fraction on NO formation. The results at ? = 1.5 suggest that substantial quantities of fixed nitrogen species, e.g., HCN, are only slowly oxidized in the post-flame zone under these conditions, leading to a significant discrepancy between the measured NO mole fraction and that obtained by integrating over the CH profile. Detailed calculations using GRI-Mech 3.0 predict the experimental results at ? = 1.3 nearly quantitatively, but show increasing differences with the measurements for both CH and NO profiles with increasing equivalence ratio.  相似文献   

5.
6.
One of the main concerns regarding ammonia combustion is its tendency to yield high nitric oxide (NO) emissions. Burning ammonia under slightly rich conditions reduces the NO mole fraction to a low level, but the penalties are poor combustion efficiency and unburnt ammonia. As an alternative solution, this paper reports the experimental investigation of premixed swirl flames fueled with ammonia-hydrogen mixtures under very-lean to stoichiometric conditions. A gas analyzer was used to measure the NO mole fraction in the flame and post flame regions, and it was found that low NO emissions (as low as 100 ppm) in the exhaust were achieved under very lean conditions (? ≈ 0.40). Low NO emission was also possible at higher equivalence ratios, e.g. ? = 0.65, for very large ammonia fuel fractions (XNH3 > 0.90). 1-D flame simulations were performed to elaborate on experimental findings and clarify the observations of the chemical kinetics. In addition, images of OH* chemiluminescence intensity were captured to identify the flame structure. It was found that, for some conditions, the OH* chemiluminescence intensity can be used as a proxy for the NO mole fraction. A monotonic relationship was discovered between OH* chemiluminescence intensities and NO mole fraction for a wide range of ammonia-hydrogen blends (0.40 < ? < 0.90 and 0.25 < XNH3 < 0.90), making it possible to use the low-cost OH* chemiluminescence technique to qualify NO emission of flames fueled with hydrogen-enriched ammonia blends.  相似文献   

7.
Laser-Induced Fluorescence (LIF) excitation spectra in the NOA–X (0-0) band were used for temperature measurements in the postflame region of high-pressure CH4/air flames. To improve the quality of the measured spectra and to perform reliable line-shape measurements, the initial mixture was doped with approximately 400 ppm NO. At pressures up to 18 bar, excellent agreement was obtained between NO LIF temperatures and NARS/rotational Raman temperatures. Effective broadening coefficients were also determined in these flames. Problems with quantitative concentration measurements of NO and single-pulse temperature measurements at high pressures are discussed.  相似文献   

8.
Starting from force constant values calculated by an ab initio MO method (4-31G(N1)), and by adjusting the diagonal elements, a practical force constant matrix (F) has been reached which could explain the observed infrared and Raman spectra (in the frequency range lower than 2000 cm?1) of the gauche form of the ethylamine CH3CH2NH2 molecule and five isotopic species CH313CH2NH2, CH3CH215NH2, CH3CD2NH2, CH3CH2ND2, and CD3CD2NH2. The F matrix for the trans form of ethylamine was constructed by transferring ab initio 4-31G(N1) values and by revising diagonal elements with conversion factors whose values are equal to the corresponding values of gauche form. A nearly complete set of assignments was achieved of the vibrational bands of ethylamines, observed so far in the spectral range 2000–100 cm?1. In matrix isolation spectroscopy, two bands assignable to the NH2 wagging vibrations of gauche and trans forms have been found at 775 and 782 cm?1, respectively, for CH3CH2NH2. They are at 768 and 774 cm?1, respectively, for CD3CD2NH2. From the intensity changes of these bands observed on changing the nozzle temperature in the matrix formation, the energy difference ΔE (gauche-trans) of these two conformers has been estimated to be 100 ± 10 cm?1.  相似文献   

9.
Ammonia (NH3) direct combustion is attracting attention for energy utilization without CO2 emissions, but fundamental knowledge related to ammonia combustion is still insufficient. This study was designed to examine effects of radiation heat loss on laminar ammonia/air premixed flames because of their very low flame speeds. After numerical simulations for 1-D planar flames with and without radiation heat loss modeled by the optically thin model were conducted, effects of radiation heat loss on flame speeds, flame structure and emissions were investigated. Simulations were also conducted for methane/air mixtures as a reference. Effects of radiation heat loss on flame speeds were strong only near the flammability limits for methane, but were strong over widely diverse equivalence ratios for ammonia. The lower radiative flame temperature suppressed the thermal decomposition of unburned ammonia to hydrogen (H2) at rich conditions. The equivalence ratio for a low emission window of ammonia and nitric oxide (NO) in the radiative condition shifted to a lower value than that in the adiabatic condition.  相似文献   

10.
Chemical energy vectors will play a crucial role in the transition of the global energy system, due to their essential advantages in storing energy in form of gaseous, liquid, or solid fuels. Ammonia (NH3) has been identified as a highly promising candidate, as it is carbon-free, can be stored at moderate pressures, and already has a developed distribution infrastructure. As a fuel NH3 has poor combustion properties that can be improved by the addition of hydrogen, which can be obtained energy-efficiently by partially cracking ammonia into hydrogen (H2) and nitrogen (N2) prior to the combustion process. The resulting NH3/H2/N2 blend leads to significantly improved flame stability and resilience to strain-induced blow-out, despite similar laminar flame properties compared to equivalent methane/air flames. This study reports the first measurements of extinction strain rates, measured using the premixed twin-flame configuration in a laminar opposed jet burner, for two NH3/H2/N2 blends over a range of equivalence ratios. Local strain rates are measured using particle tracking velocimetry (PTV) and are related to the inflow conditions, such that the local strain rate at the extinction point can be approximated. The results are compared with 1D-simulations using three recent kinetic mechanisms for ammonia oxidation. By relating the extinction strain rates to laminar flame properties of the unstretched flame, a comparison of the extinction behaviour of CH4 and NH3/H2/N2 blends can be made. For lean mixtures, NH3/H2/N2-air flames show a significant higher extinction resistance in comparison to CH4/air. In addition, a strong non-linear dependence between the resistance to extinction and equivalence ratio for NH3/H2/N2 blends is observed.  相似文献   

11.
Lean premixed combustion has potential advantages of reducing pollutants and improving fuel economy. In some lean engine concepts, the fuel is directly injected into the combustion chamber resulting in a distribution of lean fuel/air mixtures. In this case, very lean mixtures can burn when supported by hot products from more strongly burning flames. This study examines the downstream interaction of opposed jets of a lean-limit CH4/air mixture vs. a lean H2/air flame. The CH4 mixtures are near or below the lean flammability limit. The flame composition is measured by laser-induced Raman scattering and is compared to numerical simulations with detailed chemistry and molecular transport including the Soret effect. Several sub-limit lean CH4/air flames supported by the products from the lean H2/air flame are studied, and a small amount of CO2 product (around 1% mole fraction) is formed in a “negative flame speed” flame where the weak CH4/air mixture diffuses across the stagnation plane into the hot products from the H2/air flame. Raman scattering measurements of temperature and species concentration are compared to detailed simulations using GRI-3.0, C1, and C2 chemical kinetic mechanisms, with good agreement obtained in the lean-limit or sub-limit flames. Stronger self-propagating CH4/air mixtures result in a much higher concentration of product (around 6% CO2 mole fraction), and the simulation results are sensitive to the specific chemical mechanism. These model-data comparisons for stronger CH4/air flames improve when using either the C2 or the Williams mechanisms.  相似文献   

12.
The heat capacity of the layer compounds tetrachlorobis (n-propylammonium) manganese II and tetrachlorobis (n-propylammonium) cadmium II, (CH3CH2CH2NH3)2MnCl4 and (CH3CH2CH2NH3)2CdCl4 respectively, has been measured over the temperature range 10 K ?T ? 300 K.Two known structural phase transitions were observed for the Mn compound in this temperature region: at T = 112.8 ± 0.1 K (ΔHt= 586 ± 2 J mol?1; ΔSt = 5.47 ± 0.02 J K?1mol?1) and at T =164.3 ± (ΔHt = 496 ± 7 J mol?1; ΔSt =3.29 ± 0.05 J K?1mol?1). The lower transition is known to be from a monoclinic structure to a tetragonal structure, while the upper is from the tetragonal phase to an orthorhombic one. From comparison with the results for the corresponding methyl Mn compound it is deduced that the lower transition primarily involves changes in H-bonding while the upper transition involves motion in the propyl chain.A new structural phase transition was observed in the Cd compound at T= 105.5 ± 0.1 K (ΔHt= 1472.3 ± 0.1 J mol?1; ΔSt = 13.956 ± 0.001 J K?1mol?1), in addition to two transitions that have been observed previously by other techniques. The higher of these transitions(T = 178.7 ± 0.3 K; ΔHt = 982 ± 4 J mol?1 ΔSt = 6.16 ± 0.02 J K? mol?1) is known to be between two orthorhombic structures, while the structural changes at the lower transition (T= 156.8 ± 0.2 K; ΔHt = 598 ± 5 J mol?1, ΔSt = 3.85 ± 0.03 J K?1 mol?1) and at the new transition are not known. It is proposed that these two transitions correspond respectively to the tetragonal to orthorhombic and monoclinic to tetragonal transitions in the propyl Mn compounds.In addition to the structural phase transitions (CH3CH2CH2NH3)2MnCl4 magnetically orders at t? 130 K. The magnetic contribution to the heat capacity is deduced from the heat capacity of the corresponding diamagnetic Cd compound and is of the form expected for a quasi 2-dimensional Heisenberg antiferromagnet.  相似文献   

13.
14.
Ammonia is a promising alternative clean fuel due to its carbon-free character and high hydrogen density. However, the low reactivity of ammonia and the potential high NOx emissions hinder its applications. Blending methane into ammonia can effectively improve the reactivity of pure NH3. In addition, lean combustion, as a high-efficiency and low-pollution combustion technology, is an effective measure to control the potential increase in NOx emissions. In the present work, the ignition delay times (IDTs) of NH3/CH4 mixtures highly diluted in Ar (98%) with CH4 mole fractions of 0%, 10%, and 50% were measured in a shock tube at an equivalence ratio of 0.5, pressures of 1.75 and 10 bar and a temperature range of 1421 K - 2149 K. A newly comprehensive kinetic model (named as HUST-NH3 model) for the NH3/CH4 mixtures oxidation was developed based on our previous work. Four kinetic models, the HUST-NH3 model, Glarborg model [19], Okafor model [7], and CEU model [10], were evaluated against the ignition delay times, laminar flame speeds, and species profiles of pure ammonia and ammonia/methane mixtures from the present work and literature. The simulation results indicated that the HUST-NH3 model shows the best performance among the above four models. Kinetic analysis results indicated that the absence of NH3 + M = NH2 + H + M (R819) and N2H2 + M = H + NNH + M (R902) in the CEU model and Okafor model cause the deviations between the experimental and simulation results. The overestimation of the rate constants of NH2 + NO = NNH + OH (R838) in the Glarborg model is the main reason for the overprediction of the NH3 laminar flame speeds.  相似文献   

15.
The heat capacity of the layer compound, tetrachlorobis (methylammonium) manganese II, (CH3NH3)2MnCl4, has been measured over the range 10K <T<300K. In this region, two structural phase transitions have been observed previously by other techniques: one transition is from a monoclinic low temperature (MLT) phase to a tetragonal low temperature (TLT) phase, and the other is from TLT to an orthorhombic room temperature (ORT) phase. The present experiments have shown that the lower transition (MLT→TLT) occurs at T = 94.37±0.05K with ΔHt = 727±5 J mol?1 and ΔSt = 7.76±0.05 J K?1 mol?1, and the upper transition (TLT→ORT) takes place at T = 257.02±0.07K with ΔHt = 116±1J mol?1 and ΔSt = 0.451±0.004 J K?1mol?1. These results are discussed in the light of recent measurements on (CH3NH3)2CdCl4, and also with regard to a recent theoretical model of the structural phase transitions in compounds of this type.In addition to the structural phase transitions, (CH3NH3)2MnCl4 also undergoes magnetic ordering at T < 150K. The magnetic component to the heat capacity, as deduced from a corresponding states comparison of the heat capacity of the present compound with that of the Cd compound, is shown to be consistent with the behaviour expected for a quasi 2-dimensional Heisenberg antiferromagnet.  相似文献   

16.
Due to issues surrounding carbon dioxide emissions from carbon-containing fuels, there is growing interest in ammonia (NH3) as an alternative combustion fuel. One attractive method of burning NH3 is to co-fire it with hydrocarbons, such as natural gas, and in this case soot formation is possible. To begin understanding the influence of NH3 on soot formation when co-fired with hydrocarbons, soot volume fractions and mole fractions of gas-phase species were computationally and experimentally interrogated for CH4 flames with up to 40% NH3 by volumetric fuel fraction. Mole fractions of gas-phase species, including C2H2 and C6H6, were measured with on-line electron impact mass spectrometry, and soot volume fractions were obtained via color-ratio pyrometry. The simulations employed a detailed chemical mechanism developed for capturing nitrogen interactions with hydrocarbons during combustion. The results are compared to findings in N2CH4 flames, in order to separate thermal and dilution effects from the chemical influence of NH3 on soot formation. Experimentally, C2H2 concentrations were found to decrease slightly for the NH3CH4 flames relative to N2CH4 flames, and a stronger suppression of C6H6 was found for NH3 relative to N2 additions. The measured results show a strong suppression of soot with the addition of NH3, with soot concentrations reduced by over a factor of 10 with addition of up to 20% or more NH3 by mole fraction. The model satisfactorily captured relative differences in maximum centerline C2H2, C6H6, and soot concentrations with addition of N2, but was unable to match measured differences in NH3CH4 flames. These results highlight the need for an improved understanding of fuel-nitrogen interactions with higher hydrocarbons to enable accurate models for predicting particulate emissions from NH3/hydrocarbon combustion.  相似文献   

17.
Transported probability density function (TPDF) simulation with sensitivity analysis has been conducted for turbulent non-premixed CH4/H2 flames of the jet-into-hot-coflow (JHC) burner, which is a typical model to emulate moderate or intense low oxygen dilution combustion (MILD). Specifically, two cases with different levels of oxygen in the coflow stream, namely HM1 and HM3, are simulated to reveal the differences between MILD and hot-temperature combustion. The TPDF simulation well predicts the temperature and species distributions including those of OH, CO and NO for both cases with a 25-species mechanism. The reduced reaction activity in HM1 as reflected in the peak OH concentration is well correlated to the reduced oxygen in the coflow stream. The particle-level local sensitivities with respect to mixing and chemical reaction further show dramatic differences in the flame characteristics. HM1 is less sensitive to mixing and reaction parameters than HM3 due to the suppressed combustion process. Specifically, for HM1 the sensitivities to mixing and chemical reactions have comparable magnitude, indicating that the combustion progress is controlled by both mixing and reaction in MILD combustion. For HM3, there is however a change in the combustion mode: during the flame initialization, the combustion progress is more sensitive to chemical reactions, indicating that finite-rate chemistry is the controlling process during the autoignition process for flame stabilization; at further downstream where the flame has established, the combustion progress is controlled by mixing, which is characteristic of nonpremixed flames. An examination of the particles with the largest sensitivities reveals the difference in the controlling mixtures for flame stabilization, namely, the stoichiometric mixtures are important for HM1, whereas, fuel-lean mixtures are controlling for HM3. The study demonstrates the potential of TPDF simulations with sensitivity analysis to investigate the effects of finite-rate chemistry on the flame characteristics and emissions, and reveal the controlling physio-chemical processes in MILD combustion.  相似文献   

18.
NH is a key short-lived radical involved in the prompt-NO formation. Quantification of NH is thus particularly important for testing the NO kinetic mechanisms. However, quantitative measurements of native NH in hydrocarbon/oxygen/nitrogen flames remain very scarce. Therefore, in this work, the mole fractions of native NH were obtained using a combination of laser-based diagnostics; Laser Induced Fluorescence (LIF) and Cavity Ring-Down Spectroscopy (CRDS). The NH species was probed after exciting the transition R1(6) in the A3Π-X3Σ? (0-0) system at 333.9?nm. The mole fraction profiles of NH were successfully obtained in premixed low-pressure flames of CH4/O2/N2 and C2H2/O2/N2 at two equivalence ratios of 1.00 and 1.25. The estimated detection limit for the NH radical was around 4.5?×?108 molecule cm?3 (i.e. 2 ppb in mole fraction at 1600?K), which is nearly 2 orders of magnitude lower than previous values reported in the literature. These new experimental results were compared with predictions by a recently developed NO model (namely NOMecha2.0). In the case of the CH4 flames, a satisfying agreement between the experiment and model was observed. However, in the case of the C2H2 flames, some discrepancies were observed. Model analysis has highlighted the importance of the HCCO radicals in the NH formation through the HCNO→HNCO→NH2 reactions pathway. Modification of the rate constant values of the reactions C2H2+?O and HCCO?+?O2, which are key reactions for both the acetylene laminar flame speed and the HCCO predictions, has enabled the model to satisfactorily predict the experimental NH and NO profiles also in the C2H2 flames.  相似文献   

19.
20.
The paper examines eight diverse regimes in which fuels can mix and react with air. These comprise: (i) Lifted subsonic; and (ii) supersonic jet flames, with (iii) and without (iv) cross flows; (v) Rim-attached flames; (vi) Early Downwash flames; (vii) Downwash-attached jet flames; and (viii) Fire Whirls.Correlations of characteristics within these regimes are principally in terms of a dimensionless Flow Number, U*, Cross Flow Reynolds number, Rec, and, for Fire Whirls, a dimensionless Critical Velocity, CV. Boundaries of seven of the eight regimes are identified, through plots of U*, against Rec, and of the eighth through a plot of CV against U*. The circumstances of transitions between regimes are identified. The study involves a variety of CH4 cross flow flame measurements, in a wind tunnel. Cross flows can initially create a small lee-side flame downwash, due to the depression in pressure. With increasing fuel flow this might extend 1.3 m downwards from the horizontal tip of the vertical burner. Jet flames can attach to the downwash, which can become significant above Rec ≈ 2000. More extensive downwash might further delay blow-off. Regime boundaries are constructed on the U*/Rec diagram covering lifted flames, early downwash, and downwash-attached flames. The most powerful flames tend to be lifted, choked, flames, with cross flow, and fire whirls. Combustion becomes less efficient at high Rec and low U*, although CH4 was efficiently reacted.Experimental values of the ratio of fuel to air velocity, u/uc, of CH4 flames ranged between about 10 and 30 for lifted flames, and between 0.3 and 3.6, at blow-off, for rim-attached flames. The latter comprise an important category, often intermediate between lifted flames and downwash-attached flames.  相似文献   

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