The effect of CO addition on extinction and NOx 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
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
The effect of hydrogen addition to ultra lean counterflow CH4/air premixed flames on the extinction limits and the characteristics of NOx emission was investigated by numerical simulation. Detailed chemistry and complex thermal and transport properties were employed. The results show that the addition of hydrogen can significantly enlarge the flammable region and extend the flammability limit to lower equivalence ratios. If the equivalence ratio is kept constant, the addition of hydrogen increases the emission of NO in a flame due to the enhancement in the rate of the NNH or N2O intermediate NO formation routes. The addition of hydrogen causes a monotonic decrease in the formation of NO2 and N2O, except flames near the extinction limits, where the emission of NO2 and N2O first increases, and then decreases with the increase in the fraction of hydrogen. Overall, hydrogen enrichment technology allows stable combustion under ultra lean conditions, resulting in significant CO2 and NO emission reduction. 相似文献
Ethylene is a key intermediate in the combustion mechanisms of most practical fuels. It plays also an important role in the formation of aromatic hydrocarbons and soot particules. The latter has motivated many experimental and numerical studies carried out on rich ethylene-air mixtures. Less studies have been devoted to lean mixtures, and the development of strategies based on lean, premixed flames to reduce soot and NOx production requires additional experimental data in lean conditions. In this work, the chemical structure of lean premixed ethylene-oxygen-nitrogen flames stabilized on a flat-flame burner at atmospheric pressure was determined experimentally. The species mole fraction profiles were also computed by the Premix code (Chemkin II version) and four detailed reaction mechanisms. A very good agreement was observed for the main flame properties: reactants consumption, final products (CO2, H2O) and the main intermediates: CO and H2. Marked differences occurred in the prediction of active intermediate species present in small concentrations. Pathways analyses were performed to identify the origins of these discrepancies. It was shown that the same reactions were involved in the four mechanisms to describe the consumption of ethylene, but with marked differences in their relative importance. C2H3 and CH2HCO are the main radicals formed in this first step and their consumption increases the differences between the mechanisms either by the use of different kinetic data for common reactions or by differences in the nature of the consumption reactions. 相似文献
The kinetic effects of NO addition on the flame dynamics and burning limits of n-dodecane cool and warm diffusion flames are investigated experimentally and computationally using a counterflow system. The results show that NO plays different roles in cool and warm flames due to their different reaction pathway sensitivities to the flame temperature and interactions with NO. We observe that NO addition decreases the cool flame extinction limit, delays the extinction transition from warm flame to cool flame, and promotes the ignition transition from warm flame to hot flame. In addition, jet-stirred reactor (JSR) experiments of n-dodecane oxidation with and without NO addition are also performed to develop and validate a n-dodecane/NOx kinetic model. Reaction pathway and sensitivity analyses reveal that, for cool flames, NO addition inhibits the low-temperature oxidation of n-dodecane and reduces the flame temperature due to the consumption of RO2 via NO+RO2?NO2+RO, which competes with the isomerization reaction that continues the peroxy radical branching sequence. The model prediction captures well the experimental trend of the inhibiting effect of NO on the cool flame extinction limit. For warm flames, two different kinds of warm flame transitions, the warm flame extinction transition to cool flame and the warm flame reignition transition to hot flame, were observed. The results suggest that warm extinction transition to cool flame is suppressed by NO addition while the warm flame reignition transition to hot flame is promoted. The kinetic model developed captures well the experimentally observed warm flame transitions to cool flame but fails to predict the warm flame reignition to hot flame at similar experimental conditions. 相似文献
There is a need for prediction models of soot particles and polycyclic aromatic hydrocarbons (PAHs) formation in parametric conditions prevailing in automotive engines: large fuel molecules and high pressure. A detailed kinetic mechanism able to predict the formation of benzene and PAHs up to four rings from C2 fuels, recently complemented by consumption reactions of decane, was extended in this work to heptane and iso-octane oxidation. Species concentrations measured in rich, premixed flat flames and in a jet stirred reactor (JSR) were used to check the ability of the mechanism to accurately predict the formation of C2 and C3 intermediates and benzene at pressures ranging from 0.1 to 2.0 MPa. Pathways analyses show that propargyl recombination is the only significant route to benzene in rich heptane and iso-octane flames. When included as the first step of a soot particle formation model, the gas-phase kinetic mechanism predicts very accurately the final soot volume fraction measured in a rich decane flame at 0.1 MPa and in rich ethylene flames at 1.0 and 2.0 MPa. 相似文献
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
This study examined the effects of OH concentration and temperature on the NO emission characteristics of turbulent, non-premixed methane (CH4)/ammonia (NH3)/air swirl flames in two-stage combustors at high pressure. Emission data were obtained using large-eddy simulations with a finite-rate chemistry method from model flames based on the energy fraction of NH3 (ENH3) in CH4/NH3 mixtures. Although NO emissions at the combustor exit were found to be significantly higher than those generated by CH4/air and NH3/air flames under both lean and stoichiometric primary zone conditions, these emissions could be lowered to approximately 300 ppm by employing far-rich equivalence ratios (?) of 1.3 to 1.4 in the primary zone. This effect was possibly due to the lower OH concentrations under far-rich conditions. An analysis of local flame characteristics using a newly developed mixture fraction equation for CH4/NH3/air flames indicated that the local temperature and NO and OH concentration distributions with local ? were qualitatively similar to those in NH3/air flames. That is, the maximum local NO and OH concentrations appeared at local ? of 0.9, although the maximum temperature was observed at local ? of 1.0. Both the temperature and OH concentration were found to gradually decrease with the partial replacement of CH4 with NH3. Consequently, NO emissions from CH4/NH3 flames were maximized at ENH3 in the range of 20% to 30%, after which the emissions decreased. Above 2100 K, the NO emissions from CH4/NH3 flames increased exponentially with temperature, which was not observed in NH3/air flames because of the lower flame temperatures in the latter. But, the maximum NO concentration in CH4/NH3 flames was occurred at a temperature slightly below the maximum temperature, just as in NH3/air flames. The apparent exponential increase in NO emissions from CH4/NH3 flames is attributed to a similar trend in the OH concentration at high temperatures. 相似文献
The interaction of a premixed methane-air flame with a two-dimensional counter-rotating vortex pair is studied under stoichiometric and rich conditions using a detailed C1C2 chemical mechanism. The flame structure and transient response are examined, both at curved cusps and on the vortex-pair centreline. Differences between the two flames are observed in the unsteady behaviour of species mole fractions and production rates. In contrast with earlier one-dimensional opposed-jet flame data, the present results show that the rich flame exhibits a faster response to unsteady strain-rate disturbances than does the stoichiometric flame. Analysis of the results suggest this may be due to the increased dependence of the flame on H, and the decreased role of OH, under rich conditions. Results are also presented from an experimental V-flame vortex-pair interaction study. Measured peak CH and OH data are also found to exhibit a faster flame response under rich conditions. 相似文献
A study of formation and destruction of NO in adiabatic laminar premixed flames of CH4 + O2 mixtures diluted with N2 or Ar (with various dilution ratios) in a range of equivalence ratios at atmospheric pressure is presented. Nitric oxide was seeded into the flames using mixtures of diluent gas + 100 ppm of NO. The heat flux method was employed to measure adiabatic burning velocities of these flames. Nitric oxide concentrations in the post-flame zone at 10, 15 and 20 mm above the burner surface were measured using probe sampling. Burning velocities and NO concentrations simulated using a previously developed chemical kinetic mechanism were compared with the experimental results. The conversion ratio of NO seeded into the flames was determined. The kinetic mechanism accurately predicts burning velocities over the range of equivalence ratios and NO conversion in the rich flames. Significant discrepancies between measured and calculated NO conversion in the lean and near-stoichiometric flames were observed and discussed. 相似文献
We address the plausibility of singlet methylene (1CH2) in the prompt NO formation mechanism via examination of experimental species profiles and kinetic flame modeling of several low-pressure methane-oxygen-nitrogen flames. Existing kinetic models assuming CH as the only prompt NO precursor greatly underpredict NO formation under very fuel-lean conditions. We have constructed a kinetic pathway initiated by the recombination of singlet CH2 with molecular nitrogen to form diazomethane, CH2NN, early in the flame. Although the majority of the diazomethane is predicted to react with flame radicals to regenerate N2, a small percentage (approximately 10%) is predicted to react via cleavage of the NN bond leading to NO formation. This leads to accurate prediction of the experimental measurements of NO formation in lean, low-pressure flames. Assuming reasonable kinetic parameters for the reactions of CH2, the large underprediction of NO under lean conditions can be rectified by the inclusion of the 1CH2 prompt NO pathway in the kinetic mechanism. 相似文献
In this paper, we present a study on the effect of Lewis number, Le, on the stabilization and blow-off of laminar lean limit premixed flames stabilized on a cylindrical bluff body. Numerical simulations and experiments are conducted for propane, methane and two blends of hydrogen with methane as fuel gases, containing 20% and 40% of hydrogen by volume, respectively. It is found that the Le?>?1 flame blows-off via convection from the base of the flame (without formation of a neck) when the conditions for flame anchoring are not fulfilled. Le?≤?1 flames exhibit a necking phenomenon just before lean blow-off. This necking of the flame front is a result of the local reduction in mass burning rates causing flame merging and quenching of the thin flame tube formed. The structure of these flames at the necking location is found to be similar to tubular flames. It is found that extinction stretch rates for tubular flames closely match values at the neck location of bluff-body flames of corresponding mixtures, suggesting that excessive flame stretch is directly responsible for blow-off of the studied Le?≤?1 flames. After quenching of the neck, the upstream part forms a steady and stable residual flame in the wake of the bluff body while the downstream part is convected away. 相似文献
This paper describes the dynamics of non-premixed flames responding to bulk velocity fluctuations, and compares the dynamics of the flame sheet position and spatially integrated heat release to that of a premixed flame. The space–time dynamics of the non-premixed flame sheet in the fast chemistry limit is described by the stoichiometric mixture fraction surface, extracted from the solution of the -equation. This procedure has some analogies to premixed flames, where the premixed flame sheet location is extracted from the G = 0 surface of the solution of the G-equation. A key difference between the premixed and non-premixed flame dynamics, however, is the fact that the non-premixed flame sheet dynamics are a function of the disturbance field everywhere, and not just at the reaction sheet, as in the premixed flame problem. A second key difference is that the non-premixed flame does not propagate and so flame wrinkles are convected downstream at the axial flow velocity, while wrinkles in premixed flames convect downstream at a vector sum of the flame speed and axial velocity. With the exception of the flame wrinkle propagation speed, however, we show that that the solutions for the space–time dynamics of the premixed and non-premixed reaction sheets in high velocity axial flows are quite similar. In contrast, there are important differences in their spatially integrated unsteady heat release dynamics. Premixed flame heat release fluctuations are dominated by area fluctuations, while non-premixed flames are dominated by mass burning rate fluctuations. At low Strouhal numbers, the resultant sensitivity of both flames to flow disturbances is the same, but the non-premixed flame response rolls off slower with frequency. Hence, this analysis suggests that non-premixed flames are more sensitive to flow perturbations than premixed flames at O(1) Strouhal numbers. 相似文献
Most studies of triple flames in counterflowing streams of fuel and oxidizer have been focused on the symmetric problem in which the stoichiometric mixture fraction is 1/2. There then exist lean and rich premixed flames of roughly equal strengths, with a diffusion flame trailing behind from the stoichiometric point at which they meet. In the majority of realistic situations, however, the stoichiometric mixture fraction departs appreciably from unity, typically being quite small. With the objective of clarifying the influences of stoichiometry, attention is focused on one of the simplest possible models, addressed here mainly by numerical integration. When the stoichiometric mixture fraction departs appreciably from 1/2, one of the premixed wings is found to be dominant to such an extent that the diffusion flame and the other premixed flame are very weak by comparison. These curved, partially premixed flames are expected to be relevant in realistic configurations. In addition, a simple kinematic balance is shown to predict the shape of the front and the propagation velocity reasonably well in the limit of low stretch and low curvature. 相似文献
An experimental and kinetic modeling study is reported on three premixed nitroethane/oxygen/argon flames at low pressure (4.655 kPa) with the equivalence ratios (Φ) of 1.0, 1.5 and 2.0. Over 30 flame species were identified with tunable synchrotron vacuum ultraviolet photoionization mass spectrometry, with their mole fractions quantified as the function of the height above burner. The flame temperature profiles were measured with a Pt–6%Rh/Pt–30%Rh thermocouple. A detailed kinetic mechanism with 115 species and 730 reactions was proposed and validated against experimental results. The computed predictions have shown satisfactory agreement with the experimental results. Basing on the rate-of-production analysis, the reaction pathways that feature the combustion of nitroethane were revealed, including the primary decomposition of C–N bond fission, the oxidation of C2 and C1 hydrocarbons and the formation of nitrogenous species. The presence of NO2 and NO has been proved to be important for these processes. 相似文献
To investigate (fuel-)lean/rich limits and essential stoichiometries, i.e., the borders of lean/rich combustion, one-dimensional steady computations with detailed chemistry for flame balls, counterflow flames, and stretch-free planar flames were conducted using a CH4/O2/Xe mixture that has been used in microgravity experiments. As continuous converged solutions were obtained under lean/rich conditions, it was suggested that the existence of flame ball not only under lean but also under rich condition. Flame radii and temperatures of flame balls decreased and increased toward the lean/rich limits from their maximum and minimum values, respectively. The lean limits were wider in the order of the flame ball, counterflow flame, and stretch-free planar flame. Therefore, the lean flammability limit corresponded to the lean limit of the flame ball in the mixture. Conversely, the rich limits were wider in the order of the counterflow flame, stretch-free planar flame, and flame ball. Thus, the rich flammability limit corresponded to the rich limit of the counterflow flame in the mixture. Essential stoichiometry, which represents the actual stoichiometry depending on the dominant transport in near-flame front, was not uniquely determined as conventional stoichiometry (ϕ = 1); it was located between the equivalence ratio of ϕ = 1 and ϕc, where ϕc denotes the critical equivalence ratio is evaluated using the fuel and oxidizer Lewis number of a target mixture. The results indicated that the essential stoichiometry of the stretch-free planar flame corresponded to ϕ = 1, that of the flame ball corresponded to ϕ = ϕc, and that of the stretched flame was located between ϕ = 1 and ϕc depending on the stretch rate. 相似文献
Chemiluminescence has been observed since the beginning of spectroscopy, nevertheless, important facts still remain unknown. Especially, reaction pathways leading to chemiluminescent species such as OH?, CH?, $\mathrm{C}_{2}^{*}$, and $\mathrm{CO}_{2}^{*}$ are still under debate and cannot be modeled with standard codes for flame simulation. In several cases, even the source species of spectral features observed in flames are unknown. In recent years, there has been renewed interest in chemiluminescence, since it has been shown that this radiation can be used to determine flame parameters such as stoichiometry and heat release under some conditions. In this work, we present a reaction mechanism which predicts the OH?, CH? (in A- and B-state), and $\mathrm{C}_{2}^{*}$ emission strength in lean to fuel-rich stoichiometries. Measurements have been performed in a set of low-pressure flames which have already been well characterized by other methods. The flame front is resolved in these measurements, which allows a comparison of shape and position of the observed chemiluminescence with the respective simulated concentrations. To study the effects of varying fuels, methane flame diluted in hydrogen are measured as well. The 14 investigated premixed methane–oxygen–argon and methane–hydrogen–oxygen–argon flames span a wide parameter field of fuel stoichiometry (?=0.5 to 1.6) and hydrogen content (H2 vol%=0 to 50). The relative comparison of measured and simulated excited species concentrations shows good agreement. The detailed and reliable modeling for several chemiluminescent species permits correlating heat release with all of these emissions under a large set of flame conditions. It appears from the present study that the normally used product of formaldehyde and OH concentration may be less well suited for such a prediction in the flames under investigation. 相似文献
Flame propagation under mixture stratification is relevant to a wide range of applications including gas turbine combustors and internal combustion engines. One of the local stratification effects is known as the back-support effect, where the laminar flame speed is modified when a premixed flame propagates into gradually richer or leaner mixtures. A majority of previous studies have focused on the propagation of methane/air stratified flames under standard temperature and pressure. However, stratified combustion often occurs under elevated temperature and pressure in practical applications, which may influence the characteristics of the back support effect through modified reaction pathways. This study performs numerical simulations of stratified laminar counterflow flames under an Atmospheric Temperature and Pressure (ATP) condition and an Elevated Temperature and Pressure (ETP) condition and examines the influence of elevated temperature and pressure on the back-support effect. Reaction flow analyses were extensively conducted to elucidate the difference in the primary reaction pathway between the two conditions. When scaled by the stratification Damköhler number, the back-support effect on the rich-to-lean stratified flame is weaker under the ETP condition than the ATP condition in the stoichiometric to lean region. This is due to increased contribution from reactions involved with OH radicals under the ETP condition, which leads to lower H2 reproduction in the reaction zone than under the ATP condition. The contribution from OH radicals is increased under the ETP condition because the conversion of H into OH is enhanced. These results suggest that the back-support effect may become negligibly small in practical combustors operating under elevated temperature and pressure due to (1) the flame being less sensitive to stratification because of the thinner flame, and (2) the lower H2 reproduction that deteriorates the radical production that drives the back-support effect. 相似文献
A review of the physics and modelling of mass diffusion involving different gaseous chemical species is firstly proposed. Both accurate and simplified models for mass diffusion involve the calculation of individual species diffusion coefficients. Since these are computationally expensive, in CFD they are commonly estimated by assuming constant Lewis or Schmidt numbers for each chemical species. The constant Lewis number assumption is particularly used. As a matter of fact, these assumptions have never been theoretically justified nor verified in practical flames. The only published information are the first observations by Smooke and Giovangigli about the Lewis number against temperature distributions in methane–air premixed and counterflow diffusion one-dimensional flames. The aim of this work is to verify these assumptions. Functional dependences of molecular properties appearing in these numbers are made explicit to show that while Sci depends only on composition, Lei depends also on temperature and therefore it certainly cannot be assumed constant in a flame. Then, accurately calculating molecular properties, distributions of these characteristic numbers against temperature are obtained a posteriori from numerical simulations of different flames, premixed and non-premixed, and burning different fuels. For non-premixed flames, individual species Lewis number distributions are broad for most of the species considered in this article, whilst they are tight for premixed flames. Some attention is focused on the particular shape of Lewis distributions in non-premixed flames: they are characterized by four or five (when extinction is experienced) branches associated to precise regions in the flame (basically, lean, rich and stoichiometric combusting zones). Instead, the Schmidt distributions are always tighter, also when extinctions take place: for many species they can be approximatively assumed constant. Finally, a simplified procedure to estimate individual species diffusion coefficients is suggested, assuming the median of non-premixed flame Schmidt distributions has a constant value for each chemical species. 相似文献
The effect of CO2 dilution on the flame characteristics and pollutant emission of a partially premixed CH4-air flame in a confined bluff body and swirl influenced flowfield is investigated using optical and laser diagnostic methods. The non-premixed burner produced a converging-diverging flowfield at the burner exit and a lifted flame is produced at all test cases, with an upstream movement of the flame with decreasing global equivalence ratios (?g). Based on variations in ?g, two flame stabilization modes – bluff body influenced and swirl stabilized – with a transition mode in-between is observed for the cases with (flame FB) and without dilution (flame FM). The characteristics of the heat release zone are influenced by dilution, with the FB flames being longer and also less intense when compared to FM flames. Pollutant measurement at 30 mm downstream from the combustor exit highlighted the ultra-low NOx capability of the IIST-GS2 burner. CO2 dilution leads to a reduction in NOx emission due to both thermal and chemical effects. For ?g ≥ 0.7 extreme low levels of CO and unburned hydrocarbons (UHC) are observed for both cases. For ?g ≤ 0.6 the dramatic increase of both CO and UHC maybe due to the lower flame temperatures and shorter flame zone residence times, respectively. 相似文献