Solid support flame synthesis of 1-D and 3-D tungsten-oxide nanostructures

In this paper we report the growth of 1-D and 3-D tungsten-oxide nanostructures on tungsten wire probes inserted in an opposed-flow oxy-fuel flame. The probe diameter and oxygen content in the oxidizer were varied to study their influence on the growth of tungsten-oxide nanostructures. The introduction of a 1-mm diameter W probe into the flame environment with an oxidizer composition of 50%O₂ + 50%N₂, resulted in the formation of 1-D nanorods on the upper surface of the probe. The formation of triangular, rectangular, square, and cylindrical 3-D channels with completely hollow or semi-hollow morphology was achieved by reducing the probe diameter to 0.5 mm. Whereas, the increase of the O₂ content to 100% and the employment of a 1-mm probe resulted in the growth of ribbon-like micron-sized structures. The lattice spacing of ∼0.38 nm measured for the 1-D W-oxides closely matches a monoclinic WO₃ structure. X-ray photoelectron spectroscopy analysis revealed that the larger 3-D structures also consist of WO₃ confirming that the chemical composition of the structures remains the same while varying the probe and flame parameters. The proposed growth mechanism states that the 3-D WO₃ structures are formed through the lateral coalescence of 1-D W-oxide nanorods.     

Catalyst influence on the flame synthesis of aligned carbon nanotubes and nanofibers

Since prepared substrates offer an appropriate method for the selective production of uniform arrays of aligned CNTs and CNFs, it is important to illustrate the influence of different catalysts on the resulting nanostructures. This investigation characterizes the activity of three catalysts—iron in alloyed form as stainless steel, nickel, and platinum—on carbon nanostructure formation under identical conditions in an ethylene/air nonpremixed flame. We have synthesized well-aligned multi-walled CNTs (on Ni) and CNFs (on stainless steel). The third transition metal Pt produces CNF structures of a different kind, and its activity has not been previously characterized in flames. The catalyst and gas-phase conditions leading to the formation of these different structures are discussed.     

Uncertainty assessment of species measurements in acetone counterflow diffusion flames

To quantitatively understand the uncertainty of intrusive species sampling measurements using a microprobe, velocity and speciation profiles of acetone counterflow diffusion flames have been experimentally investigated with cross validations using non-intrusive particle image velocimetry (PIV) and laser induced fluorescence (LIF) measurements. It is shown that the separation distance between the fuel and oxidizer nozzles needs to be sufficiently large to achieve uniform radial velocity profiles at the nozzle exit and accurate measurements of fuel concentration distributions in flames. The impacts of the diffusion flame location relative to the stagnation plane and the diffusion flame thickness on quantitative species sampling are investigated by varying the fuel to oxygen ratio as well as nitrogen and helium as fuel diluents. The results show that the diffusion flame needs to be located on the fuel side far from the stagnation plane in order to obtain reliable speciation measurements of fuel oxidation-related species. For helium dilution in the fuel side, a significant deviation from the model prediction is found due to the excessively fast diffusion velocity of helium. The impact of the intrusive probe on the flow field and the structure of the counterflow diffusion flame are identified by acetone and OH LIF measurements. The uncertainty in the speciation measurement associated with flow perturbations by the probe is quantified and found to be comparable to the outer diameter of the probe, ±0.3 mm. A simple Reynolds number analysis shows that the flow near the probe is just on the outskirts of the Stokes regime. Finally, the structure of the acetone diffusion flame is measured quantitatively with species measurements of ethane, ethylene, and acetylene. The comparison between predictions and measurements indicate that the current C₂ kinetic mechanism needs to be improved for quantitative prediction of the acetone flame structures.     

On the chemical characteristics and dynamics of n-alkane low-temperature multistage diffusion flames

We demonstrate experimentally, perhaps for the first time, the existence of low-temperature multistage diffusion flames of n-alkanes. Multistage diffusion flames of n-heptane, n-decane, and n-dodecane are established in an atmospheric counterflow burner. Planar laser-induced fluorescence, chemiluminescence, and thermometry are used to probe the structures of such flames. In the first flame zone, the majority of the fuel is partially oxidized via low-temperature peroxy chemistry. In the second flame zone, the intermediate species produced are further oxidized via intermediate-temperature chemistry. The two stages of the flame are coupled such that significant fuel and oxidizer leakage occur, respectively, from the first and second reaction zones. The fuel is then further consumed, in the second stage, after the radical pool is replenished by the oxidation of the intermediates. The structure of the n-alkane multistage flame is found to be consistent with that previously observed for acyclic ethers. Owing to the different classes of temperature-dependent chemistries dominating the first and second stages, the reaction zone structure of multistage diffusion flames is dramatically influenced by the reactant concentrations and flame temperatures. The first stage is relatively favored at lower temperatures whereas the second stage is favored at elevated temperatures. Moreover, near extinction where the flame temperature is low, the multistage flame dynamics are controlled by the first oxidation stage, governed by peroxy chemistry, whereas the second oxidation stage, governed by intermediate chemistry, is dominant near high-temperature ignition conditions. Finally, by doping the oxidizer with ozone, we demonstrate the role of ozone doping on the multistage flame structure and the existence of a separate low-temperature ozone-assisted burning mode.     

Structure of partially premixed n-heptane–air counterflow flames

To avoid the complexities associated with the droplet/vapor transport and nonuniform evaporation processes, a fundamental investigation of liquid fuel combustion in idealized configurations is very useful. An experimental–computational investigation of prevaporized n-heptane nonpremixed and partially premixed flames established in a counterflow burner is described. There is a general agreement between various facets of our nonpremixed flame measurements and the literature data. The partially premixed flames are characterized by a double flame structure. This becomes more distinct as the strain rate decreases and partial premixing increases, which also increases the separation distance between the two reaction zones. The peak partially premixed flame temperature increases with increasing premixing of the fuel stream. The peak CO₂ and H₂O concentrations are relatively insensitive to partial premixing. The CO and H₂ peak concentrations on the premixed side increase as the fuel-side equivalence ratio decreases. These species are transported to the nonpremixed reaction zone where they oxidize. The C₂ species have peaks in the premixed reaction zone. The concentrations of olefins are ten times larger than those of the corresponding paraffins. The oxidizer is present in partially premixed flames throughout the combustion system and there are no regions characterized by simultaneous high temperature and high fuel concentration. As a result, pyrolysis reactions leading to soot formation are greatly diminished.     

LES of oxy-fuel jet flames using the Eulerian Stochastic Fields method with differential diffusion

The Eulerian Stochastic Fields (ESF) Monte Carlo method to solve the transported PDF (TPDF) equation is extended to account for differential diffusion effects by incorporating species individual molecular diffusivities. The method has been applied in Large Eddy simulation (LES) to non-piloted oxy-fuel jet flames at different Reynolds numbers experimentally investigated by Sevault et al. [1]. Due to the high H₂ content in the fuel stream and CO₂ in the oxidizer these flames pose new challenges to combustion modeling as the flame structures are different compared to CH₄/air flames. The simulations show very good agreement with the experiments in terms of mixture fraction conditional mean values for temperature and mayor species on the fuel lean side and the reaction zone, deviations on the fuel rich side are discussed. The trend and location of localized extinction is reproduced well in the simulations, as well as differential diffusion effects in the near field. Additionally, it is shown that a neglect of differential diffusion in the combustion model leads to a lifted flame.     

Combustion of a high-velocity hydrogen microjet effluxing in air

This study is devoted to experimental investigation of hydrogen-combustion modes and the structure of a diffusion flame formed at a high-velocity efflux of hydrogen in air through round apertures of various diameters. The efflux-velocity range of the hydrogen jet and the diameters of nozzle apertures at which the flame is divided in two zones with laminar and turbulent flow are found. The zone with the laminar flow is a stabilizer of combustion of the flame as a whole, and in the zone with the turbulent flow the intense mixing of fuel with an oxidizer takes place. Combustion in these two zones can occur independently from each other, but the steadiest mode is observed only at the existence of the flame in the laminar-flow zone. The knowledge obtained makes it possible to understand more deeply the features of modes of microjet combustion of hydrogen promising for various combustion devices.     

Experimental investigation on the flame front resistance of gas channel growth with melt formation in iron ore sinter beds

The resistance of the flame front within the solid bed constitutes a fundamental and crucial area in porous bed combustion as the flame front propagation is highly related to the productivity and product quality. This paper focuses on the iron ore sintering, a thermal agglomeration process in steel mills. The results from a detailed experimental study of the pilot-scale pot tests under the conditions of a wide range of fuel rate are presented. The primary objective is to provide better understanding of the growth of gas channels relating to melt formation in the flame front and its resistance to flow. The sintering bed was divided into several zones based on the temperature profile and component distribution. Even though there is a continuous one-to-one replacement of humidified zone with porous sintered zone, a constant air flow rate during sintering could be obtained, indicating the ～100?mm high-temperature zone has a controlling effect on sintering bed permeability. The specific pressure drop value in high-temperature zone increases from ～3?kPa in upper bed to ～7?kPa in bottom bed, which varies with the bed temperature and structure properties. Both the green bed and sintered bed were scanned by X-ray computed tomography, the reconstruction and image analysis showed that the sintered bed has large gas channels and many more closed pores due to solid-melt-gas coalescence. More melt is generated when the heat is accumulated along the bed or input higher coke content, showing a propensity to suppress the gas channel growth and amplify the mismatch of gas transportation along the bed. Higher coke rate leads to a higher resistance in flame front, resulting in a slower flame front speed. These results are aimed to provide quantitative validation for improvements of a numerical sintering model in a future work.     

Formation of the preheated zone ahead of a propagating flame and the mechanism underlying the deflagration-to-detonation transition

The Letter presents analytical, numerical and experimental studies of the mechanism underlying the deflagration-to-detonation transition (DDT). Insight into how, when, and where DDT occurs is obtained by analyzing analytically and by means of multidimensional numerical simulations dynamics of a flame accelerating in a tube with no-slip walls. It is shown that the deflagration-to-detonation transition exhibits three separate stages of evolution corroborating majority experimental observations. During the first stage flame accelerates and generates shocks far ahead of the flame front. During the second stage the flame slows down, shocks are formed in the immediate proximity of the flame front and the preheated zone ahead of the flame front is created. The third stage is self-restructuring of the steep temperature profile within the flame, formation of a reactivity gradient and the actual formation of the detonation wave itself. The mechanism for the detonation wave formation, given an appropriate formation of the preheated zone, seems to be universal and involves a reactivity gradient formed from the initially steep flame temperature profile in the presence of the preheated zone. The developed theory and numerical simulations are found to be well consistent with extensive experiments of the DDT in hydrogen-oxygen and ethylene-oxygen mixtures in tubes with smooth and rough walls.     

Single-walled carbon nanotube formation on iron oxide catalysts in diffusion flames

Single-walled carbon nanotubes (SWCNTs) are shown to grow rapidly on iron oxide catalysts on the fuel side of an inverse ethylene diffusion flame. The pathway of carbon in the flame is controlled by the flame structure, leading to formation of SWCNTs free of polycyclic aromatic hydrocarbons (PAH) or soot. By using a combination of oxygen-enrichment and fuel dilution, fuel oxidation is favored over pyrolysis, PAH growth, and subsequent soot formation. The inverse configuration of the flame prevents burnout of the SWCNTs while providing a long carbon-rich region for nanotube formation. Furthermore, flame structure is used to control oxidation of the catalyst particles. Iron sub-oxide catalysts are highly active toward SWCNT formation while Fe and Fe₂O₃ catalysts are less active. This can be understood by considering the effects of particle oxidation on the dissociative adsorption of gas-phase hydrocarbons. The optimum catalyst particle composition and flame conditions were determined in near real-time using a scanning mobility particle sizer (SMPS) to measure the catalyst and SWCNT size distributions. In addition, SMPS results were combined with flame velocity measurement to measure SWCNT growth rates. SWCNTs were found to grow at rates of over 100 μm/s.     

Flame structure and stabilization of lean-premixed sprays in a counterflow with low-volatility fuel

An experimental study was performed on the combustion of lean-premixed spays in a counterflow. n-Decane was used as a liquid fuel with low volatility. The flame structure and stabilization were discussed based on the flame-spread mechanism of a droplet array with a low-volatility fuel. The spray flame consisted of a blue region and a yellow luminous region. The flame spread among droplets and group-flame formation through the droplet interaction were observed on the premixed spray side, while envelope flames were also observed on the opposing airflow side. The blue-flame region consisted of premixed flames propagating in the mixture layer around each droplet, the envelope diffusion flames around each droplet, the lower parts of the group diffusion flame surrounding each droplet cluster, and the envelope flame around droplets passing through the group flame. The flame was stabilized within a specific range of the mean droplet diameter via a balance between the droplet velocity and the flame-spread rate of the premixed spray.     

The extended IEM mixing model in the framework of the composition PDF approach: applications to diesel spray combustion

A steady, two-dimensional corner flame is established when fuel and oxidizer enter the reaction zone in mutually perpendicular directions. A model problem in which the velocity fields are linear functions of spatial position is utilized to study the resulting flame. The flame structure is comprised of a diffusion flame surrounded on either side by fuel-rich and fuel-lean partially premixed laminar flames, similar to, but distinct from, triple flames. Using suitable coordinate transformations and change of variables, the governing equations in the thermodiffusive approximation are recast into a form akin to classical triple flames, with the strain rate appearing as the eigenvalue. A new exact integral representation of the solution to the mixture fraction equation is then utilized and high activation energy asymptotics are applied to solve approximately for the resulting flame shape, the imposed strain rate and, most significantly, the position of flame stabilization. This theoretically predicted flame is computed numerically, and comparisons are made between theory and computation.     

Transition of carbon nanostructures in heptane diffusion flames

The flame synthesis has high potential in industrial production of carbon nanostructure (CNS). Unfortunately, the complexity of combustion chemistry leads to less controlling of synthesized products. In order to improve the understanding of the relation between flames and CNSs synthesized within, experiments were conducted through heptane flames in a stagnation-point liquid-pool system. The operating parameters for the synthesis include oxygen supply, sampling position, and sampling time. Two kinds of nanostructures were observed, carbon nanotube (CNT) and carbon nano-onion (CNO). CNTs were synthesized in a weaker flame near extinction. CNOs were synthesized in a more sooty flame. The average diameter of CNTs formed at oxygen concentration of 15% was in the range of 20–30 nm. For oxygen concentration of 17%, the average diameter of CNTs ranged from 24 to 27 nm, while that of CNOs was around 28 nm. For oxygen concentration of 19%, the average diameter of CNOs produced at the sampling position 0.5 mm below the flame front was about 57 nm, while the average diameters of CNOs formed at the sampling positions 1–2.5 mm below the flame front were in the range of 20–25 nm. A transition from CNT to CNO was observed by variation of sampling position in a flame. We found that the morphology of CNS is directly affected by the presence of soot layer due to the carbonaceous environment and the growth mechanisms of CNT and CNO. The sampling time can alter the yield of CNSs depending on the temperature of sampling position, but the morphology of products is not affected.     

Combustion of partially premixed spray jets

Gas turbines, liquid rocket motors, and oil-fired furnaces utilize the spray combustion of continuously injected liquid fuels. In most cases, the liquid spray is mixed with an oxidizer prior to combustion, and further oxidizer is supplied from the outside of the spray to complete diffusion combustion. This rich premixed spray is called “partially premixed spray.” Partially premixed sprays have not been studied systematically although they are of practical importance. In the present study, the burning behavior of partially premixed sprays was experimentally studied with a newly developed spray burner. A fuel spray and an oxidizer, diluted with nitrogen, was injected into the air. The overall equivalence ratio of the spray jet was set larger than unity to establish partially premixed spray combustion. In the present burner, the mean droplet diameter of the atomized liquid fuel could be varied without varying the overall equivalence ratio of the spray jet. Two combustion modes with and without an internal flame were observed. As the mean droplet diameter was increased or the overall equivalence ratio of the spray jet was decreased, the transition from spray combustion only with an external group flame to that with the internal premixed flame occurred. The results suggest that the internal flame was supported by flammable mixture through the vaporization of fine droplets, and the passage of droplet clusters deformed the internal flame and caused internal flame oscillation. The existence of the internal premixed flame enhanced the vaporization of droplets in the post-premixed-flame zone within the external diffusion flame.     

Diffusion-controlled combustion of gases in the absence of forced convection

A mathematical model for the laminar diffusion combustion of gases in the absence of forced convection is developed. This combustion mode is realized near an orifice in the partition that separates the fuel and oxidizer. The stationary solution, size and shape of the flame, temperature distribution, and profiles of the concentrations of fuel, oxidizer, and combustion products are determined. It is shown that the limiting diameter of the diffusion flame is inversely proportional to the burning rate of an equivalent premixed mixture of the same fuel and oxidizer, whereas the flame length is proportional to the diameter of the orifice. The unsteady (quasi-stationary) solution to this problem for the case where the gas is confined in a finite-volume vessel is obtained. The time it takes the flame to approach the partition of the vessel with fuel and enter inside is determined. Experiments on studying the diffusion combustion of natural gas in the absence of forced convection near orifices and a slit in the partition separating the gaseous fuel and oxidizer in a finite-volume vessel are performed. The time of combustion is obtained. Depending on the orifice diameter and slit width, three modes of diffusion combustion were identified: combustion above the partition ending in flame extinction, combustion with a breakthrough, and combustion inside the vessel (submerged flame).     

Simultaneous OH-PLIF and PIV measurements in a gas turbine model combustor

In highly turbulent environments, combustion is strongly influenced by the effects of turbulence chemistry interactions. Simultaneous measurement of the flow field and flame is, therefore, obligatory for a clear understanding of the underlying mechanisms. In the current studies simultaneous PIV and OH-PLIF measurements were conducted in an enclosed gas turbine model combustor for investigating the influence of turbulence on local flame characteristics. The swirling CH₄/air flame that was investigated had a thermal power of 10.3 kW with an overall equivalence ratio of ϕ=0.75 and exhibited strong thermoacoustic oscillations at a frequency of approximately 295 Hz. The measurements reveal the formation of reaction zones at regions where hot burned gas from the recirculation zones mixes with the fresh fuel/air mixture at the nozzle exit. However, this does not seem to be a steady phenomenon as there always exist regions where the mixture has failed to ignite, possibly due to the high local strain rates present, resulting in small residence time available for a successful kinetic runaway to take place. The time averaged PIV images showed flow fields typical of enclosed swirl burners, namely a big inner recirculation zone and a small outer recirculation zone. However, the instantaneous images show the existence of small vortical structures close to the shear layers. These small vortical structures are seen playing a vital role in the formation and destruction of reaction zone structures. One does not see a smooth laminar flame front in the instantaneous OH-PLIF images, instead isolated regions of ignition and extinction highlighting the strong interplay between turbulence and chemical reactions. PACS 33.20.-t; 33.50.-j; 47.27.-i; 47.32.Ef; 47.70.Pq; 82.33.Vx; 82.40.-g     

W型火焰燃烧的实验研究

本文设计了1 MW“W型”火焰煤粉燃烧实验台,并对焦作无烟煤进行了热态试验,分析了炉膛最高温度(火焰中心)的位置对W火焰的稳定形成的重要性,通过实验测得了其合理的相关位置。实验结果表明: W型火焰燃烧有很强的低负荷稳燃性,特别适合于低挥发份煤的燃烧。当火焰中心位置处于最下层二次风处时,炉内才能形成较好的W火焰;下炉膛中前后墙的壁面热负荷较为均匀,而左右墙的壁面热负荷分布呈“中间温度高两边温度低”的特性;上炉膛左右墙与前后墙的壁面温度分布基本一致。     

Transient and steady-state behavior of auto-igniting propane and dimethyl ether fuel jets in high-temperature vitiated coflows

In the current study, the auto-ignition dynamics of cold fuel jets issuing into a high-temperature, vitiated environments is investigated. Due to the short time scale of these events, high-speed measurements are used to resolve the coupled spatio-temporal behavior. The present study uses high-speed (20-kHz) OH* chemiluminescence imaging to identify the location and timing of the formation of the initial ignition kernels, providing visualization of the ignition dynamics and a detailed statistical evaluation of ignition heights and ignition delay times across a broad parameter space which includes variations in fuel type, dilution levels, coflow temperature, and coflow oxidizer content. The auto-ignition location and ignition delay times show a strong sensitivity to coflow temperature with increased sensitivities at lower coflow temperatures. Comparisons between kernel formation location for the transient jet and the fluctuating flame base of the subsequent, steady-state flame is presented, highlighting the role of flame propagation on flame stabilization. Results indicate that at lower temperatures the flame stabilization mechanism is dominated by auto-ignition, but at higher coflow temperatures, flame propagation plays a key role. The effects of variations in the hot, coflow oxidizer content on ignition properties were found to be noticeable, but still significantly less than variations in the temperature.     

On the mechanism of the deflagration-to-detonation transition in a hydrogen-oxygen mixture

The flame acceleration and the physical mechanism underlying the deflagration-to-detonation transition (DDT) have been studied experimentally, theoretically, and using a two-dimensional gasdynamic model for a hydrogen-oxygen gas mixture by taking into account the chain chemical reaction kinetics for eight components. A flame accelerating in a tube is shown to generate shock waves that are formed directly at the flame front just before DDT occurred, producing a layer of compressed gas adjacent to the flame front. A mixture with a density higher than that of the initial gas enters the flame front, is heated, and enters into reaction. As a result, a high-amplitude pressure peak is formed at the flame front. An increase in pressure and density at the leading edge of the flame front accelerates the chemical reaction, causing amplification of the compression wave and an exponentially rapid growth of the pressure peak, which “drags” the flame behind. A high-amplitude compression wave produces a strong shock immediately ahead of the reaction zone, generating a detonation wave. The theory and numerical simulations of the flame acceleration and the new physical mechanism of DDT are in complete agreement with the experimentally observed flame acceleration, shock formation, and DDT in a hydrogen-oxygen gas mixture.     

Investigation of droplet combustion in strained counterflow diffusion flames using planar laser-induced fluorescence

Experimental investigation of an isolated droplet burning in a convective flow is reported. Acetone droplets were injected in a steady laminar diffusion counterflow flame operating with methane. Planar laser-induced fluorescence measurements applied to OH radical and acetone was used to measure the spatial distribution of fuel vapour and the structure of the flame front around the droplet. High-magnification optics was used in order to image flow areas with a ratio of 1:1.2. The different combustion regimes of an isolated droplet could be observed from the configuration of the envelope flame to that of the boundary-layer flame, and occurrence of these regimes was found to depend on the droplet Reynolds number. Experimental results were compared with 1D numerical simulations using detailed chemistry for the configuration of the envelope flame. Good agreement was obtained for the radial profile of both OH radical and fuel vapour. Influence of droplet dynamics on the counterflow flame front was also investigated. Results show that the flame front could be strongly distorted by the droplet crossing. In particular, droplets with high velocity led to local extinction of the flame front whereas droplets with low velocity could ignite within the flame front and burn on the oxidiser side. PACS 33.50.-j; 42.62.-b; 47.55.D-; 47.70.Pq; 47.80.Jk