Experimental and numerical investigation of hetero-/homogeneous combustion of CO/H2/O2/N2 mixtures over platinum at pressures up to 5 bar

The hetero-/homogeneous combustion of fuel-lean CO/H₂/O₂/N₂ mixtures over platinum is investigated at pressures up to 5 bar, inlet temperatures (T_IN) up to 874 K, and a constant CO:H₂ molar ratio of 2:1. Experiments are performed in an optically accessible channel-flow catalytic reactor and involve planar laser induced fluorescence (LIF) of the OH radical for the assessment of homogeneous (gas-phase) ignition and 1-D Raman measurements of major gas-phase species concentrations over the catalyst boundary layer for the evaluation of the heterogeneous (catalytic) processes. Simulations are carried out with an elliptic 2-D model that includes detailed heterogeneous and homogeneous chemical reaction schemes. The predictions reproduce the Raman-measured catalytic CO and H₂ consumption, and it is further shown that for wall temperatures in the range 975 ? T_w ? 1165 K the heterogeneous pathways of CO and H₂ are largely decoupled. However, for wall temperatures below a limiting value of 710–720 K and for the range of pressures and mixture preheats investigated, CO(s) blockage of the surface inhibits the catalytic conversion of both fuel components. The homogeneous ignition distance is well-reproduced by the model for T_IN > 426 K, but it is modestly overpredicted at lower T_IN. Possible reasons for these modest differences can be the values of third body efficiencies in the gas-phase reaction mechanism. The sensitivity of homogeneous ignition distance on the catalytic reactions is weak, while the H₂/O₂ subset of the CO/H₂/O₂ gaseous reaction mechanism controls the onset of homogeneous ignition. Pure hydrogen hetero-/homogeneous combustion results in flames established very close to the catalytic walls. However, in the presence of CO the gaseous combustion of hydrogen extends well-inside the channel core, thus allowing homogeneous consumption of H₂ at considerably shorter reactor lengths. Finally, implications of the above findings for the design of syngas-based catalytic reactors for power generation systems are discussed.     

Hetero-/homogeneous combustion of hydrogen/air mixtures over platinum at pressures up to 10 bar

The hetero-/homogeneous combustion of fuel-lean hydrogen/air premixtures over platinum was investigated experimentally and numerically in the pressure range 1 bar  p  10 bar. Experiments were carried out in an optically accessible channel-flow catalytic reactor and included planar laser induced fluorescence (LIF) of the OH radical for the assessment of homogeneous (gas-phase) ignition, and 1-D Raman measurements of major gas-phase species concentrations for the evaluation of the heterogeneous (catalytic) processes. Simulations were performed with a full-elliptic 2-D model that included detailed heterogeneous and homogeneous chemical reaction schemes. The predictions reproduced the measured catalytic hydrogen consumption, the onset of homogeneous ignition at pressures of up to 3 bar and the diminishing gas-phase combustion at p  4 bar. The suppression of gaseous combustion at elevated pressures bears the combined effects of the intrinsic homogeneous hydrogen kinetics and of the hetero/homogeneous chemistry coupling via the catalytically produced water over the gaseous induction zone. Transport effects, associated with the large diffusivity of hydrogen, have a smaller impact on the limiting pressure above which gaseous combustion is suppressed. It is shown that for practical reactor geometrical confinements, homogeneous combustion is still largely suppressed at p  4 bar even for inlet and wall temperatures as high as 723 and 1250 K, respectively. The lack of appreciable gaseous combustion at elevated pressures is of concern for the reactor thermal management since homogeneous combustion moderates the superadiabatic surface temperatures attained during the heterogeneous combustion of hydrogen.     

Experimental and numerical investigation of the hetero-/homogeneous combustion of lean propane/air mixtures over platinum

The pure heterogeneous and the coupled hetero-/homogeneous combustion of fuel-lean propane/air mixtures over platinum have been investigated at pressures 1 bar  p  7 bar, fuel-to-air equivalence ratios 0.23  φ  0.43, and catalytic wall temperatures 723 K  T_w  1286 K. Experiments were performed in an optically accessible catalytic channel-flow reactor and involved 1-D Raman measurements of major gas-phase species concentrations across the reactor boundary layer for the assessment of catalytic fuel conversion and planar laser induced fluorescence (LIF) of the OH radical for the determination of homogeneous ignition. Numerical predictions were carried out with a 2-D elliptic CFD code that included a one-step catalytic reaction for the total oxidation of propane on Pt, an elementary C₃ gas-phase chemical reaction mechanism, and detailed transport. A global catalytic reaction step valid over the entire pressure–temperature-equivalence ratio parameter range has been established, which revealed a p^0.75 dependence of the catalytic reactivity on pressure. The aforementioned global catalytic step was further coupled to a detailed gas-phase reaction mechanism in order to simulate homogeneous ignition characteristics in the channel-flow reactor. The predictions reproduced within 10% the measured homogeneous ignition distances at pressures p  5 bar, while at p = 7 bar the simulations overpredicted the measurements by 19%. The overall model performance suggests that the employed hetero-/homogeneous chemical reaction schemes are suitable for the design of propane-fueled catalytic microreactors.     

Homogeneous ignition of CH4/air and H2O and CO2-diluted CH4/O2 mixtures over Pt; an experimental and numerical investigation at pressures up to 16 bar

The homogeneous ignition of CH₄/air, CH₄/O₂/H₂O/N₂, and CH₄/O₂/CO₂/N₂ mixtures over platinum was investigated experimentally and numerically at pressures 4 bar p 16 bar, temperatures 1120 K T 1420 K, and fuel-to-oxygen equivalence ratios 0.30 0.40. Experiments have been performed in an optically accessible catalytic channel-flow reactor and included planar laser induced fluorescence (LIF) of the OH radical for the determination of homogeneous (gas-phase) ignition and one-dimensional Raman measurements of major species concentrations across the reactor boundary layer for the assessment of the heterogeneous (catalytic) processes preceding homogeneous ignition. Numerical predictions were carried out with a 2D elliptic CFD code that included elementary heterogeneous and homogeneous chemical reaction schemes and detailed transport. The employed heterogeneous reaction scheme accurately captured the catalytic methane conversion upstream of the gaseous combustion zone. Two well-known gas-phase reaction mechanisms were tested for their capacity to reproduce measured homogeneous ignition characteristics. There were substantial differences in the performance of the two schemes, which were ascribed to their ability to correctly capture the p–T– parameter range of the self-inhibited ignition behavior of methane. Comparisons between measured and predicted homogeneous ignition distances have led to the validation of a gaseous reaction scheme at 6 bar p 16 bar, a pressure range of particular interest to gas-turbine catalytically stabilized combustion (CST) applications. The presence of heterogeneously produced water chemically promoted the onset of homogeneous ignition. Experiments and predictions with CH₄/O₂/H₂O/N₂ mixtures containing 57% per volume H₂O have shown that the validated gaseous scheme was able to capture the chemical impact of water in the induction zone. Experiments with CO₂ addition (30% per volume) were in good agreement with the numerical simulations and have indicated that CO₂ had only a minor chemical impact on homogeneous ignition.     

Simulations and experiments on the ignition probability in turbulent premixed bluff-body flames

The ignition characteristics of a premixed bluff-body burner under lean conditions were investigated experimentally and numerically with a physical model focusing on ignition probability. Visualisation of the flame with a 5 kHz OH* chemiluminescence camera confirmed that successful ignitions were those associated with the movement of the kernel upstream, consistent with previous work on non-premixed systems. Performing many separate ignition trials at the same spark position and flow conditions resulted in a quantification of the ignition probability P_ign, which was found to decrease with increasing distance downstream of the bluff body and a decrease in equivalence ratio. Flows corresponding to flames close to the blow-off limit could not be ignited, although such flames were stable if reached from a richer already ignited condition. A detailed comparison with the local Karlovitz number and the mean velocity showed that regions of high P_ign are associated with low Ka and negative bulk velocity (i.e. towards the bluff body), although a direct correlation was not possible. A modelling effort that takes convection and localised flame quenching into account by tracking stochastic virtual flame particles, previously validated for non-premixed and spray ignition, was used to estimate the ignition probability. The applicability of this approach to premixed flows was first evaluated by investigating the model's flame propagation mechanism in a uniform turbulence field, which showed that the model reproduces the bending behaviour of the S_T-versus-u′ curve. Then ignition simulations of the bluff-body burner were carried out. The ignition probability map was computed and it was found that the model reproduces all main trends found in the experimental study.     

Experiments and modeling of ignition delay times, flame structure and intermediate species of EHN-doped stoichiometric n-heptane/air combustion

The combustion of stoichiometric Ethyl-hexyl-nitrate (EHN)-doped n-heptane/oxygen/argon and (EHN)-doped n-heptane/air mixtures, respectively, was investigated in a low-pressure burner with a molecular-beam mass spectrometer and ignition delay-time (τ_ign) measurements were performed in a high-pressure shock tube. The experiments with the low-pressure flame were used for the determination of the flame structure including concentration profiles of reactants, products and important intermediates in the flame. The shock tube experiments provided τ_ign for a temperature range of 690 K ? T ? 1275 K at a pressure of 40 ± 2 bar for stoichiometric and lean mixtures under engine relevant conditions. A chemical mechanism for n-heptane/EHN mixtures was developed from an automatically generated mechanism for n-heptane by manually adding reactions to describe the influence of EHN. This mechanism was validated against the shock-tube data for various temperatures, levels of EHN-doping and equivalence ratios by homogeneous reactor calculations.The ignition delay times predicted by the model agree well with the shock tube results for a large range of temperatures, equivalence ratios and EHN concentrations. The influence of EHN onto ignition delay was largest in the low-temperature regime (770-1000 K).Numerical analysis suggests that the prevalent reason for the ignition-enhancing effect of EHN is the formation of highly reactive heptyl radicals by thermal decomposition of EHN. Due to this comparatively simple and generic mechanism, EHN is expected to have a similar ignition-enhancing effect also for other hydrocarbon fuels.     

Effect of methane on pilot-fuel auto-ignition in dual-fuel engines

The ignition behavior of n-dodecane micro-pilot spray in a lean-premixed methane/air charge was investigated in an optically accessible Rapid Compression-Expansion Machine at dual-fuel engine-like pressure/temperature conditions. The pilot fuel was admitted using a coaxial single-hole 100?µm injector mounted on the cylinder periphery. Optical diagnostics include combined high-speed CH₂O-PLIF (10?kHz) and Schlieren (80?kHz) imaging for detection of the first-stage ignition, and simultaneous high-speed OH* chemiluminescence (40?kHz) imaging for high-temperature ignition. The aim of this study is to enhance the fundamental understanding of the interaction of methane with the auto-ignition process of short pilot-fuel injections. Addition of methane into the air charge considerably prolongs ignition delay of the pilot spray with an increasing effect at lower temperatures and with higher methane/air equivalence ratios. The temporal separation of the first CH₂O detection and high-temperature ignition was found almost constant regardless of methane content. This was interpreted as methane mostly deferring the cool-flame reactivity. In order to understand the underlying mechanisms of this interaction, experimental investigations were complemented with 1D-flamelet simulations using detailed chemistry, confirming the chemical influence of methane deferring the reactivity in the pilot-fuel lean mixtures. This shifts the onset of first-stage reactivity towards the fuel-richer conditions. Consequently, the onset of the turbulent cool-flame is delayed, leading to an overall increased high-temperature ignition delay. Overall, the study reveals a complex interplay between entrainment, low T and high T chemistry and micro-mixing for dual-fuel auto-ignition processes for which the governing processes were identified.     

Partial catalytic oxidation of methane to synthesis gas over rhodium: in situ Raman experiments and detailed simulations

The partial catalytic oxidation of methane to synthesis gas over Rh/ZrO₂ was investigated experimentally and numerically at fuel-to-air equivalence ratios of 2.5 and 4.0 and pressures of 4 and 6 bar. Experiments were performed in an optically accessible, laboratory-scale, channel-flow catalytic reactor and involved in situ one-dimensional Raman measurements of major species (CH₄, O₂, H₂O, CO₂, H₂, CO, and N₂) concentrations across the reactor boundary layer. The numerical model included a two-dimensional elliptic code with elementary homogeneous (gaseous) and heterogeneous (catalytic) chemical reaction schemes. Homogeneous ignition experiments and numerical predictions have validated the employed gas-phase reaction mechanism and have further delineated the reactor extent over which the contribution of the homogeneous reaction pathway was negligible. Over the reactor extent where oxygen was still available, the employed heterogeneous reaction scheme provided good agreement with the measured species concentrations, overpredicting only to a small degree the partial over the total oxidation route. In the oxygen-depleted zones of the reactor, however, the heterogeneous scheme overpredicted to a greater degree the impact of steam reforming and water gas shift reactions, resulting in higher computed hydrogen yields at the reactor exit. Additional experiments and predictions were carried out in a sub-scale gas-turbine honeycomb reactor, at operating conditions leading to oxygen breakthrough. The predictions again favored the partial over the total oxidation route. A modified heterogeneous scheme was proposed that provided very good agreement with measurements in the honeycomb reactor and in the oxygen-rich zones of the laboratory-scale reactor. The hydrogen produced during partial oxidation was partly re-adsorbed on the catalyst leading to superadiabatic surface temperatures, thus exemplifying the importance of proper thermal management in commercial reactors.     

Hetero-/homogeneous combustion of ethane/air mixtures over platinum at pressures up to 14 bar

The hetero-/homogeneous combustion of fuel-lean ethane/air mixtures over platinum was investigated experimentally and numerically at pressures of 1–14 bar, equivalence ratios of 0.1–0.5, and surface temperatures ranging from 700 to 1300 K. Experiments were carried out in an optically accessible channel-flow reactor and included in situ 1-D Raman measurements of major gas phase species concentrations across the channel boundary layer for determining the catalytic reactivity, and planar laser induced fluorescence (LIF) of the OH radical for assessing homogeneous ignition. Numerical simulations were performed with a 2-D CFD code with detailed hetero-/homogeneous C₂ kinetic mechanisms and transport. An appropriately amended heterogeneous reaction scheme has been proposed, which captured the increase of ethane catalytic reactivity with rising pressure. This scheme, when coupled to a gas-phase reaction mechanism, reproduced the combustion processes over the reactor extent whereby both heterogeneous and homogeneous reactions were significant and moreover, provided good agreement to the measured homogeneous ignition locations. The validated hetero-/homogeneous kinetic schemes were suitable for modeling the catalytic combustion of ethane at elevated pressures and temperatures relevant to either microreactors or large-scale gas turbine reactors in power generation systems. It was further shown that the pressure dependence of the ethane catalytic reactivity was substantially stronger compared to that of methane, at temperatures up to 1000 K. Implications for high-pressure catalytic combustion of natural gas were finally drawn.     

Catalytic ignition and autothermal combustion of JP-8 and its surrogates over a Pt/γ-Al2O3 catalyst

With the aim of utilizing JP-8 fuel for small scale portable power generation systems, catalytic combustion of JP-8 is studied. The surface ignition, extinction and autothermal combustion of JP-8, of a six-component surrogate fuel mixture, and the individual components of the surrogate fuel over a Pt/γ-Al₂O₃ catalyst are experimentally investigated in a packed bed flow reactor. The surrogate mixture exhibits similar ignition–extinction behavior and autothermal temperatures compared to JP-8 suggesting the possibility of using this surrogate mixture for detailed kinetics of catalytic combustion of JP-8. It is shown that JP-8 ignites at low temperatures in the presence of catalyst. Upon ignition, catalytic combustion of JP-8 and the surrogate mixture is self-sustained and robust combustion is observed under fuel lean as well as fuel rich conditions. It is shown that the ignition temperature of the hydrocarbon fuels increases with increasing equivalence ratio. Extinction is observed under fuel lean conditions, whereas sustained combustion was also observed for fuel rich conditions. The effect of dilution in the air flow on the catalytic ignition and autothermal temperatures of the fuel mixture is also investigated by adding helium to the air stream while keeping the flow rate and the equivalence ratio constant. The autothermal temperature decreases linearly as the amount of dilution in the flow is increased, whereas the ignition temperature shows no dependence on the dilution level under the range of our conditions, showing that ignition is dependent only on the type and relative concentration of the active species.     

Kinetic analysis of n-decane–hydrogen blend combustion in premixed and non-premixed supersonic flows

Numerical analysis of ignition and combustion of an n-decane–hydrogen fuel blend in a premixed supersonic flow and in a model scramjet duct is performed using a reduced reaction mechanism built especially to describe the oxidation of blended n-C₁₀H₂₂–H₂ fuel in air at the temperature T₀ > 900–1000 K in the pressure range P₀ = 0.1–13 atm. The developed kinetic mechanism involves the principal reactions responsible for chain mechanism development both for n-decane and for hydrogen oxidation. It has been shown that using blended n-C₁₀H₂₂–H₂ fuel makes it possible to enhance the ignition and combustion both in premixed and in non-premixed supersonic fuel–air flows compared to burning pure hydrogen–air and n-decane–air mixtures. This allows high combustion completeness in the scramjet duct at the distance of ～1 m even at extremely low air temperature T₀ = 1000 K and pressure P₀ = 0.3 atm. This is due to the interaction of kinetics of the formation of highly reactive atoms and radicals, carriers of chain mechanism, in H₂–air and n-C₁₀H₂₂–air mixtures.     

On the influence of hydrogen on the low-temperature reactivity of n-pentane, 1-pentene and 3-pentanone: an experimental and modeling study

Hydrogen can be blended with other surrogate fuels to avoid its hazard as a highly flammable and explosive gas. The effect of hydrogen addition on the ignition delay times of n-pentane, 3-pentanone, and 1-pentene was investigated by measuring the ignition delay times in a rapid compression machine. The experiments were performed at pressures of 10, 15, and 20 bar, equivalence ratios 0.5 and 1 and for temperatures ranging from 650 to 970 K. The molar ratios of hydrogen in the fuel mixtures were 0, 25 and 50%. The experimental data were simulated using recent models from literature, yielding good agreement. The overall observations conclude to a minor effect of hydrogen addition in the case of n-pentane and 3-pentanone, resulting in a decrease of the reactivity when the mole fraction of hydrogen increases. Hydrogen does however not impact the ignition delay times of 1-pentene significantly. Kinetic analysis is performed to shed light into the processes responsible for this phenomenon.     

An experimental and numerical investigation of the hetero-/homogeneous combustion of fuel-rich hydrogen/air mixtures over platinum

The hetero-/homogeneous combustion of hydrogen/air mixtures over platinum was investigated experimentally and numerically in a channel-flow configuration at fuel-rich equivalence ratios ranging from 2 to 7, pressures up to 5 bar and wall temperatures 760–1200 K. Experiments involved in situ one-dimensional Raman measurements of major gas-phase species concentrations over the catalyst boundary layer and planar laser induced fluorescence (LIF) of the OH radical, while simulations included an elliptic 2-D model with detailed heterogeneous and homogeneous reaction mechanisms. The employed reaction schemes reproduced the measured catalytic reactant consumption, the onset of homogeneous ignition, and the post-ignition flame shapes at all examined conditions. Although below a critical pressure, which depended on temperature, the intrinsic gas-phase kinetics of hydrogen dictated lower reactivity for the fuel-rich stoichiometries when compared to fuel-lean ones, homogeneous ignition was still more favorable for the rich stoichiometries due to the lower molecular transport of the deficient oxygen reactant that resulted in modest catalytic reactant consumption over the gaseous induction zone. Above the critical pressure, the intrinsic gaseous hydrogen kinetics yielded higher reactivity for the rich stoichiometries, which resulted in vigorous gaseous combustion at pressures up to 5 bar, in contrast to lean stoichiometry studies whereby homogeneous combustion was altogether suppressed above 3 bar. Computations at fuel-rich stoichiometries in practical channel geometries indicated that homogeneous combustion was not of concern for reactor thermal management, since the larger than unity Lewis number of the deficient oxygen reactant confined the flames to the core of the channel, away from the solid walls.     

Effect of steam on the single particle ignition of solid fuels in a drop tube furnace under air and simulated oxy-fuel conditions

This article investigates the effect of steam on the ignition of single particles of solid fuels in a drop tube furnace under air and simulated oxy-fuel conditions. Three solid fuels, all in the size range 125–150 µm, were used in this study; specifically, a low rank sub-bituminous Colombian coal, a low-rank/high-ash sub-bituminous Brazilian coal and a charcoal residue from black acacia. For each solid fuel, particles were burned at a constant drop tube furnace wall temperature of 1475?K, in six different mixtures of O₂/N₂/CO₂/H₂O, which allowed simulating dry and wet conventional and oxy-fuel combustion conditions. A high-speed camera was used to record the ignition process and the collected images were treated to characterize the ignition mode (either gas-phase or surface mode) and to calculate the ignition delay times. The Colombian coal particles ignite predominately in the gas-phase for all test conditions, but under simulated oxy-fuel conditions there is a decrease in the occurrence of this ignition mode; the charcoal particles experience surface ignition regardless of the test condition; and the Brazilian coal particles ignite predominately in the gas-phase when combustion occurs in mixtures of O₂/N₂/H₂O, but under simulated oxy-fuel conditions the ignition occurs predominantly on the surface. The ignition delay times for particles that ignited in the gas-phase are smaller than those that ignited on the surface, and generally the simulated oxy-fuel conditions retard the onset of both gas-phase and surface ignition. The addition of steam decreases the gas-phase and surface ignition delay times of the particles of both coals under simulated oxy-fuel conditions, but has a small impact on the gas-phase ignition delay times when the combustion occurs in mixtures of O₂/N₂/H₂O. The steam gasification reaction is likely to be responsible for the steam effect on the ignition delay times through the production of highly flammable species that promote the onset of ignition.     

Autoignition of varied cetane number fuels at low temperatures

The reactivity of six kerosene based control fuels, specifically formulated for cetane number variation, are investigated by measuring ignition delay time in a heated rapid compression machine. Cetane numbers vary from 30 to 55 (increment of 5) while holding other properties relatively constant by adjusting chemical group composition. Main cetane variation was controlled through the distribution of normal alkanes and isoalkanes, which was fine-tuned using additives. Other fuel properties such as density, viscosity, H/C ratio, etc. were balanced using cyclic compounds and aromatics. Fuels were tested in the RCM at compressed pressures of P_c=?10 and 20?bar, equivalence ratios of ??=?0.25, 0.5 and 1.0, in the low to intermediate temperature range (620?K?≤?T_c?≤?730?K). Relations between cetane number and ignition delay time have been evaluated at multiple test conditions, and further analysis on multistage ignition has been conducted. Ignition delay times of fuels with higher cetane numbers are shorter at these temperatures for most conditions. First stage ignition delay time measurements have been observed to be relatively insensitive to P_c, ?, and fuel type, while deviations in overall ignition delay times are mainly attributed to second stage ignition delay time, impacted by variations in the first stage temperature. Control fuels of this type offer an opportunity to be used in practical experiments to determine the impact of cetane number on combustion dynamics.     

Ignition enhancement by addition of NO and NO2 from a N2/O2 plasma torch in a supersonic flow

The effects of NO and NO₂ produced by using a plasma jet (PJ) of a N₂/O₂ mixture on ignition of hydrogen, methane, and ethylene in a supersonic airflow were experimentally and numerically investigated. Numerical analysis of ignition delay time showed that the addition of a small amount of NO or NO₂ drastically reduced ignition delay times of hydrogen and hydrocarbon fuels at a relatively low initial temperature. In particular, NO and NO₂ were more effective than O radicals for ignition of a CH₄/air mixture at 1200 K or lower. These ignition enhancement effects were examined by including the low temperature chemistry. Ignition tests by a N₂/O₂ PJ in a supersonic flow (M = 1.7) for using hydrogen, methane, and ethylene injected downstream of the PJ were conducted. The results showed that the ignitability of the N₂/O₂ PJ is affected by the composition of the feedstock and that pure O₂ is not the optimum condition for downstream fuel injection. This result of ignition tests with downstream fuel injection demonstrated a significant difference in ignition characteristics of the PJ from the ignition tests with upstream fuel injection.     

Effects of cryogenic temperature on premixed hydrogen/air flame propagation in a closed channel

As a carbon-free fuel, hydrogen has received significant attention recently since it can help enable low-carbon-economy. Hydrogen has very broad flammability range and very low minimum ignition energy, and thereby there are severe safety concerns for hydrogen transportation and utilization. Cryo-compressed hydrogen is popularly used in practice. Therefore, it is necessary to investigate the combustion properties of hydrogen at extremely low or cryogenic temperatures. This study aims to assess and interpret the effects of cryogenic temperature on premixed hydrogen/air flame propagation and acceleration in a thin closed channel. Different initial temperatures ranging from normal temperature (T₀ = 300 K) to cryogenic temperature (T₀ = 100 K) are considered. Both one- and two-dimensional hydrogen/air flames are investigated through transient simulations considering detailed chemistry and transport. It is found that when the initial temperature decreases from T₀ = 300 K to T₀ = 100 K, the expansion ratio and equilibrium pressure both increase substantially while the laminar flame speeds relative to unburned and burned gasses decrease moderately. The one-dimensional flame propagation is determined by laminar flame speed and thereby the combustion duration increases as the initial temperature decreases. However, the opposite trend is found to happen to two-dimensional flame propagation, which is mainly controlled by the flame surface area increase due to the no-slip side wall constraint and flame instability. Based on the change in flame surface area, three stages including the initial acceleration, steady burning and rapid acceleration are identified and investigated. It is demonstrated that the large expansion ratio and high pressure rise at cryogenic temperatures can significantly increase the flame surface area in early stage and promote both Darrieus-Landau instability (hydrodynamic instability) and Rayleigh-Taylor instability in later stage. These two instabilities can substantially increase the flame surface area and thereby accelerate flame propagation in hydrogen/air mixtures at cryogenic temperatures. The present study provides useful insights into the fundamental physics of hydrogen flames at extremely low temperatures, and is closely related to hydrogen safety.     

Shock tube measurements of ignition delay times and OH time-histories in dimethyl ether oxidation

Ignition delay times and OH concentration time-histories were measured in DME/O₂/Ar mixtures behind reflected shock waves. Initial reflected shock conditions covered temperatures (T₅) from 1175 to 1900 K, pressures (P₅) from 1.6 to 6.6 bar, and equivalence ratios (?) from 0.5 to 3.0. Ignition delay times were measured by collecting OH^∗ emission near 307 nm, while OH time-histories were measured using laser absorption of the R₁(5) line of the A-X(0,0) transition at 306.7 nm. The ignition delay times extended the available experimental database of DME to a greater range of equivalence ratios and pressures. Measured ignition delay times were compared to simulations based on DME oxidation mechanisms by Fischer et al. [7] and Zhao et al. [9]. Both mechanisms predict the magnitude of ignition delay times well. OH time-histories were also compared to simulations based on both mechanisms. Despite predicting ignition delay times well, neither mechanism agrees with the measured OH time-histories. OH Sensitivity analysis was applied and the reactions DME ↔ CH₃O + CH₃ and H + O₂ ↔ OH + O were found to be most important. Previous measurements of DME ↔ CH₃O + CH₃ are not available above 1220 K, so the rate was directly measured in this work using the OH diagnostic. The rate expression k[1/s] =  1.61 × 10⁷⁹T^−18.4 exp(−58600/T), valid at pressures near 1.5 bar, was inferred based on previous pyrolysis measurements and the current study. This rate accurately describes a broad range of experimental work at temperatures from 680 to 1750 K, but is most accurate near the temperature range of the study, 1350-1750 K. When this rate is used in both the Fischer et al. and Zhao et al. mechanisms, agreement between measured OH and the model predictions is significantly improved at all temperatures.     

RANS predictions of turbulent diffusion flames: comparison of a reactor and a flamelet combustion model to the well stirred approach

The flame stabilisation process in turbulent non-premixed flames is not fully understood and several models have been developed to describe the turbulence–chemistry interaction. This work compares the performance of the multiple Representative Interactive Flamelet (mRIF) model, the Volume Reactor Fraction Model (VRFM), and the Well-Stirred reactor (WS) model in describing such flames. The predicted ignition delay and flame lift-off length of n-heptane sprays are compared to experimental results published within the Engine Combustion Network (ECN). All of the models predict the trend of ignition delay reasonably well. At a low gas pressure (42 bar) the ignition delay is overpredicted compared to the experimental data, but the difference between the models is not significant. However, the predicted lift-off lengths differ. At high pressure (87 bar) the difference between the models is small. All models slightly underpredict the lift-off length compared to the experimental data. At low gas pressure (42 bar) the mRIF model gives the best results. The VRFM and WS models predict excessively short lift-off lengths, but the VRFM model gives better results than the WS model. The flame structures of the models are also compared. The WS model and the VRFM model yield a well defined flame stabilisation point whereas the mRIF model does not. The flame of the mRIF model is more diffuse and the model is not able to predict flame propagation. All models were able to predict the experimental trends in lift-off and ignition delay, but certain differences between them are demonstrated.     

A comprehensive experimental and improved kinetic modeling study on the pyrolysis and oxidation of propyne

To improve our understanding of the combustion characteristics of propyne, new experimental data for ignition delay times (IDTs), pyrolysis speciation profiles and flame speed measurements are presented in this study. IDTs for propyne ignition were obtained at equivalence ratios of 0.5, 1.0, and 2.0 in ‘air’ at pressures of 10 and 30 bar, over a wide range of temperatures (690–1460 K) using a rapid compression machine and a high-pressure shock tube. Moreover, experiments were performed in a single-pulse shock tube to study propyne pyrolysis at 2 bar pressure and in the temperature range 1000–1600 K. In addition, laminar flame speeds of propyne were studied at an unburned gas temperature of 373 K and at 1 and 2 bar for a range of equivalence ratios. A detailed chemical kinetic model is provided to describe the pyrolytic and combustion characteristics of propyne across this wide-ranging set of experimental data. This new mechanism shows significant improvements in the predictions for the IDTs, fuel pyrolysis and flame speeds for propyne compared to AramcoMech3.0. The improvement in fuel reactivity predictions in the new mechanism is due to the inclusion of the propyne + H?₂ reaction system along with ?H radical addition to the triple bonds of propyne and subsequent reactions.