Mechanism of spontaneous ignition of high-pressure hydrogen during its release through a tube with local contraction: A numerical study

The tendency of spontaneous ignition of high-pressure hydrogen during its sudden release into a tube is one of the main threats to the safe application of hydrogen energy. A series of investigations have shown that the tube structure is a key factor affecting the spontaneous ignition of high-pressure hydrogen. In this paper, a numerical study is conducted to reveal the mechanism of spontaneous ignition of high-pressure hydrogen inside the tube with local contraction. Large Eddy Simulation, Renormalization Group, Eddy Dissipation Concept, 37-step detailed hydrogen combustion mechanism and 10-step like opening process of burst disk are employed. Three cases with burst pressures of 3.10, 4.90, and 8.45 MPa are simulated to compare against the pervious experimental study. The spontaneous conditions and positions agree well with the experimental results. The numerical results indicate that shock wave reflection takes place at the upstream vertical wall of contraction part. The interacted-shock-affected region is generated at the tube center because of the subsequent shock wave interaction. The forward reflected shock wave couples with normal shock wave and increases the pressure of leading shock wave. The sudden contraction of tube blocks the propagation of hydrogen jet and decreases the speed from supersonic flow to subsonic flow. More flammable mixture is generated inside the contraction part, as a results, the length of the flame is increased. Two mechanisms are proposed finally.     

Experimental study of spontaneous ignition induced by sudden hydrogen release through tubes with different shaped cross-sections

The shock wave dynamics, spontaneous ignition and flame variation during high-pressure hydrogen release through tubes with different cross-section shapes are experimentally studied. Tubes with square, pentagon and circular cross-section shapes are considered in the experiments. The experimental results show that the cross-section shape of the tube has no great difference on the minimum burst pressure for spontaneous ignition in our tests. In the three tubes with length of 300 mm, spontaneous ignition may occur when overpressure of shock wave is 0.9 MPa. When the spontaneous ignition is induced in a non-circular cross-section tube, the possible turbulent flow in the corner of the tube increases can promote the mixing of hydrogen and air, thus producing more amount of the hydrogen/air mixture. As a result, both the peak light signal and flame duration detected in the non-circular cross-section tubes are more intense than those in the circular tube. The smaller angle of the corner leads to a more intensity flame inside tube. When the hydrogen flame propagates to the tube exit from the circular tube, the ball-like flame developed near tube exit is relatively weak. In addition, second flame separation outside the tube is observed for the cases of non-circular cross-section tubes.     

Spontaneous ignition of high-pressure hydrogen during its sudden release into hydrogen/air mixtures

This paper investigates the effects of hydrogen additions on spontaneous ignition of high-pressure hydrogen released into hydrogen-air mixture. Hydrogen and air are premixed with different volume concentrations (0%, 5%, 10%, 15% and 20% H₂) in the tube before high-pressure hydrogen is suddenly released. Pressure transducers are employed to detect the shock waves, estimate the mean shock wave speed and record the shock wave overpressure. Light sensors are used to determine the occurrence of high-pressure hydrogen spontaneous ignition in the tube. A high-speed camera is used to capture the flame propagation behavior outside the tube. It is found that only 5% hydrogen addition could decrease the minimum storage pressure required for spontaneous ignition from 4.37 MPa to 2.78 MPa significantly. When 10% or 15% hydrogen is added to the air, the minimum storage pressure decreases to 2.81 MPa and 1.85 MPa, respectively. When hydrogen addition increases to 20%, the spontaneous ignition even takes place at burst pressure as low as 1.79 MPa inside the straight tube.     

Visualization of spontaneous ignition under controlled burst pressure

A high-pressure hydrogen jet released into the air has the possibility of igniting in a tube without any ignition source. The mechanism of this phenomenon, called spontaneous ignition, is considered to be that hydrogen diffuses into the hot air caused by the shock wave from diaphragm rupture and the hydrogen-oxidizer mixed region is formed enough to start chemical reaction. Recently, flow visualization studies on the spontaneous ignition process have been conducted to understand its detailed mechanism, but such ignition has not yet been well clarified. In this study, the spontaneous ignition phenomenon was observed in a rectangular tube. The results confirm the presence of a flame at the wall of the tube when the shock wave pressure reaches 1.2–1.5 MPa in more than 9 MPa burst pressure and that ignition occurs near the wall, followed by multiple ignitions as the shock wave propagates, with the ignitions eventually combining to form a flame.     

Experimental investigation of shock wave propagation,spontaneous ignition,and flame development of high-pressure hydrogen release through tubes with different obstacles arrangements

Experiments on shock waves propagation, spontaneous ignition, and flame development during high-pressure hydrogen release through tubes with symmetrical obstacles (O_1-1) and asymmetrical obstacles (O_1-2) are conducted. The obstacle's side is triangular with a length of 4 mm, a height of 3.6 mm, and its width is 15 mm. In the experiments, a reflected shock wave generates and propagates both upstream and downstream when the leading shock wave encounters the obstacle. At the same burst pressure, the reflected shock wave intensity in tube O_1-1 is significantly greater than that in tube O_1-2. Moreover, the presence of obstacles in the tube can induce spontaneous ignition. The minimum burst pressures for spontaneous ignition for tubes O_1-1 and O_1-2 are 2.84 MPa and 3.28 MPa respectively, lower than that for the smooth tube. Furthermore, both the initial ignition position and ignition time are greatly advanced in obstruction tubes, mainly affected by obstacle positions and burst pressures. Finally, the flame separation process near the obstacle is observed. After passing the obstacle, the flames grow rapidly in radial and axial directions on the tube sidewalls. And at the same burst pressure, the flame convergence time in tube O_1-2 is usually longer than that in tube O_1-1.     

Experimental investigation on effects of CO2 additions on spontaneous ignition of high-pressure hydrogen during its sudden release into a tube

Hydrogen is expected to be an alternative energy carrier in the future. High-pressure hydrogen storage option is considered as the best choice. However, spontaneous ignition tends to occur if hydrogen is suddenly released from a high-pressure tank into a tube. In order to improve the safety of hydrogen application, an experimental investigation on effects of CO₂ additions (5%, 10% and 15% volume concentration) on the spontaneous ignition of high-pressure hydrogen during its sudden expansion inside the tube has been conducted. Pressure transducers are used to record the pressure variation and light sensors are employed to detect the possible spontaneous ignition. It is found that the shock wave overpressure and the mean shock wave speed are almost the same inside the tube for different CO₂ additions under the close burst pressures. For cases with more CO₂ additions, the ignition detected time is longer and the average speed of the flame, the maximum value of light signals and the detected duration time of spontaneous ignition are smaller. It is shown that minimum burst pressure required for spontaneous ignition increase 1.47 times for 15% CO₂ additions. The minimum burst pressure required for spontaneous ignition increases from 4.37 MPa (0% CO₂) up to 6.41 MPa (15% CO₂). With the increasing of CO₂ additions, it requires longer distance and longer time for hydrogen and oxygen to mix and thus longer ignition delay distance/time. The results showed that additions of CO₂ to air have a good suppressing effect on hydrogen spontaneous ignition.     

Experimental study on spontaneous ignition and flame propagation of high-pressure hydrogen release through tubes

An experimental study was conducted to research the mechanism of spontaneous ignition induced by high-pressure hydrogen release through tubes with a diameter of 10 mm and varying lengths from 0.3 to 3 m. The pressure and light signals inside the tube were collected. The propagation of shock wave inside and outside the tube was also systematically investigated. The development process of the jet flame in the atmosphere was completely recorded, and the multiple Mach disks at the tube exit were observed by using a high-speed camera. The results show that the minimum release pressure, at which the jet flame is formed, is found to be 3.87 MPa with the tube length of 1.7 m. When the tube length was longer than 1.7 m, the critical pressure for forming jet flame increased rapidly. The velocity attenuation of the shock wave is mainly affected by the burst pressure but not sensitive to the tube length, and the flame propagates in the tube at a slower velocity than the shock wave. The compression of the hydrogen-air mixture by the Mach disk causes it to burn more violently after passing through the Mach disk. It is confirmed that the flame at the tube exit is lifted in the atmosphere, then a jet flame initiates behind the second Mach disk.     

Experimental study of shock wave propagation and its influence on the spontaneous ignition during high-pressure hydrogen release through a tube

An experimental study of shock wave propagation and its influence on the spontaneous ignition during high-pressure hydrogen release through a tube are measured by pressure transducers and light sensors. Results show that the pressure behind a shock wave first increases, and subsequently remains near constant value with an increase of the propagation distance. That is, a certain propagation distance is required to form a stable shock wave in the tube. In the front of the tube, the minimum value of pressure behind the shock wave (P_shock) required for spontaneous ignition decreases with the increase in axial distance to the diaphragm. However, the minimum P_shock remains nearly a constant value in the rear part of the tube. Moreover, the critical values of shock Mach number (M_S) for spontaneous ignition decrease with the increase in tube length. And the ignition delay time decreases with the increase of the M_S. As the ignition kernel grows in size to a flame, it propagates downstream along the tube with velocity greater than the theoretical flow velocity of the hydrogen-air contact surface. The flame propagation velocity relative to tube wall increases with M_S. When the self-sustained flame exits from the tube, a rapid non-premixed turbulent combustion is observed in the chamber. The combustion-wave overpressure increases with the increase of the M_S.     

基于扩散点火理论的高压氢气泄漏自燃研究

运用扩散点火理论对高压氢气泄漏到下游管道内的自燃点火情况进行了分析。利用激波管流动理论讨论了氢气射流前端激波加热区域的参数变化情况,分析了前沿激波强度、均匀区压力和温度与初始压力的关系,给出了高压氢气泄漏到下游管道后,预测前沿激波强度、均匀区压力和温度的数学方程,建立了判断高压氢气泄漏到下游管道内是否发生自燃点火的函数表达式。提出了理论点火临界压力的概念,计算发现氢气的理论点火临界压力明显低于其他几种常见的气体燃料。讨论了影响泄漏自燃发生的可能因素,结果可为预防高压储氢泄漏自燃提供科学依据。     

Effects of the geometry of downstream pipes with different angles on the shock ignition of high-pressure hydrogen during its sudden expansion

To investigate the effects of the geometry of downstream pipes on the shock ignition and the formation of the shock waves during high-pressure hydrogen sudden expansion, a series of bench-mark experiments were designed and high-pressure hydrogen were released into five types of pipes with different angles (60, 90, 120, 150 and 180°). It was found that the geometry of downstream pipes had a significant influence on the shock ignition of hydrogen. The incident shock wave would be reflected at the corner of the pipes with angles of 60, 90, 120 and 150°. The intensity of the reflected shock wave is higher if the angle is smaller. In addition, the average velocity of the leading incident shock wave would decrease when it passed the corner of the pipe. Using a pipe with smaller angle significantly increases the likelihood of shock ignition and lowers the minimal required burst pressure for shock ignition. The overpressure of the incident shock waves inside the exhaust chamber (for the cases with the angles of 60, 90, 120 and 150°) decreases sharply. There are three flame propagation behaviors inside the exhaust chamber: flame quenching, flame separation and no flame separation. The results of this study have implications concerning designs for storage safety of hydrogen energy and may help get better understanding of shock ignition mechanism of high pressure hydrogen and effect of pipeline geometry on ignition.     

Self-ignition and flame propagation of high-pressure hydrogen jet during sudden discharge from a pipe

Hydrogen is expected to serve as a clean energy carrier. However, since there are serious ignition hazards associated with its use, it is necessary to collect data on safety in a range of possible accident scenarios so as to assess hazards and develop mitigation measures. When high-pressure hydrogen is suddenly released into the air, a shock wave is produced, which compresses the air and mixes it with hydrogen at the contact surface. This leads to an increase in the temperature of the hydrogen–air mixture, thereby increasing the possibility of ignition. We investigated the phenomena of ignition and flame propagation during the release of high-pressure hydrogen. When a hydrogen jet flame is produced by self-ignition, the flame is held at the pipe outlet and a hydrogen jet flame is produced. From the experiment using the measurement pipe, the presence of a flame in the pipe is confirmed; further, when the burst pressure increased, the flame may be detected at a position near the diaphragm. At the pipe outlet, the flame is not lifted and self-ignition is initiated at the outer edge of the jet.     

Experiment study on the pressure and flame characteristics induced by high-pressure hydrogen spontaneous ignition

A series of experiments were conducted to study the pressure and combustion characteristics of the high-pressure hydrogen during the occurrence of spontaneous ignition and the conversion from spontaneous ignition to a jet fire and explosion. Different initial conditions including release pressure (4–10 MPa), tube diameter (10/15 mm), and tube length (0.3/0.7/1.2/1.7/2.2/3 m) were tested. The variation of the pressure and flame signal inside and outside of the tube and the development of the jet flame were recorded. The experimental results revealed that the minimum ignition pressure required for self-ignition of hydrogen at different tube diameters decreased first and then increased with the extension of tubes. The minimum ignition pressure for tubes diameters of 10 mm and 15 mm is no more than 4 MPa and the length of the tubes is L = 1.7 m. The minimum release pressure required for spontaneous ignition of a tube D = 15 mm is always lower than that of a tube D = 10 mm at the same tube length. When the spontaneous ignition occurred, it did not absolutely trigger the jet fire. The transition from spontaneous ignition to a jet fire must go through the specific stages.     

Experimental study on pressure dynamics and self-ignition of pressurized hydrogen flowing into the L-shaped tubes

To investigate the effects of varying right-angle corner locations inside the L-shaped tube on self-ignition induced by high-pressure hydrogen release, a series of experiments were carried out on L-shaped tubes with different right-angle corner locations and a straight tube was adopted for comparison. It is found that compared with the straight tube, the propagation of shock wave in the L-shaped tubes becomes more complicated due to the existence of reflected shock wave. The pressure profiles detected by pressure transducers before the right-angle corner will undergo secondary rapid rise. The varying right-angle corner locations inside the L-shaped tube have a significant influence on self-ignition of hydrogen. The closer the right-angle corner is to the burst disk, the lower the critical pressure that causes hydrogen self-ignition is. Three possible mechanisms of self-ignition inside the L-shaped tubes are discussed. Nevertheless, different right-angle corner locations have no obvious effects on development process of out-tube jet flame, only the velocity of flame tip and the length and width of jet flame have slight differences.     

Numerical simulation of the effect of multiple obstacles inside the tube on the spontaneous ignition of high-pressure hydrogen release

Self-ignition may occur during hydrogen storage and transportation if high-pressure hydrogen is suddenly released into the downstream pipelines, and the presence of obstacles inside the pipeline may affect the ignition mechanism of high-pressure hydrogen. In this work, the effects of multiple obstacles inside the tube on the shock wave propagation and self-ignition during high-pressure hydrogen release are investigated by numerical simulation. The RNG k-ε turbulence model, EDC combustion model, and 19-step detailed hydrogen combustion mechanism are employed. After verifying the reliability of the model with experimental data, the self-ignition process of high-pressure hydrogen release into tubes with obstacles with different locations, spacings, shapes, and blockage ratios is numerically investigated. The results show that obstacles with different locations, spacings, shapes and blockage ratios will generate reflected shock waves with different sizes and propagation trends. The closer the location of obstacles to the burst disk, the smaller the spacing, and the larger the blockage ratio will cause the greater the pressure of the reflected shock wave it produces. Compared with the tubes with rectangular-shaped, semi-circular-shaped and triangular-shaped obstacles, self-ignition is preferred to occur in tube with triangular-shaped obstacles.     

Physics of spontaneous ignition of high-pressure hydrogen release and transition to jet fire

The aim of this study is to gain an insight into the physical phenomena underlying the spontaneous ignition of hydrogen following a sudden release from high-pressure storage and transition to sustained jet fire. The modelling and large-eddy simulation (LES) of the spontaneous ignition dynamics in a tube with a non-inertial rupture disk separating the high-pressure hydrogen storage and the atmosphere is described. Numerical experiments confirmed that due to the stagnation conditions a chemical reaction first commences in the tube boundary layer, and subsequently propagates throughout the tube cross-section. The dynamics of flame formation outside the tube, simulated by the LES model, has reproduced the combustion patterns, including vortex induced “flame separation”, which have been experimentally observed by high-speed photography. It is concluded that the LES model can be applied for hydrogen safety engineering, e.g. for the development of innovative pressure relief devices.     

Experimental and numerical investigation of hydrogen gas auto-ignition

This paper describes hydrogen self-ignition as a result of the formation of a shock wave in front of a high-pressure hydrogen gas propagating in the tube and in the semi-confined space, for which the numerical and experimental investigation was done. An increase in the temperature behind the shock wave leads to the ignition on the contact surface of the mixture of combustible gas with air. The required condition of combustible self-ignition is to maintain the high temperature in the mixture for a time long enough for inflammation to take place. Experimental technique was based on a high-pressure chamber inflating with hydrogen, burst disk failure and pressurized hydrogen discharge into tube of round or rectangular cross section filled with air. Two numerical models involving the gas-dynamic transport of a viscous gas, the detailed kinetics of hydrogen oxidation, turbulence model, and heat exchange were used for calculations of the hydrogen self-ignition both in semi-confined space and a tube.     

Numerical study on spontaneous ignition of pressurized hydrogen release through a length of tube

The issue of spontaneous ignition of highly pressurized hydrogen release is of important safety concern, e.g. in the assessment of risk and design of safety measures. This paper reports on recent numerical investigation of this phenomenon through releases via a length of tube. This mimics a potential accidental scenario involving release through instrument line. The implicit large eddy simulation (ILES) approach was used with the 5th-order weighted essentially non-oscillatory (WENO) scheme. A mixture-averaged multi-component approach was used for accurate calculation of molecular transport. The thin flame was resolved with fine grid resolution and the autoignition and combustion chemistry were accounted for using a 21-step kinetic scheme.The numerical study revealed that the finite rupture process of the initial pressure boundary plays an important role in the spontaneous ignition. The rupture process induces significant turbulent mixing at the contact region via shock reflections and interactions. The predicted leading shock velocity inside the tube increases during the early stages of the release and then stabilizes at a nearly constant value which is higher than that predicted by one-dimensional analysis. The air behind the leading shock is shock-heated and mixes with the released hydrogen in the contact region. Ignition is firstly initiated inside the tube and then a partially premixed flame is developed. Significant amount of shock-heated air and well developed partially premixed flames are two major factors providing potential energy to overcome the strong under-expansion and flow divergence following spouting from the tube.Parametric studies were also conducted to investigate the effect of rupture time, release pressure, tube length and diameter on the likelihood of spontaneous ignition. It was found that a slower rupture time and a lower release pressure will lead to increases in ignition delay time and hence reduces the likelihood of spontaneous ignition. If the tube length is smaller than a certain value, even though ignition could take place inside the tube, the flame is unlikely to be sufficiently strong to overcome under-expansion and flow divergence after spouting from the tube and hence is likely to be quenched.     

Experimental study on explosion characteristics of syngas with different ignition positions and hydrogen fraction

The influence of different ignition positions and hydrogen volume fractions on the explosion characteristics of syngas is studied in a rectangular half-open tube. Three ignition positions were set at the axis of the tube, which are 0 mm, 600 mm and 1100 mm away from the closed end, respectively. A range of hydrogen volume fraction (φ) from 10% to 90% were concerned. Experimental results show that different ignition positions and hydrogen volume fraction have important influence on flame propagation structure. When ignited at 600 mm from the closed end on the tube axis, distorted tulip flame forms when flame propagates to the closed end. The formations of the tulip flame and the distorted tulip flame are accompanied by a change in the direction of the flame front propagation. The flame propagation structure and pressure are largely affected by the ignition position and the hydrogen volume fraction. At the same ignition position, flame propagation speed increases with the growing of hydrogen volume fraction. And the pressure oscillates more severe as the ignition location is closer to the open end. And pressure oscillations bring two different forms. The first form is that the pressure has a periodic oscillation. The amplitude of the pressure oscillation gradually increases. It takes several cycles from the start of the oscillation to the peak. For the second form, the pressure reaches the peak of the oscillation in the first cycle of the start to the oscillation.     

An experimental study of the effect of 2.5% methane addition on self-ignition and flame propagation during high-pressure hydrogen release through a tube

This paper demonstrates experimental investigation on the self-ignition and subsequent flame propagation of high-pressure hydrogen-methane mixture release via a tube. The proportion of methane added to hydrogen is 2.5% (vol.). A transparent rectangular tube (d = 15 mm, L = 400 mm) is used in the experiments. It is shown that the minimum burst pressure required for self-ignition increases 1.57 times for only 2.5% methane addition from 2.89 MPa (pure hydrogen) up to 4.68 MPa (2.5% CH₄ addition). This is mainly caused by the following reasons: on the one hand, methane addition can result in the decease of shock intensity inside the tube, thereby lowering the temperature of the combustible mixture; on the other hand, the hydrogen-methane mixture has the higher minimum ignition energy than that of pure hydrogen. Besides, 2.5% methane addition can increase the initial ignition time, weaken the flame intensity and reduce the flame propagation velocity relative to tube wall inside the tube. Moreover, for cases with 2.5% methane addition, the complete flame throughout the tube is formed closer to the back end of the tube. When the self-sustained flame exits from the tube, the maximum overpressure in a confined space increases with 2.5% methane addition.     

A pressure-ratio equivalent method for ultra-high pressure hydrogen spontaneous ignition experiment

Increasing hydrogen storage pressure brings high economic benefits and high risks. Pressurized hydrogen leakage spontaneous ignition experiment is an important means to reveal the mechanism of hydrogen leakage spontaneous ignition and improve the safety of hydrogen storage equipment. However, due to the extremely high cost and danger of ultra-high pressure, there is a serious lack of experimental data. In this paper, a pressure-ratio equivalent (PRE) method of experiments is proposed based on the theory of the shock tube problem. By keeping the hydrogen-air pressure ratio constant while reducing the absolute pressure of air and hydrogen, the difficulty of the experiment is greatly reduced. The effectiveness of the PRE method is evaluated theoretically and experimentally. The results show the PRE method retains the ignition characteristics of hydrogen leakage spontaneous ignition largely when the air pressure is within 0.05–0.1 MPa. It is found the pressure ratio of hydrogen to air dominates the leakage spontaneous ignition process. In the experiments of different air pressures, the shock Mach numbers are close to theoretical values. In addition, leakage spontaneous ignition of hydrogen mixed with 30% (vol.) CO is found in experiments using the PRE method, with pressure ratios of up to 250. This indicates that when the storage pressure is high enough, there is also a risk of spontaneous ignition of syngas from high-pressure leakage. The PRE method can widely broaden the pressure scope of experimental research on leakage spontaneous ignition, and it provides a new idea for obtaining the experimental data of gas high-pressure leakage spontaneous ignition.