在以传统化石能源为主体到纯H₂大规模应用的过渡阶段，H₂/CH₄混合气体作为氢能的重要载体，是氢能应用体系的重要组成部分。在H₂中添加少量CH₄可一定程度上降低H₂的高压泄放自燃倾向性，进而推动氢能大规模安全应用。为此，开展了多工况下高压H₂/CH₄混合气体泄放自燃实验，研究了其泄放激波及自燃特性，结合三维CFD数值模拟和化学动力学分析，揭示了激波诱导点火作用机制和自燃化学动力学机理。主要研究成果如下：

在高压H₂/CH₄混合气体泄放激波特性方面，基于自主搭建的高压可燃气体泄放自燃实验平台，研究了不同工况下高压H₂/CH₄混合气体泄放的激波传播特征。由于圆形破口和矩形泄放管道之间的形状突变，爆破片破裂后首先在管道角落发生激波反射，最终在泄放管道内形成复杂的多维反射激波。随着泄放压力的增大，激波压力和激波传播速度显著增大。在同等泄放压力水平时，随着掺CH₄比例的增大，激波压力和激波传播速度明显减小。基于激波管流动理论，构建了高压H₂/CH₄混合气体泄放激波特性参数计算模型。通过对比分析计算结果与文献数据和本文实验数据，证实了所构建的激波特性参数计算模型具有较强的适用性。

在高压H₂/CH₄混合气体泄放自燃特性方面，高压H₂/CH₄混合气体泄放到管道时，管道内可能出现多次自燃和火焰淬灭现象。当泄放压力超过自燃临界泄放压力，泄放管道内自燃火焰可稳定燃烧并传播至管道外部。随着掺CH₄比例的增大，H₂/CH₄混合气体自燃临界泄放压力增大，自燃火焰淬灭概率也更大。将H₂/CH₄混合气体中的CH₄替换为N₂或提高储气温度对激波特性参数及自燃临界泄放压力无明显影响。基于实验数据，建立了H₂/CH₄比例、泄放压力与激波强度间的量化关系，提出了高压H₂/CH₄混合气体泄放自燃判别方法。当管道内未发生自燃时，管道内10 cm处测点压力（P₂）大于20 cm处测点压力（P₃）。当泄放压力远大于自燃临界压力时，管道内发生自燃，并在P₃附近发展为剧烈燃烧，进而增大了P₃处的激波压力，体现为P₃>P₂。当泄放压力略高于自燃临界泄放压力时，P₂、P₃处的压力大小关系取决于掺CH₄比例。

对于高压H₂/CH₄混合气体泄放自燃的空气动力学机理，基于CFD软件GASFLOW-MPI，建立了高压H₂/CH₄混合气体泄放自燃三维CFD数值模型。基于该数值模型，研究了泄放过程中流场演化规律、燃料/空气混合以及自燃行为特征，揭示了管道内三次典型自燃的激波诱导点火机制。管道角落和管壁中心的反射激波交汇以及马赫反射加热了燃料/空气混合物，导致在管道角落、管壁中心以及管道中心分别发生第一次、第二次和第三次自燃。将掺混气体CH₄替换为N₂后，对反应初期的能量释放速率无明显影响，但降低了稳定燃烧阶段的能量释放速率。当泄放压力以及H₂占比均足够大时，半球形激波直接引发半球形火焰，以及第二次和第三次自燃火焰迅速蔓延至整个燃料/空气混合层的燃烧行为，均造成能量释放速率的激增。由于自燃反应初期的初始温度主要来源于激波的加热作用，因此，储气温度的改变对反应初期的能量释放速率无明显影响。但在稳定燃烧阶段，储气温度的改变直接影响参与反应的燃料温度，进而对能量释放速率产生显著的影响。CFD模拟中不同初始工况下能量释放规律与高压H₂/CH₄混合气体泄放自燃行为的实验结果相互印证。

对于高压H₂/CH₄混合气体泄放自燃的化学动力学机理，利用CHEMKIN-2022对高压H₂/CH₄混合气体泄放自燃反应进行了化学动力学分析。在高压H₂/CH₄混合气体泄放过程中，所发生的三次自燃反应在引发阶段的主要反应路径相似，均以H₂的氧化反应为主。自燃反应的点火延迟时间主要由H₂氧化反应控制，掺混气体的化学反应性质、掺混比例、当量比等燃料组成情况对点火延迟时间的影响程度有限，但反应初始温度对点火延迟时间的影响极为显著。初始温度较高时，大量H₂直接一步氧化生成 OH，造成点火延迟时间呈指数式降低。当泄放压力较大时，激波对燃料/空气混合区的增压升温效能提高，使H₂/CH₄混合气体自燃时点火延迟时间缩短，自燃概率增大。以更高的初始温度和初始压力引发的自燃反应 OH峰值浓度更高，自燃火焰更容易维持。宏观上表现为随着泄放压力的增高或掺CH₄比例的减小，高压H₂/CH₄混合气体泄放自燃概率越大，越容易发展为稳定的燃烧火焰向下游传播。

The transition from conventional fossil fuels to large-scale hydrogen utilization emphasizes the importance of the H₂/CH₄ mixture as a critical energy carrier. And adding a amount of CH₄ to H₂ can reduce the propensity of H₂ spontaneous ignition during it high-pressure discharge, and thus promote the large-scale safe application of hydrogen energy. Therefore, this study investigates the characteristics of flow field and spontaneous ignition during high-pressure H₂/CH₄ mixture discharge, integrating experimental approaches with three-dimensional Computational Fluid Dynamics (CFD) simulations and chemical kinetics analysis to elucidate the underlying mechanisms of shock-induced ignition and the kinetics of ignition reactions.

Firstly, the propagation characteristics of shock waves during the high-pressure H₂/CH₄ mixture discharge were studied on self-improved experimental platform. Observations indicated that intense reflected shock waves were initially generated at the transition from a circular rupture disc to a rectangular discharge tube, leading to complex multidimensional wave patterns inside the tube. With the increase in burst pressure, both shock wave pressure and propagation velocity increase significantly. At the same burst pressure level, as the CH₄ concentration increases, both shock wave pressure and propagation velocity decrease noticeably. Based on shock tube flow theory, a model for calculating the shock wave characteristics of high-pressure H₂/CH₄ mixture discharge was developed. Comparative analysis between calculated results and published literature data as well as experimental data in this study confirms the high applicability for calculating shock wave characteristic parameters.

For the spontaneous ignition characteristics during high-pressure H₂/CH₄ gas mixtures discharge. when high-pressure H₂/CH₄ mixture leaks into the rectangular tube, multiple occurrences of spontaneous ignition and flame quenching phenomena may happen inside the rectangular tube. When the burst pressure is sufficiently high, the spontaneous ignition flame can stably combust and propagate to the exterior of the tube. With the increase of the CH₄ concentration, the critical burst pressure for spontaneous ignition increases, and the possibility of flame quenching is higher. Replacing CH₄ in the H₂/CH₄ mixture with N₂ or increasing the storage temperature does not cause significant changes in the shock wave characteristics or the critical burst pressure for spontaneous ignition. Based on experimental data, a quantitative relationship between H₂/CH₄ ratio, burst pressure, and shock wave intensity is established, and a method for discriminating the spontaneous ignition during high-pressure H₂/CH₄ mixture discharge was proposed. When spontaneous ignition does not occur inside the tube, the pressure of the measurement point at 10 cm of the tube(P₂) is higher than that of the 20 cm of the tube (P₃). When the burst pressure greatly exceeds the critical burst pressure for spontaneous ignition, spontaneous ignition occurs inside the tube, leading to intense combustion near P₃, thereby increasing the shock wave pressure at P₃, which is reflected as P₃>P₂. When the burst pressure is slightly higher than the critical burst pressure for spontaneous ignition, the pressure relationship at P₂ and P₃ depends on the CH₄ concentration.

For the aerodynamic mechanism of spontaneous ignition during high-pressure H₂/CH₄ mixture discharge. Utilizing CFD software GASFLOW-MPI, a three-dimensional CFD simulation model for spontaneous ignition during high-pressure H₂/CH₄ mixture discharge was developed. Using the simulation model, characteristics such as the evolution of the flow field, fuel/air mixing, and spontaneous ignition behaviors during the discharge process were obtained, and the mechanisms of shock-induced ignition for the typical spontaneous ignition that may occur inside the tube was revealed. The intersection of reflected shock waves at tube corners and tube wall centers, along with Mach reflection, heats the fuel/air mixture, leading to the 1st, 2nd, and 3rd spontaneous ignition at tube corners, tube wall centers, and tube center, respectively. Replacing CH₄ in the H₂/CH₄ mixture with N₂ has no significant effect on the energy release rate during the initial phase of the reaction but reduces the energy release rate during the stable combustion phase. When the burst pressure and the H₂ concentration is high enough, the combustion behavior of a hemispherical flame triggered by hemispherical shock wave and the 2nd and 3rd spontaneous ignition flames propagate throughout the entire fuel-air mixture layer rapidly, causing a significant increase in energy release rate. Since the initial temperature of spontaneous ignition reaction primarily comes from the heating effect of shock waves, changes in storage temperature have no significant effect on the energy release rate of the initial reaction. However, during the stable combustion phase, changes in storage temperature directly affect the temperature of the fuel participating in the reaction, thereby significantly influencing the energy release rate. The energy release patterns under different initial conditions obtained by CFD simulation are corroborated with experimental results on the combustion behavior during high-pressure H₂/CH₄ gas mixtures discharge.

Lastly, using CHEMKIN-2022, a reaction kinetics analysis of the initiation stage of the spontaneous ignition reaction was conducted. This analysis underscored that the initiation reaction phase of the spontaneous ignition inside the tube predominantly follows H₂ oxidation pathways. The ignition delay time is mainly controlled by the oxidation reaction of H₂, and the effect of the chemical reactivity of mixture, blending gas ratio, equivalence ratio, and other fuel composition conditions on the ignition delay time is limited. However, the initial temperature of the spontaneous ignition reaction has a significant impact on the ignition delay time. When the initial temperature is high, H₂ directly oxidizes to produce OH, resulting in an exponential decrease in the ignition delay time. When the burst pressure is high, the ability of shock waves to increase pressure and temperature in the mixing zone is enhanced, leading to a decrease in the ignition delay time of the ignition reaction and a significant increase in spontaneous ignition probability. Spontaneous ignition reactions initiated with higher temperature and pressure result in higher peak concentrations of OH, making it easier to sustain the flames. On a macroscopic level, as the burst pressure increases and the CH₄ concentration decreases, the probability of spontaneous ignition during high-pressure H₂/CH₄ mixture discharge increases, and it is more likely to develop into stable flames propagating downstream.

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