Abstract Meso-scale modeling of heterogeneous energetic materials requires accurate description of the chemical reaction model that governs the decomposition of solid energetic crystals to gaseous products. For HMX, various 1-step and multi-step Arrhenius based chemical kinetic models are available; these chemical kinetics models for HMX have been calibrated against macro-scale experimental data under different ranges of pressure and temperature conditions, which may lie outside the ranges that arise during void collapse. Therefore, depending on the reaction model, the predicted meso-scale hotspot initiation and growth behavior can vary. Here, we examine the effects of five global HMX reaction kinetics models on predictions of void collapse induced hotspots, viz. the Henson-Smilowitz 1-step (HS1), Menikoff 1-step (M1), Tarver-Nichols 3-step (TN3), Henson-Smilowitz 9-step (HS9) and a 7-step extended Brill-Yetter model (BYS7). Variations in the hotspot behavior predicted using the different models are observed to be significant. A detailed examination of the individual reaction mechanisms of each of these global chemistry models is undertaken to provide insights and understanding of the reaction steps that lead to the differences in the predicted hotspot behavior. For the temperature regime relevant to the void collapse generated hotspots, the differences in the hotspot behavior are attributed to the orders of magnitude variations in the reaction rates that govern the maximum energy release during HMX decomposition. The paper shows that the issue of a suitable kinetics model, even for the commonly used HMX material, remains unsettled.

中文翻译：

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用于 HMX 中热点起始和生长的中尺度模拟的反应动力学模型评估

摘要 异质含能材料的中尺度建模需要准确描述控制固体含能晶体分解为气态产物的化学反应模型。对于 HMX，可以使用各种基于 Arrhenius 的 1 步和多步化学动力学模型；这些 HMX 的化学动力学模型已经针对不同压力和温度条件范围下的宏观实验数据进行了校准，这些数据可能超出了空隙坍塌过程中出现的范围。因此，根据反应模型，预测的中尺度热点起始和生长行为可能会有所不同。在这里，我们研究了五种全局 HMX 反应动力学模型对空隙坍塌诱导热点预测的影响，即。Henson-Smilowi​​tz 1-step (HS1), Menikoff 1-step (M1), Tarver-Nichols 3-step (TN3), Henson-Smilowi​​tz 9 步 (HS9) 和 7 步扩展 Brill-Yette 模型 (BYS7)。观察到使用不同模型预测的热点行为的变化是显着的。对这些全球化学模型中的每一个的个体反应机制进行了详细检查，以提供对导致预测热点行为差异的反应步骤的见解和理解。对于与空隙坍塌产生的热点相关的温度范围，热点行为的差异归因于控制 HMX 分解过程中最大能量释放的反应速率的数量级变化。该论文表明，即使对于常用的 HMX 材料，合适的动力学模型的问题仍未解决。