Pressure effects on the thermal decomposition of the LLM-105 crystal
Pressure effects on the thermal decomposition of the LLM-105 crystal
复制标题
压力对LLM-105晶体热分解的影响
DOI：
10.1039/d1cp04076f
复制
发表时间：
2021-12-22
影响因子：
3.3
通讯作者：
Zhang, Zengming
中科院分区：
文献类型：
--
作者：
Wang, Junke;Gao, Chan;Zhang, Zengming
高温高压下的热力学响应是了解含能材料性能的基本信息。本文研究了压力对2,6-二氨基-3,5-二硝基吡嗪-1-氧化物（LLM-105）热衰减的影响。在4.6 GPa的初始压力下，LLM-105晶体建立了压力依赖的分解边界，直到LLM-105晶体分解才发生相变。通过较弱的加载压力，分解温度显著提高。实验测量证实了密度功能紧密结合分子动力学方法预测的分解产物NO2、CO2和NH3。计算描述了高压下初始阶段热衰减的细节。高压下与氢键相关的拉曼模式位移的突然下降表明分子间氢键的增强和晶体分解前分子间氢转移的发生。模拟结果支持了分子间氢传递的存在，并提供了传递路径和分解机理。所有这些工作不仅有助于理解含能材料的热分解作为压力的函数，而且有助于理解敏感机制和安全问题。
Thermal mechanical responses under high temperature and high pressure are basic information to understand the performance of energetic materials. In this work, the pressure effects on the thermal decay of 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) are explored. Up to the initial pressure of 4.6 GPa, the pressure dependent decomposition boundary is built and no phase transition occurs until the decomposition of the LLM-105 crystal. The decomposition temperature is significantly lifted via a weak loading pressure. The experimental measurement confirms the decomposition products, including NO2, CO2 and NH3, which are predicted by the density functional tight-binding molecular dynamics method. The calculation described the details of thermal decay in the initial stages under high pressure. The sudden drop in the shifts of the Raman modes associated with hydrogen bonds under high pressure indicates the strengthening of the intermolecular hydrogen bonds and the occurrence of intermolecular hydrogen transfer prior to crystal decomposition. The simulation supported the existence of intermolecular hydrogen transfer and provided the transfer path and decomposition mechanism. All of these jobs not only contribute significantly to the understanding of thermal decomposition of energetic materials as a function of pressure, but also contribute to the understanding of sensitivity mechanisms and safety issues.