异伍兹烷衍生物高温热分解规律分子动力学模拟  

Molecular Dynamics Simulation on the High Temperature Thermal Decomposition of Derivatives of Isowurtzitane

作　　者：甘强[1] 张文博 王亚军[1] 梁琳 任姝 李根[1] 何佳峻 冯长根[1] GAN Qiang;ZHANG Wen-bo;WANG Ya-jun;LIANG Lin;REN Shu;LI Gen;HE Jia-jun;FENG Chang-gen(State Key Laboratory of Explosion Science and Safety Protection,Beijing Institute of Technology,Beijing 100081,China)

机构地区：[1]北京理工大学爆炸科学与安全防护全国重点实验室,北京100081

出　　处：《含能材料》2024年第7期711-725,共15页Chinese Journal of Energetic Materials

基　　金：国家自然科学基金(22275018);爆炸科学与技术国家重点实验室(北京理工大学)自主课题(QNKT20-04)。

摘　　要：异伍兹烷衍生物是当前最具潜力的笼形含能化合物之一,为了系统研究异伍兹烷衍生物的高温热分解规律,明确其爆轰机理,研究采用ReaxFF-lg反应性力场和分子动力学方法,对3种典型异伍兹烷衍生物ε-六硝基六氮杂异伍兹烷(ε-CL-20)、4,10-二硝基-2,6,8,12-四氧杂-4,10-二氮杂四环十二烷(TEX)和4,10-二叠氮甲基-2,6,8,12-四硝基六氮杂异伍兹烷(BATNIW)进行高温(1500~3500 K)热分解研究。结果表明,脱硝基和开环是3种衍生物的主要初始反应,其中开环反应集中在五元环C—N键或C—O键。不同温度下热分解终产物中CO_(2)和H_(2)含量差异较大,3000 K以上N_(2)含量接近。3种衍生物中,BATNIW热分解生成N_(2)速度最快、产量最高;TEX热分解易生成团簇,生成特征产物乙二醛。3种衍生物热分解活化能排序为TEX>BATNIW>ε-CL-20,说明TEX稳定性最好。研究初步揭示了3种异伍兹烷衍生物分子结构与热分解规律的内在联系。Isowurtzitane derivatives are currently one of the most potential cage energetic compounds.In order to systematically study the high temperature thermal decomposition law of isowoodsane derivatives and clarify their detonation mechanism,in this work,the thermal decomposition properties of hexanitrohexaazaisowurtzitane(ε-CL-20),4,10-dinitro-2,6,8,12-tetraoxa-4,10-diaztetracyclododecane(TEX)and 4,10-diazomethyl-2,6,8,12-tetranitrohexaazaisowurzane(BATNIW)under high temperature(1500-3500 K)were studied by molecular dynamic simulations with ReaxFF-lg reactive force field and molecular dynamics method.The results show that the denitro and ring opening are the main initial reactions ofε-CL-20,TEX and BATNIW,in which the ring opening mainly occurs at the C─N bonds or C─O bonds of the five membered rings.Among the decomposition products,the yields of CO_(2) and H_(2) change significantly under different temperature,while content of N_(2) are similar at temperature higher than 3000 K.The decomposition of BATNIW produced N_(2) with the highest reaction rate and the maximum yield.During the thermal decomposition of TEX,clusters could easily be produced,and glyoxal could be regarded as its characteristic product.The order of thermal decomposition activation energy of the three derivatives is TEX>BATNIW>ε-CL-20,which suggests TEX shows the best stability.This work preliminarily reveals the relationship between the molecular structure and thermal decomposition of three isowurtzitane derivatives.

关 键 词：异伍兹烷衍生物 六硝基六氮杂异伍兹烷 高温热分解 分子动力学方法 ReaxFF-lg反应性力场 

分 类 号：TJ55[兵器科学与技术—军事化学与烟火技术] O64[理学—物理化学]