基于Noradamantane的高能量密度富氮笼型含能分子设计与性能预估  

Design and Performance Prediction of High⁃energy⁃density Nitrogen⁃rich Cage Energetic Molecules based on Noradamantane

作　　者：王威文 陈丽珍[1] 张朝阳[2] 谢炜宇 WANG Wei-wen;CHEN Li-zhen;ZHANG Chao-yang;XIE Wei-yu(School of Chemistry and Chemical Engineering,North University of China,Taiyuan 030051,China;Institute of Chemical Materials,Chinese Academy of Engineering Physics,Mianyang 621999,China)

机构地区：[1]中北大学化学与化工学院,山西太原030051 [2]中国工程物理研究院化工材料研究所,四川绵阳621999

出　　处：《含能材料》2024年第10期1099-1109,共11页Chinese Journal of Energetic Materials

摘　　要：研究提出一种通过化学键键能差进行能量密度快速估算的方法,和一种利用拉普拉斯键级和分子片段键离解能相结合快速判断笼型结构稳定性的方法。通过穷举法构建了基于Noradamantane的所有富氮骨架及其435种硝基衍生物,应用上述计算方法筛选兼具高能量密度和稳定性的分子结构,并采用量子化学能量计算和过渡态反应势垒计算验证筛选结果的可靠性。计算发现了两种兼顾高能量密度和结构稳定性的硝基化合物,其爆热、爆速、爆压和金属加速能力的理论计算最大值分别达到7.77 k J·g^(-1)、10.1 km·s^(-1)、47 GPa和1.14倍HMX的金属加速能力,且结构分解反应势垒≥96 k J·mol^(-1)。本研究所建立的含能分子能量密度和稳定性快速筛选方法,可为高能稳定的含能分子设计提供参考。This study presents a method for rapidly estimating energy density based on the energy difference of chemical bonds,along with a technique for promptly evaluating cage structural stability by integrating Laplacian bond order and the bond dissoci-ation energy of molecular fragments.By exhaustively constructing all nitrogen-rich frameworks derived from Noradamantane and its 435 nitro derivatives,the study applied the aforementioned computational methods to screen molecular structures with high energy density and stability.The reliability of the screening results was confirmed through quantum chemical energy calculations and transition state reaction barrier calculations.Two nitro compounds exhibiting both high energy density and structural stability were identified,with theoretical maximum values of detonation heat,detonation velocity,detonation pressure,and metal accel-eration capability reaching 7.77 kJ·g^(-1),10.1 km·s^(-1),47 GPa,and 1.14 times the metal acceleration capability of HMX,respec-tively,and with structural decomposition reaction barriers≥96 kJ·mol^(-1).The rapid screening method for energy density and sta-bility of energetic molecules established in this study can provide theoretical guidance for the future design of high-energy stable energetic molecules.

关 键 词：富氮笼型分子 能量估算 稳定结构筛选 高能量密度材料 

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]