新型高氮含能叠氮化物的分子设计与理论研究(英文)

Molecular Design and Theoretical Study on Novel High-nitrogen Energetic Azido Compounds

根据CH4、BH3、NH3以及C2H4的结构特点,设计了7种新型叠氮类高氮含能化合物C(N3)4、B(N3)3和N(N3)3;CC(N3)4、BN(N3)4、NN(N3)4和CC(N3)6,在B3PW91/6-311+G(d)水平下对上述化合物进行了构型优化、振动频率以及键级分析,计算结果表明,所有化合物均无虚频,为势能面上的稳定结构,理论计算的红外结果与现有的实验结果十分相符。键级结果表明中心原子形成的键相对较弱,为爆炸时可能的首发键。计算得到了目标化合物的生成热、密度、爆速和爆压。计算得到几乎所有分子的爆速和爆压都超过了HMX,在含能材料领域具有潜在的应用前景。

Seven high-nitrogen energetic compounds were devised： C（N3）4, B（N3）3, N（N3）3; CC（N3）4, BN（N3）4, NN（N3）4 and CC（N3）6, which are structurally similar to CH4, BH3, NH3 and C2H4. The molecular geometries, IR spectra, bond order and frontier orbital energies of these compounds were obtained at B3PW91/6-311＋G（d） level of theory. The calculated results show that they were stable on the related potential energy surface. The theoretical spectrum agreed well with the experimental value. According to the results of bond orders, we could predict that the possible primary decomposition reactions of the title compounds may be the elimination of azido group or the center bond breaking. The heat of formation, density and detonation performance of the above compounds were obtained. These results indicate that almost all titled compounds have potential applications in the field of high energy density materials.