摘要
基于2-叠氮-1,3-咪唑、3-叠氮-1,2,4-三唑和5-叠氮-1氢-四唑的晶体结构数据,自行设计了同系列化合物叠氮-五唑的分子结构.采用B3LYP方法,选取6-311++G**基组,对叠氮唑类化合物进行优化并得到了稳定的分子构型,结构参数与现有的实验数据相符.故在此水平下对此系列化合物进行红外振动、键级及自然键轨道分析,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,分子中存在一个大的共轭体系;根据前线轨道能隙差(ΔEL-H)得到4种化合物的热稳定顺序为:5-叠氮-1-氢-四唑>3-叠氮-1,2,4-三唑>叠氮-五唑>2-叠氮-1,3-咪唑;计算得到的生成热、密度、爆速爆压均随着体系中含氮量的增加而增加,即叠氮-五唑的爆速、爆压最大,爆速达到了9897 m·s-1,爆压达到了46.0 GPa,在含能材料领域具有潜在的应用前景.
Based on the crystal data of 2-azido-1,3-imidazole,3-azido-1,2,4-triazole and 5-azido-1H-tetrazole,a novel of azido-pentazole was firstly devised.The most stable molecular geometries of azide-azole compounds were obtained using B3LYP methods with 6-311＋＋G＊＊ basis set.Compared with existing experimental data,B3LYP/6-311＋＋G＊＊ is the suitable basis set for compounds.Moreover,IR spectra and bond order of azide-azole nitrogen-rich energetic compounds were obtained.The results show that they have not imaginary frequencies,so they were stable on the potential energy surface.There is a great conjugate system among molecular structures.The frontier orbital energies and their differences predict that the stabilities of the title compounds decrease in the order： 5-azido-1H-tetrazole3-azide-1,2,4-triazole azido-pentazole2-azido-1,3-imidazole.The results show that heat of formation,density,detonation veloc-ity and detonation pressure of the title compounds linearly increase with increasing nitrogen mass fraction in the system.Azido-pentazole with detonation velocity of 9897 m·s-1,and the detonation pressure of 46.0 GPa,which has potential applications in the high energy density materials.
出处
《化学学报》
SCIE
CAS
CSCD
北大核心
2011年第6期610-616,共7页
Acta Chimica Sinica
基金
国家自然科学基金委-中国工程物理研究院联合基金(No.10776002)
国家自然科学基金(No.20911120033)
教育部新世纪优秀人才支持计划(NCET-09-0051)资助项目
关键词
高氮化合物
结构优化
振动分析
生成热
爆速
爆压
nitrogen-rich compounds
molecular geometry
frequency analysis
heat of formation
detona-tion velocity
detonation pressure
