含能双环HMX衍生物分子设计的密度泛函研究（英文）
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摘要
运用DFT-B3LYP/6-311G(d,p)方法,计算了所设计的三种双环HMX(2,4,6,8-四硝基-2,4,6,8-四氮杂双环[3.3.0]辛烷)衍生物分子.基于理论晶体密度和固态生成热计算衍生物分子的爆轰性能;通过前线轨道能与特征高度(h_(50))评价衍生物分子的感度.结果表明,理论晶体密度均高于1.90 g·cm~(-3),爆速高于9.0 km·s~(-1),爆压约为40 GPa.三种双环HMX衍生物分子是潜在的高能量密度材料.
Three new bicyclo-HMX(2,4,6,8-tetranitro-1 H,5 H-2,4,6,8-tetraaza-bicyclo[3.3.0]octane) derivatives have been designed and calculated at the density functional theory(DFT)-B3 LYP/6-311 G(d,p) level. Detonation performance was evaluated by Kamlet-Jacobs(K-J) equations based on the theoretical crystal densities and condensed-phase heats of formation. Sensitivity was evaluated using the frontier orbital energies and characteristic heights(h_(50)). The predicted theoretical crystal densities of the derivatives were above 1.90 g·cm~(-3), detonation velocities were over 9.0 km·s~(-1), and detonation pressures were about 40 GPa, showing that bicyclo-HMX derivatives may be the potential high energetic density materials(HEDMs).
Three new bicyclo-HMX(2,4,6,8-tetranitro-1 H,5 H-2,4,6,8-tetraaza-bicyclo[3.3.0]octane) derivatives have been designed and calculated at the density functional theory(DFT)-B3 LYP/6-311 G(d,p) level. Detonation performance was evaluated by Kamlet-Jacobs(K-J) equations based on the theoretical crystal densities and condensed-phase heats of formation. Sensitivity was evaluated using the frontier orbital energies and characteristic heights(h_(50)). The predicted theoretical crystal densities of the derivatives were above 1.90 g·cm~(-3), detonation velocities were over 9.0 km·s~(-1), and detonation pressures were about 40 GPa, showing that bicyclo-HMX derivatives may be the potential high energetic density materials(HEDMs).
引文
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[8] Lee C,Yang W,Parr R G.Development of the colle-salvetti correlation-energy formula into a functional of the electron density [J].Phys.Rev.B,1988,37:785.
[9] Becke A D.Density functional thermochemistry.III.the role of exact exchange [J].J.Chem.Phys.,1993,98:5648.
[10] Hariharan P C,Pople J A.The influence of polarization functions on molecular orbital hydrogenation energies [J].Theor.Chim.Acta,1973,28:213.
[11] Wei T,Zhu W H,Zhang J,et al.DFT study on energetic tetrazolo-[1,5-b]-1,2,4,5- tetrazine and 1,2,4-triazolo-[4,3-b]-1,2,4,5-tetrazine derivatives [J].J.Hazard Mater.,2010,179:581.
[12] Guo X J,Li B,Ren F D,et al.A theoretical prediction of the relationships between the impact sensitivity and electrostatic potential in nitrocyclobutane explosive with the C-NO2 groups and its derivatives [J].J.At.Mol.Phys.,2016,33:773 (in Chinese)
[13] Politzer P,Martinez J,Murray J S,et al.An electrostatic interaction correction for improved crystal density prediction [J].Mol.Phys.,2009,107:2095.
[14] Lide D R.CRC handbook of chemistry and physics [M].Florida:CRC Press,2002.
[15] Atkins P W.Physical chemistry[M].2nd ed.Oxford:Oxford University Press,1982.
[16] Politzer P,Murray J S,Grice M E,et al.Calculation of heats of sublimation and solid phase heats of formation [J].Mol.Phys.,1997,91:923.
[17] Xiao H M,Zhu W H,Xiao J J,et al.Separation and incorporation of microcosmic theoretical investigation for high energetic materials [J].Chin.J.Energ.Mater.,2015,23:1038 (in Chinese)
[18] Jaidann M,Roy S,Abou-Rachid H,et al.A DFT theoretical study of heats of formation and detonation properties of nitrogen-rich explosives [J].J.Hazard Mater.,2010,176:165.
[19] Hill T L.Introduction to Statistic Thermodynamics [M].New York:Addison-Wesley,1960.
[20] Kamlet M J,Jacobs S J.A simple method for calculating detonation properties of C [single bond] H [single bond] N [single bond] O explosives [J].J.Chem.Phys.,1968,48:23.
[21] Pospí?il M,Vávra P,Concha M C,et al.A possible crystal volume factor in the impact sensitivities of some energetic compounds [J].J.Mol.Model.,2010,16:895.