奥克托今/3-硝基-1,2,4-三唑-5-酮共晶炸药晶体缺陷的分子动力学研究
|
摘要
为研究晶体缺陷对奥克托今(HMX)/3-硝基-1,2,4-三唑-5-酮(NTO)共晶炸药稳定性、感度、爆轰性能与力学性能的影响,分别建立了"完美"型与含有掺杂、空位与位错缺陷的共晶炸药模型。采用分子动力学方法,预测了"完美"型与缺陷模型的性能,得到了不同模型的结合能、引发键键长分布、键连双原子作用能、内聚能密度、爆轰参数与力学性能参数,并进行了比较。结果表明:由于晶体缺陷的影响,造成炸药结合能减小,稳定性变差;缺陷晶体的引发键最大键长增大,键连双原子作用能与内聚能密度减小,炸药感度升高,安全性减弱;缺陷晶体的密度、爆速与爆压减小,能量密度与威力降低;与"完美"型晶体相比,缺陷晶体的拉伸模量、体积模量与剪切模量减小,柯西压力增大,炸药刚性与硬度减弱,柔性与延展性增强。
The "perfect"and defective cocrystal models with adulteration,vacancy and dislocation are established to investigate the influence of crystal defect on stability,sensitivity,detonation performance and mechanical property of octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine( HMX)/3-nitro-1,2,4-triazol-5-one( NTO) cocrystal explosive. Molecular dynamics method is applied to predict the properties of the proposed crystal models. The binding energy,bond length distribution of trigger bond,interaction energy of trigger bond,cohesive energy density,detonation parameters and mechanical properties were obtained and compared. The results show that the binding energy of explosive is declined and its stability is weakened due to the influence of crystal defect. The maximum trigger bond length of defective crystal model is increased,while the interaction energy of trigger bond and the cohesive energy density are decreased,meaning that the sensitivity of explosive is increased and its safety is worsened. The density,detonation velocity and detonation pressure of defective crystal model are declined,indicating that the energy density and power are lessened. Compared with the "perfect"crystal model,the tensile modulus,bulkmodulus and shear modulus of defective crystal model are decreasaed,and Cauchy pressure is increased,namely,the rigidity and stiffness are declined and the plastic property and ductility are increased.
The "perfect"and defective cocrystal models with adulteration,vacancy and dislocation are established to investigate the influence of crystal defect on stability,sensitivity,detonation performance and mechanical property of octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine( HMX)/3-nitro-1,2,4-triazol-5-one( NTO) cocrystal explosive. Molecular dynamics method is applied to predict the properties of the proposed crystal models. The binding energy,bond length distribution of trigger bond,interaction energy of trigger bond,cohesive energy density,detonation parameters and mechanical properties were obtained and compared. The results show that the binding energy of explosive is declined and its stability is weakened due to the influence of crystal defect. The maximum trigger bond length of defective crystal model is increased,while the interaction energy of trigger bond and the cohesive energy density are decreased,meaning that the sensitivity of explosive is increased and its safety is worsened. The density,detonation velocity and detonation pressure of defective crystal model are declined,indicating that the energy density and power are lessened. Compared with the "perfect"crystal model,the tensile modulus,bulkmodulus and shear modulus of defective crystal model are decreasaed,and Cauchy pressure is increased,namely,the rigidity and stiffness are declined and the plastic property and ductility are increased.
引文
[1] BOLTON O,SIMKE L R,PAGORIA P F,et al. High power explosive with good sensitivity:a 2∶1 cocrystal of CL-20:HMX[J].Crystal Growth&Design,2012,12(9):4311-4314.
[2] LIU K,ZHANG G,LUAN J Y,et al. Crystal structure,spectrum character and explosive property of a new cocrystal CL-20/DNT[J]. Journal of Molecular Structure,2016,1110:91-96.
[3]侯聪花,刘志强,张园萍,等. TATB/HMX共晶炸药的制备及性能研究[J].火炸药学报,2017,40(4):44-49.HOU C H,LIU Z Q,ZHANG Y P,et al. Study on preparation and properties of TATB/HMX cocrystal explosive[J]. Chinese Journal of Explosives&Propellants,2017,40(4):44-49.(in Chinese)
[4] GAO H,DU P,KE X,et al. A novel method to prepare nanosized CL-20/NQ cocrystal:vacuum freeze drying[J]. Propellants,Explosives,Pyrotechnics,2017,42(8):889-895.
[5] LIN H,ZHU S G,ZHANG L,et al. Intermolecular interactions,thermodynamic properties,crystal structure,and detonation performance of HMX/NTO cocrystal explosive[J]. International Journal of Quantum Chemistry,2013,113(10):1591-1599.
[6] ZHOU T T,HUANG F L. Effects of defects on thermal decomposition of HMX via Reax FF molecular dynamics si-mulations[J].The Journal of Physical Chemistry B,2011,115(2):278-287.
[7]陈科全,蓝林钢,路中华,等.含预制缺陷PBX炸药裂纹扩展过程的试验研究[J].兵器装备工程学报,2017,38(1):134-136.CHEN K Q,LAN L G,LU Z H,et al. Experimental study on the crack growth of polymer bonded explosives with prefabricated defects[J]. Journal of Ordnance Equipment Engineering,2017,38(1):134-136.(in Chinese)
[8]王洪波,王旗华,卢永刚,等. PBX炸药细观孔洞缺陷对其冲击点火特性的影响[J].火炸药学报,2015,38(5):31-36.WANG H B,WANG Q H,LU Y G,et al. Effect of meso-defect holes on the shock-to-ignition characteristics of PBX explosives[J]. Chinese Journal of Explosives&Propellants,2015,38(5):31-36.(in Chinese)
[9] XUE X G,WEN Y S,LONG X P,et al. Influence of dislocations on the shock sensitivity of RDX:molecular dynamics simulations by reactive force field[J]. The Journal of Physical Chemistry C,2015,119(24):13735-13742.
[10]吕鹏博,王伟力,刘晓夏,等.含装药缺陷的侵爆战斗部穿甲过程装药安定性的数值模拟[J].海军航空工程学院学报,2017,32(4):389-394.LYU P B,WANG W L,LIU X X,et al. Numerical simulation of the stability of the charge of invasion of explosive warheads containing defects in armor-piercing process[J]. Journal of Naval Aeronautical and Astronautical University,2017,32(4):389-394.(in Chinese)
[11] SUN H,REN P,FRIED J R. The COMPASS force field:parameterization and validation for polyphosphazenes[J]. Computational and Theoretical Polymer Science,1998,8(1/2):229-246.
[12] SUN H. COMPASS:an ab initio force-field optimized for condensed-phase applications-overview with details on alkane and benzene compound[J]. The Journal of Physical Chemistry B,1998,102(38):7338-7364.
[13] ANDERSEN H C. Molecular dynamics simulations at constant pressure and/or temperature[J]. Journal of Chemical Physics,1980,72(4):2384-2393.
[14] PARRINELLO M,RAHMAN A. Polymorphic transitions in single crystals:a new molecular dynamics method[J]. Journal of Applied Physics,1981,52(12):7182-7190.
[15] BOWDEN F P,YOFFE A D. Initiation and growth of explosion in liquids and solids[M]. Cambridge,UK:Cambridge University Press,1952.
[16] KAMLET M J,ADOIPH H G. The relationship of impact sensitivity with structure of organic high explosives[J]. Propellants,Explosives,Pyrotechnics,1979,4(2):30-34.
[17]朱伟,刘冬梅,肖继军,等.多组分高能复合体系的感度判别、热膨胀和力学性能的MD研究[J].含能材料,2014,22(5):582-587.ZHU W,LIU D M,XIAO J J,et al. Molecular dynamics study on sensitivity criterion,thermal expansion and mechanical properties of multi-component high energy system[J]. Chinese Journal of Energetic Materials,2014,22(5):582-587.(in Chinese)
[18]刘强,肖继军,张将,等. CL-20/TNT共晶炸药的分子动力学研究[J].高等学校化学学报,2016,37(3):559-566.LIU Q,XIAO J J,ZHANG J,et al. Molecular dynamics simulation on CL-20/TNT cocrystal explosive[J]. Chemical Journal of Chinese Universities,2016,37(3):559-566.(in Chinese)
[19] SUN T,XIAO J J,LIU Q,et al. Comparative study on structure,energetic and mechanical properties of aε-CL-20/HMX cocrystal and its composite with molecular dynamics simulation[J].Journal of Materials Chemistry A,2014,2(34):13898-13904.
[20] XIAO J J,ZHAO L,ZHU W,et al. Molecular dynamics study on the relationships of modeling,structural and energy properties with sensitivity for RDX-based PBXs[J]. Science China Chemistry,2012,55(12):2587-2594.
[21] ZHU W,WANG X J,XIAO J J,et al. Molecular dynamics simulations of AP/HMX composite with a modified force field[J].Journal of Hazardous Materials,2009,167(1):810-816.
[22] MULLAY J. Relationship between impact sensitivity and molecular electronic structure[J]. Propellants,Explosives,Pyrotechnics,1987,12(4):121-124.
[23] BRILL B T,JAMES J K. Kinetics and mechanisms of thermal decomposition of nitroaromatic explosives[J]. Chemical Reviews,1993,93(8):2667-2692.
[24]彭亚晶,蒋艳雪.分子空位缺陷对环三亚甲基三硝胺含能材料几何结构、电子结构及振动特性的影响[J].物理学报,2015,64(24):243102-1-243102-9.PENG Y J,JIANG Y X. Analyses of the influences of molecular vacancy defect on the geometrical structure,electronic structure,and vibration characteristics of hexogeon energetic material[J].Acta Physica Sinica,2015,64(24):243102-1-243102-9.(in Chinese)
[25] DUAN X H,LI W P,PEI C H,et al. Molecular dynamics simulations of void defects in the energetic material HMX[J]. Journal of Molecular Modeling,2013,19(9):3893-3899.
[26]国迂贤,张厚生.炸药爆轰性质计算的氮当量公式及修正氮当量公式:炸药爆速的计算[J].爆炸与冲击,1983,3(3):56-66.GUO Y X,ZHANG H S. Nitrogen equivalent(NE)and modified nitrogen equivalent(MNE)equations for predicting detonation parameters of explosives-prediction of detonation velocity of explosives[J]. Explosion and Shock Waves,1983,3(3):56-66.(in Chinese)
[27]吴家龙.弹性力学[M].上海:同济大学出版社,1993.WU J L. Mechanics of elasticity[M]. Shanghai:Tongji University Press,1993.(in Chinese)
[28] WEINER J H. Statistical mechanics of elasticity[M].New York,NY,US:John Wiley&Sons,1983.
[2] LIU K,ZHANG G,LUAN J Y,et al. Crystal structure,spectrum character and explosive property of a new cocrystal CL-20/DNT[J]. Journal of Molecular Structure,2016,1110:91-96.
[3]侯聪花,刘志强,张园萍,等. TATB/HMX共晶炸药的制备及性能研究[J].火炸药学报,2017,40(4):44-49.HOU C H,LIU Z Q,ZHANG Y P,et al. Study on preparation and properties of TATB/HMX cocrystal explosive[J]. Chinese Journal of Explosives&Propellants,2017,40(4):44-49.(in Chinese)
[4] GAO H,DU P,KE X,et al. A novel method to prepare nanosized CL-20/NQ cocrystal:vacuum freeze drying[J]. Propellants,Explosives,Pyrotechnics,2017,42(8):889-895.
[5] LIN H,ZHU S G,ZHANG L,et al. Intermolecular interactions,thermodynamic properties,crystal structure,and detonation performance of HMX/NTO cocrystal explosive[J]. International Journal of Quantum Chemistry,2013,113(10):1591-1599.
[6] ZHOU T T,HUANG F L. Effects of defects on thermal decomposition of HMX via Reax FF molecular dynamics si-mulations[J].The Journal of Physical Chemistry B,2011,115(2):278-287.
[7]陈科全,蓝林钢,路中华,等.含预制缺陷PBX炸药裂纹扩展过程的试验研究[J].兵器装备工程学报,2017,38(1):134-136.CHEN K Q,LAN L G,LU Z H,et al. Experimental study on the crack growth of polymer bonded explosives with prefabricated defects[J]. Journal of Ordnance Equipment Engineering,2017,38(1):134-136.(in Chinese)
[8]王洪波,王旗华,卢永刚,等. PBX炸药细观孔洞缺陷对其冲击点火特性的影响[J].火炸药学报,2015,38(5):31-36.WANG H B,WANG Q H,LU Y G,et al. Effect of meso-defect holes on the shock-to-ignition characteristics of PBX explosives[J]. Chinese Journal of Explosives&Propellants,2015,38(5):31-36.(in Chinese)
[9] XUE X G,WEN Y S,LONG X P,et al. Influence of dislocations on the shock sensitivity of RDX:molecular dynamics simulations by reactive force field[J]. The Journal of Physical Chemistry C,2015,119(24):13735-13742.
[10]吕鹏博,王伟力,刘晓夏,等.含装药缺陷的侵爆战斗部穿甲过程装药安定性的数值模拟[J].海军航空工程学院学报,2017,32(4):389-394.LYU P B,WANG W L,LIU X X,et al. Numerical simulation of the stability of the charge of invasion of explosive warheads containing defects in armor-piercing process[J]. Journal of Naval Aeronautical and Astronautical University,2017,32(4):389-394.(in Chinese)
[11] SUN H,REN P,FRIED J R. The COMPASS force field:parameterization and validation for polyphosphazenes[J]. Computational and Theoretical Polymer Science,1998,8(1/2):229-246.
[12] SUN H. COMPASS:an ab initio force-field optimized for condensed-phase applications-overview with details on alkane and benzene compound[J]. The Journal of Physical Chemistry B,1998,102(38):7338-7364.
[13] ANDERSEN H C. Molecular dynamics simulations at constant pressure and/or temperature[J]. Journal of Chemical Physics,1980,72(4):2384-2393.
[14] PARRINELLO M,RAHMAN A. Polymorphic transitions in single crystals:a new molecular dynamics method[J]. Journal of Applied Physics,1981,52(12):7182-7190.
[15] BOWDEN F P,YOFFE A D. Initiation and growth of explosion in liquids and solids[M]. Cambridge,UK:Cambridge University Press,1952.
[16] KAMLET M J,ADOIPH H G. The relationship of impact sensitivity with structure of organic high explosives[J]. Propellants,Explosives,Pyrotechnics,1979,4(2):30-34.
[17]朱伟,刘冬梅,肖继军,等.多组分高能复合体系的感度判别、热膨胀和力学性能的MD研究[J].含能材料,2014,22(5):582-587.ZHU W,LIU D M,XIAO J J,et al. Molecular dynamics study on sensitivity criterion,thermal expansion and mechanical properties of multi-component high energy system[J]. Chinese Journal of Energetic Materials,2014,22(5):582-587.(in Chinese)
[18]刘强,肖继军,张将,等. CL-20/TNT共晶炸药的分子动力学研究[J].高等学校化学学报,2016,37(3):559-566.LIU Q,XIAO J J,ZHANG J,et al. Molecular dynamics simulation on CL-20/TNT cocrystal explosive[J]. Chemical Journal of Chinese Universities,2016,37(3):559-566.(in Chinese)
[19] SUN T,XIAO J J,LIU Q,et al. Comparative study on structure,energetic and mechanical properties of aε-CL-20/HMX cocrystal and its composite with molecular dynamics simulation[J].Journal of Materials Chemistry A,2014,2(34):13898-13904.
[20] XIAO J J,ZHAO L,ZHU W,et al. Molecular dynamics study on the relationships of modeling,structural and energy properties with sensitivity for RDX-based PBXs[J]. Science China Chemistry,2012,55(12):2587-2594.
[21] ZHU W,WANG X J,XIAO J J,et al. Molecular dynamics simulations of AP/HMX composite with a modified force field[J].Journal of Hazardous Materials,2009,167(1):810-816.
[22] MULLAY J. Relationship between impact sensitivity and molecular electronic structure[J]. Propellants,Explosives,Pyrotechnics,1987,12(4):121-124.
[23] BRILL B T,JAMES J K. Kinetics and mechanisms of thermal decomposition of nitroaromatic explosives[J]. Chemical Reviews,1993,93(8):2667-2692.
[24]彭亚晶,蒋艳雪.分子空位缺陷对环三亚甲基三硝胺含能材料几何结构、电子结构及振动特性的影响[J].物理学报,2015,64(24):243102-1-243102-9.PENG Y J,JIANG Y X. Analyses of the influences of molecular vacancy defect on the geometrical structure,electronic structure,and vibration characteristics of hexogeon energetic material[J].Acta Physica Sinica,2015,64(24):243102-1-243102-9.(in Chinese)
[25] DUAN X H,LI W P,PEI C H,et al. Molecular dynamics simulations of void defects in the energetic material HMX[J]. Journal of Molecular Modeling,2013,19(9):3893-3899.
[26]国迂贤,张厚生.炸药爆轰性质计算的氮当量公式及修正氮当量公式:炸药爆速的计算[J].爆炸与冲击,1983,3(3):56-66.GUO Y X,ZHANG H S. Nitrogen equivalent(NE)and modified nitrogen equivalent(MNE)equations for predicting detonation parameters of explosives-prediction of detonation velocity of explosives[J]. Explosion and Shock Waves,1983,3(3):56-66.(in Chinese)
[27]吴家龙.弹性力学[M].上海:同济大学出版社,1993.WU J L. Mechanics of elasticity[M]. Shanghai:Tongji University Press,1993.(in Chinese)
[28] WEINER J H. Statistical mechanics of elasticity[M].New York,NY,US:John Wiley&Sons,1983.