This study investigates the paradoxical detonation behavior of TKX-50,a nitrogen-rich energetic material,exhibiting higher detonation velocities but lower metal acceleration ability compared to HMX.Through experimenta...This study investigates the paradoxical detonation behavior of TKX-50,a nitrogen-rich energetic material,exhibiting higher detonation velocities but lower metal acceleration ability compared to HMX.Through experimental measurements and theoretical calculations,we propose a novel three-factor competition mechanism to explain this phenomenon.TKX-50-based PBX formulations achieved detonation velocities up to 9100 m/s,surpassing HMX-based counterparts.However,cylinder expansion tests revealed a 15%reduction in metal acceleration ability.Thermochemical measurements showed lower detonation heat for TKX-50(4900 J/g)versus HMX(5645 J/g).Our mechanism involves:(1)compositional effects prevailing at high pressures;(2)Energy release becoming essential as pressure drops;(3)Pressure-dependent product composition evolution functioning at low pressure.VLW code calculations unveiled a"crossover"in Hugoniot curves,lending support to this mechanism.This study furnishes a new framework for comprehending the performance of nitrogen-rich energetic materials,with significant implications for the design and optimization of future high-energy density materials.展开更多
Chemical inclusions significantly alter shock responses of crystalline explosives in macroscale gap experiments but their microscale dynamics origin remains unclear.Herein shock-induced energy localization,overall phy...Chemical inclusions significantly alter shock responses of crystalline explosives in macroscale gap experiments but their microscale dynamics origin remains unclear.Herein shock-induced energy localization,overall physical responses,and reactions in a-1,3,5-trinitro-1,3,5-triazinane(a-RDX)crystal entrained various chemical inclusions were investigated by the multi-scale shock technique implemented in the reactive molecular dynamics method.Results indicated that energy localization and shock reaction were affected by the intrinsic factors within chemical inclusions,i.e.,phase states,chemical compositions,and concentrations.The atomic origin of chemical-inclusions effects on energy localization is dependent on the dynamics mechanism of interfacial molecules with free space volume,which includes homogeneous intermolecular compression,interfacial impact and shear,and void collapse and jet.As introducing various chemical inclusions,the initiation of those dynamics mechanisms triggers diverse decay rates of bulk RDX molecules and hereby impacts on growth speeds of final reactions.Adding chemical inclusions can reduce the effectiveness of the void during the shock impacting.Under the shockwave velocity of 9 km/s,the parent RDX decay rate in RDX entrained amorphous carbon decreases the most and is about one fourth of that in RDX with a vacuum void,and solid HMX and TATB inclusions are more reactive than amorphous carbon but less reactive than dry air or acetone inclusions.The lessdense shocking system denotes the greater increases in local temperature and stress,the faster energy liberation,and the earlier final reaction into equilibrium,revealing more pronounced responses to the present intense shockwave.The quantitative models associated with the relative system density(RD_(sys))were proposed for indicating energy-localization mechanisms and evaluating initiation safety in the shocked crystalline explosive.RD_(sys)is defined by the density ratio of defective RDX to perfect crystal after dynamics relaxation and reveals the global density characteristic in shocked systems filled with chemical inclusions.When RD_(sys)is below 0.9,local hydrodynamic jet initiated by void collapse dominates upon energy localization instead of interfacial impact.This study sheds light on novel insights for understanding the shock chemistry and physical-based atomic origin in crystalline explosives considering chemical-inclusions effects.展开更多
The practical application of energetic materials, particularly 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(CL-20), is frequently impeded by phase transition challenges. In this study, we propose a novel...The practical application of energetic materials, particularly 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(CL-20), is frequently impeded by phase transition challenges. In this study, we propose a novel strategy to enhance the stability of CL-20 by employing a thermo-sensitive polymer,poly(N-isopropylacrylamide)(PNIPAM), to modulate its phase transitions. Our approach involves the use of an in-situ polymerized polydopamine(PDA) shell as a platform for surface grafting through atom transfer radical polymerization, yielding a core-shell structured CL-20@PDA-PNIPAM. Through comprehensive characterization, the successful grafting of PNIPAM is confirmed, significantly enhanced the phase stability of CL-20. Notably, our core-shell structure exhibits a 13℃ increase in phase transition temperature compared to raw CL-20, thereby delaying the ε→a phase transition by over 80 min under combined thermal and solvent conditions. The enhanced stability is attributed to the hydrophobic nature of PNIPAM above its low critical solution temperature in water, which effectively shields the CL-20 crystal. These findings provide new insights into enhancing the stability and safety of energetic materials in complex environments, highlighting the potential of our molecular switch mechanism.展开更多
Understanding the response of solid combustibles under high radiant fluxes is critical in predicting the thermal damage from extreme scenarios.Unlike the more moderate radiant fluxes in conventional hydrocarbon fires,...Understanding the response of solid combustibles under high radiant fluxes is critical in predicting the thermal damage from extreme scenarios.Unlike the more moderate radiant fluxes in conventional hydrocarbon fires,extreme events such as strong explosion,concentrated sunlight and directed energy can generate dynamic radiant fluxes at the MW/m^(2) level,creating a unique threat to materials.This study investigates the pyrolysis and spontaneous ignition behaviors of corrugated cardboard by using both experimental and numerical methods,under 10-cm dynamic high radiant fluxes ranging from 0.2 to 1.25 MW/m^(2) for 10 s.The spontaneous ignition process at dynamic high radiant fluxes was recorded and quantified.Two ignition modes were found at the critical radiant flux of 0.4 MW/m^(2),namely hot-gas spontaneous ignition and hot-residue piloted ignition.The latter is not the focus of this paper due to its extremely small probability of occurrence.The research reveals that the increase in flux intensity induces shorter delay times for both pyrolysis and ignition,lower ignition energy density,along with a corresponding rise in the critical mass flux and surface temperature at ignition moment.The simulation results are generally aligned with the experimental findings,despite some divergences may be attributed to model simplifications and parameter assumptions.The work contributes to a deeper insight into material behavior under extreme radiation,with valuable implications for fire safety and hazard assessment.展开更多
基金support provided by the National Natural Science Foundation of China(Grant No.12102405)the Presidential Foundation of CAEP(Grant No.YZJJZQ2023008).
文摘This study investigates the paradoxical detonation behavior of TKX-50,a nitrogen-rich energetic material,exhibiting higher detonation velocities but lower metal acceleration ability compared to HMX.Through experimental measurements and theoretical calculations,we propose a novel three-factor competition mechanism to explain this phenomenon.TKX-50-based PBX formulations achieved detonation velocities up to 9100 m/s,surpassing HMX-based counterparts.However,cylinder expansion tests revealed a 15%reduction in metal acceleration ability.Thermochemical measurements showed lower detonation heat for TKX-50(4900 J/g)versus HMX(5645 J/g).Our mechanism involves:(1)compositional effects prevailing at high pressures;(2)Energy release becoming essential as pressure drops;(3)Pressure-dependent product composition evolution functioning at low pressure.VLW code calculations unveiled a"crossover"in Hugoniot curves,lending support to this mechanism.This study furnishes a new framework for comprehending the performance of nitrogen-rich energetic materials,with significant implications for the design and optimization of future high-energy density materials.
基金the financial support from National Natural Science Foundation of China(Grant Nos.11872119,12172051,and 11972329)Natural Science Foundation of Hubei Province(Grant No.2021CFB120)。
文摘Chemical inclusions significantly alter shock responses of crystalline explosives in macroscale gap experiments but their microscale dynamics origin remains unclear.Herein shock-induced energy localization,overall physical responses,and reactions in a-1,3,5-trinitro-1,3,5-triazinane(a-RDX)crystal entrained various chemical inclusions were investigated by the multi-scale shock technique implemented in the reactive molecular dynamics method.Results indicated that energy localization and shock reaction were affected by the intrinsic factors within chemical inclusions,i.e.,phase states,chemical compositions,and concentrations.The atomic origin of chemical-inclusions effects on energy localization is dependent on the dynamics mechanism of interfacial molecules with free space volume,which includes homogeneous intermolecular compression,interfacial impact and shear,and void collapse and jet.As introducing various chemical inclusions,the initiation of those dynamics mechanisms triggers diverse decay rates of bulk RDX molecules and hereby impacts on growth speeds of final reactions.Adding chemical inclusions can reduce the effectiveness of the void during the shock impacting.Under the shockwave velocity of 9 km/s,the parent RDX decay rate in RDX entrained amorphous carbon decreases the most and is about one fourth of that in RDX with a vacuum void,and solid HMX and TATB inclusions are more reactive than amorphous carbon but less reactive than dry air or acetone inclusions.The lessdense shocking system denotes the greater increases in local temperature and stress,the faster energy liberation,and the earlier final reaction into equilibrium,revealing more pronounced responses to the present intense shockwave.The quantitative models associated with the relative system density(RD_(sys))were proposed for indicating energy-localization mechanisms and evaluating initiation safety in the shocked crystalline explosive.RD_(sys)is defined by the density ratio of defective RDX to perfect crystal after dynamics relaxation and reveals the global density characteristic in shocked systems filled with chemical inclusions.When RD_(sys)is below 0.9,local hydrodynamic jet initiated by void collapse dominates upon energy localization instead of interfacial impact.This study sheds light on novel insights for understanding the shock chemistry and physical-based atomic origin in crystalline explosives considering chemical-inclusions effects.
基金supported by National Natural Science Foundation of China(Grant Nos.U2130207,21875232,12372342)Foundation of President of China Academy of Engineering Physics(Grant Nos.YZJJZQ2023008,YZJJZQ2022006)the Foundation of China Academy of Engineering Physics(Grant Nos.CX20210015,CX20210027)。
文摘The practical application of energetic materials, particularly 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(CL-20), is frequently impeded by phase transition challenges. In this study, we propose a novel strategy to enhance the stability of CL-20 by employing a thermo-sensitive polymer,poly(N-isopropylacrylamide)(PNIPAM), to modulate its phase transitions. Our approach involves the use of an in-situ polymerized polydopamine(PDA) shell as a platform for surface grafting through atom transfer radical polymerization, yielding a core-shell structured CL-20@PDA-PNIPAM. Through comprehensive characterization, the successful grafting of PNIPAM is confirmed, significantly enhanced the phase stability of CL-20. Notably, our core-shell structure exhibits a 13℃ increase in phase transition temperature compared to raw CL-20, thereby delaying the ε→a phase transition by over 80 min under combined thermal and solvent conditions. The enhanced stability is attributed to the hydrophobic nature of PNIPAM above its low critical solution temperature in water, which effectively shields the CL-20 crystal. These findings provide new insights into enhancing the stability and safety of energetic materials in complex environments, highlighting the potential of our molecular switch mechanism.
基金the Presidential Foundation of CAEP(Grant No.YZJJZQ2023008)the National Natural Science Foundation of China(Grant No.NSFC 12372342)for financial support of this work.
文摘Understanding the response of solid combustibles under high radiant fluxes is critical in predicting the thermal damage from extreme scenarios.Unlike the more moderate radiant fluxes in conventional hydrocarbon fires,extreme events such as strong explosion,concentrated sunlight and directed energy can generate dynamic radiant fluxes at the MW/m^(2) level,creating a unique threat to materials.This study investigates the pyrolysis and spontaneous ignition behaviors of corrugated cardboard by using both experimental and numerical methods,under 10-cm dynamic high radiant fluxes ranging from 0.2 to 1.25 MW/m^(2) for 10 s.The spontaneous ignition process at dynamic high radiant fluxes was recorded and quantified.Two ignition modes were found at the critical radiant flux of 0.4 MW/m^(2),namely hot-gas spontaneous ignition and hot-residue piloted ignition.The latter is not the focus of this paper due to its extremely small probability of occurrence.The research reveals that the increase in flux intensity induces shorter delay times for both pyrolysis and ignition,lower ignition energy density,along with a corresponding rise in the critical mass flux and surface temperature at ignition moment.The simulation results are generally aligned with the experimental findings,despite some divergences may be attributed to model simplifications and parameter assumptions.The work contributes to a deeper insight into material behavior under extreme radiation,with valuable implications for fire safety and hazard assessment.
