Skip to main content
SpringerLink
Log in

The influence of temperature and component proportion on stability, sensitivity, and mechanical properties of LLM-105/HMX co-crystals via molecular dynamics simulation

  • Original Paper
  • Published:
Journal of Molecular Modeling Aims and scope Submit manuscript

Abstract

Based on molecular dynamics (MD) simulation, the binding energy, cohesive energy density (CED), bond length, and mechanical parameters were calculated for 2,6-diamino-3,5-dinitropyrazine-l-oxide (LLM-105) crystal, octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX) crystal, and their co-crystals under different temperatures. Three LLM-105/HMX patterns were constructed to investigate the influence of component proportion on structures and properties of co-crystals, in which the mole ratios of LLM-105 and HMX are 1:1, 1:2, and 2:1. The effect of temperature and components on the stability and sensitivity were investigated as well. The results show that the binding energies, CED and mechanical parameters of all the co-crystals, decrease when the temperature increases from 248 to 398 K, while their maximum N–NO2 bond length (Lmax) increases with rising temperature, indicating that the sensitivities increase and stabilities decrease when temperature rises. At all temperatures, co-crystals exhibit larger CED and shorter bond length than that of single explosive, demonstrating that they are more stable and less sensitive than single crystal, where the stability of co-crystals was ordered as 2:1>1:1>1:2. Moreover, the bulk modulus (K) and shear modulus (G) of co-crystals are lower than that of HMX, conversely, the Cauchy pressure and K/G are higher than that of HMX, implying co-crystals have better ductility. Finally, the 2:1 ratio of LLM-105/HMX co-crystal was identified as the excellent one, owning to the highest binding energy, highest CED, shortest Lmax, and greatest ductility.

Models of LLM-105/HMX and one of the properties

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6

Similar content being viewed by others

References

  1. Zhang CY, Wang XC, Huang H (2008) Pi-stacked interactions in explosive crystals: buffers against external mechanical stimuli. J. Am. Chem. Soc. 130(26):8359–8365

    CAS  PubMed  Google Scholar 

  2. He WD, Zhou G, Wong NB, Tian AM, Long XP (2005) Intramolecular H-bonds in LLM-105 and its derivatives : a DFT study. J. Mol. Struct Theochem 723(1):217–222

    CAS  Google Scholar 

  3. Anniyappan M, Talawar MB, Gore GM, Venugopalan S, Gandhe BR (2006) Synthesis, characterization and thermolysis of 1,1-diamino-2,2-dinitroethylene (FOX-7) and its salts. J. Hazard. Mater. 137(2):812–819

    CAS  PubMed  Google Scholar 

  4. Wei CX, Huang H, Duan XH, Pei CH (2011) Structures and properties prediction of HMX/TATB co-crystal. Propell. Explos. Pyrot 36(5):416–423

    CAS  Google Scholar 

  5. Shen JP, Duan XH, Luo QP, Zhou Y, Bao QL, Ma YJ (2011) Preparation and characterization of a novel cocrystal explosive. Cryst. Growth Des. 11(5):1759–1765

    CAS  Google Scholar 

  6. Li X, Lin QH, Peng JH, Wang BL (2017) Compatibility study between 2,6-diamino-3,5-dinitropyrazine-1-oxide and some high explosives by thermal and nonthermal techniques. J. Therm. Anal. Calorim. 127(3):2225–2231

    CAS  Google Scholar 

  7. Han G, Gou RJ, Ren FD, Zhang SH, Wu CL, Zhu SF (2017) Theoretical investigation into the influence of molar ratio on binding energy, mechanical property and detonation performance of 1,3,5,7-tetranitro-1,3,5,7-tetrazacyclo octane (HMX)/1-methyl-4,5-dinitroimidazole (MDNI) cocrystal explosive. Computational and theoretical Chemistry 1109(27–35

  8. Hang GY, Yu WL, Wang T, Wang JT (2019) Theoretical investigations on structures, stability, energetic performance, sensitivity, and mechanical properties of CL-20/TNT/HMX cocrystal explosives by molecular dynamics simulation. J. Mol. Model. 25(1):10

    PubMed  Google Scholar 

  9. Bolton O, Simke LR, Pagoria PF, Matzger AJ (2012) High power explosive with good sensitivity: a 2:1 cocrystal of CL-20:HMX. Cryst. Growth Des. 12(9):4311

    CAS  Google Scholar 

  10. Gao B, Wang D, Zhang J, Hu Y, Yang G (2014) Facile, continuous and large-scale synthesis of CL-20/HMX nano co-crystals with high-performance by ultrasonic spray-assisted electrostatic adsorption method. J. Mater. Chem. A 2(47):19969–19974

    CAS  Google Scholar 

  11. Sun T, Ji JX, Qiang L, Feng Z, He MX (2014) Comparative study on structure, energetic and mechanical properties of a ε-CL-20/HMX cocrystal and its composite with molecular dynamics simulation. J. Mater. Chem. A 2(34):13898–13904

    CAS  Google Scholar 

  12. Sun SH, Zhang HB, Liu Y, Xu JJ, Huang SL, Wang SM, Sun J (2017) Transitions from separately crystallized CL-20 and HMX to CL-20/HMX cocrystal based on solvent media. Cryst. Growth Des. 18(1):77–84

    Article  Google Scholar 

  13. Ghosh M, Sikder AK, Banerjee S, Gonnade RG (2018) Studies on CL-20/HMX (2: 1) cocrystal: a new preparation method and structural and thermokinetic analysis. Cryst. Growth Des. 18(7):3781–3793

    Article  CAS  Google Scholar 

  14. Wei YJ, Ren FD, Shi WJ, Zhao Q (2016) Theoretical insight into the influences of molecular ratios on stabilities and mechanical properties, solvent effect of HMX/FOX-7 cocrystal explosive. J Energ Mater 34(4):426–439

    Article  CAS  Google Scholar 

  15. Schoeyer HFR, Schnorhk AJ, Korting PAOG, Van PJ, Mul JM, Gadiot GMHJL, Meulenbrugge JJ (1995) High-performance propellants based on hydrazinium nitroformate. J Propul Power 11(4):856–869

    Article  Google Scholar 

  16. Lin H, Zhu SG, Li HZ, Peng XH (2013) Structure and detonation performance of a novel HMX/LLM-105 cocrystal explosive. J. Phys. Org. Chem. 26(11):898–907

    Article  CAS  Google Scholar 

  17. Xiao JJ, Wang WR, Chen J, Ji GF, Zhu W, Xiao HM (2012) Study on structure, sensitivity and mechanical properties of HMX and HMX-based PBXs with molecular dynamics simulation. Comput Theor Chem 999(11):21–27

    Article  CAS  Google Scholar 

  18. Zhou TT, Huang FL (2012) Thermal expansion behaviors and phase transitions of HMX polymorphs via ReaxFF molecular dynamics simulations. Acta Phys. Sin-ch. Ed. 61(24):514–518

    Google Scholar 

  19. Sun H (1998) COMPASS: An ab initio force-field optimized for condensed-phase ApplicationsOverview with details on alkane and benzene compounds. J. Phys. Chem. B 102(38):7338–7364

    Article  CAS  Google Scholar 

  20. Bunte SW, Sun H (2000) Molecular modeling of energetic materials: the parameterization and validation of nitrate esters in the COMPASS force field. J. Phys. Chem. B 104(11):2477–2489

    CAS  Google Scholar 

  21. Xiao JJ, Huang H, Li JS, Zhang H, Ma XF, Xiao HM (2007) A MD simulation study of the coefficients of thermal expansion for β-HMX crystal. Chinese J Energetic Mater 15(6):622–625

    CAS  Google Scholar 

  22. Zhu W, Xiao JJ, Huang XF, Li JS, Xiao HM (2007) Temperature effect on mechanical properties of TATB and TATB/F_(2311) PBX by molecular dynamics simulation. J. Nanjing Univ. Sci. Technol 31(2):243–247

    CAS  Google Scholar 

  23. Wei XF, Xu JJ, Li HZ, Long XP, Zhang CY (2016) Comparative study of experiments and calculations on the polymorphisms of 2,4,6,8,10,12-Hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (CL-20) precipitated by solvent/antisolvent method. J. Phys. Chem. C 120(9):5042–5051

    CAS  Google Scholar 

  24. Guo R, Yang Z, Duan X, Pei C (2019) Molecular dynamics simulations for interfacial interactions and mechanical properties of LLM⁃105 with polymers. Chinese J. Energ Mater 27(8):644–651

    Google Scholar 

  25. Hang GY, Yu WL, Wang T, Wang JT (2019) Theoretical investigations into effects of adulteration crystal defect on properties of CL-20/TNT cocrystal explosive. Comp. Mater. Sci. 156(77–83

  26. Choi CS, Boutin HP (1970) A study of the crystal structure of β-cyclotetramethylene tetranitramine by neutron diffraction. Acta Crystallogr. Section B 26(9):1235–1240

    CAS  Google Scholar 

  27. Liu JJ, Liu ZL, Cheng J (2014) Synthesis, crystal structure catalytic properties of two energetic complexes containing 2, 6-diamino-3, 5-dinitropyrazine-1-oxide. Chinese J. Inorg. Chem. 30(3):696–704

    CAS  Google Scholar 

  28. Wang XJ, Xiao JJ (2017) Molecular dynamics simulation studies of the ε-CL-20/HMX co-crystal-based PBXs with HTPB. Struct. Chem. 28(6):1645–1651

    CAS  Google Scholar 

  29. Shen VK, Mountain RD, Errington JR (2007) Comparative study of the effect of tail corrections on surface tension determined by molecular simulation. J. Phys. Chem. B 111(22):6198–6207

    CAS  PubMed  Google Scholar 

  30. Stavrou E, Manaa MR, Zaug JM, Kuo IFW, Pagoria PF, Bora K, Crowhurst JC, Armstrong MR (2015) The high pressure structure and equation of state of 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) up to 20 GPa: X-ray diffraction measurements and first principles molecular dynamics simulations. J. Chem. Phys. 143(14):1209

    Google Scholar 

  31. Gilardi RD, Butcher RJ (2001) 2,6-Diamino-3,5-dinitro-1,4-pyrazine 1-oxide. Acta Cryst 57(7):657–658

    Google Scholar 

  32. Li BJ, Niu H, Zhang J, Li GP, Luo YJ, Zheng J (2018) Probing the compatibility and interaction of energetic binders based on 3,3-bis(azidomethyl)oxetane with some explosives: thermal, interfacial and simulation studies. Polym. Int. 67(1):132–140

    CAS  Google Scholar 

  33. Xu XJ, Xiao JJ, Huang H, Li JS, Xiao HM (2007) Molecular dynamics simulations on the structures and properties of ε-CL-20-based PBXs. Sci China Ser B: Chem 50(6):737–745

    CAS  Google Scholar 

  34. Herrmannsdörfer D, Gerber P, Heintz T, Herrmann MJ, Klapötke TM (2019) Investigation of crystallisation conditions to produce CL-20/HMX cocrystal for polymer-bonded explosives. Propellants, explosives, pyrotechnics 44(1-12

  35. Wang J, Xiong Y, Li H, Zhang C (2018) Reversible hydrogen transfer as new sensitivity mechanism for energetic materials against external stimuli: a case of the insensitive 2,6-Diamino- 3,5-Dinitropyrazine-1-oxide. J. Phys. Chem. C 122(2):1109–1118

    Article  CAS  Google Scholar 

  36. Politzer P, Murray JS, Lane P, Sjoberg P, Adolph HG (1991) Shock-sensitivity relationships for nitramines and nitroaliphatics. Chem. Phys. Lett. 181(1):78–82

    Article  CAS  Google Scholar 

  37. Ye CC, An Q, Zhang WQ, Goddard WA (2019) Initial decomposition of HMX energetic material from quantum molecular dynamics and the molecular structure transition of β-to δ-HMX. J. Phys. Chem. C 123(14):9232–9236

    Article  Google Scholar 

  38. Liu ZC, Zhu WH, Ji GF, Song KF, Xiao HM (2017) Decomposition mechanisms of α-Octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine nanoparticles at high temperatures. J. Phys. Chem. C 121(14):7728–7740

    Article  Google Scholar 

  39. Stefan G (2010) Semiempirical GGA-type density functional constructed with a long-range dispersion correction. J. Comput. Chem. 27(15):1787–1799

    Google Scholar 

  40. Weiner JH, Statistical mechanics of elasticity, 1983

    Google Scholar 

  41. Nicolò G, Marisol K (2018) The effect of crystal orientation on shock loading of single crystal energetic materials. Comp. Mater. Sci. 155(235–245

  42. Kang J, Butler PB, Baer MR (1992) A thermomechanical analysis of hot spot formation in condensed-phase, energetic materials. Combust. Flame. 89(117-139

  43. Oliger B, Roof B, Cady H (1978) symposium (international) on high dynamic pressures. Paris, France (August 1978)

Download references

Funding

This research did not receive any specific grant from funding agencies in the public, commercial, or not-for-profit sectors. It is appreciated for the Simulation Center of CAEP providing the computational resources.

Author information

Authors and Affiliations

  1. School of Materials Science and Engineering, Chongqing Jiaotong University, Chongqing, 400074, China

    Ming-yao Li & Feng Wang

  2. Key Laboratory of Neutron Physics and Institute of Nuclear Physics and Chemistry, CAEP, Mianyang, 621999, China

    Ming-yao Li, Liang-fei Bai, Ye-bai Shi, Guang-ai Sun & Jian Gong

  3. School of Physics, University of Science and Technology Beijing, Beijing, 100871, China

    Ye-bai Shi & Xin Ju

Authors
  1. Ming-yao Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Liang-fei Bai
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Ye-bai Shi
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Guang-ai Sun
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Feng Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Jian Gong
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Xin Ju
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Feng Wang.

Additional information

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Electronic supplementary material

ESM 1

(DOCX 102 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Li, My., Bai, Lf., Shi, Yb. et al. The influence of temperature and component proportion on stability, sensitivity, and mechanical properties of LLM-105/HMX co-crystals via molecular dynamics simulation. J Mol Model 26, 69 (2020). https://doi.org/10.1007/s00894-020-4329-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s00894-020-4329-4

Keywords

Search

Navigation