First-principle study and Hirshfeld surface analysis on the effect of H2O, NH3 and H2S on structural, electronic, elastic, optical and thermodynamic properties of a novel high-energy crystal 2,4,6-triamino-5-nitropyrimidine-1,3-dioxide
2,4,6-Triamino-5-nitropyrimidine-1,3-dioxide (ICM-102) is a new high-energy crystal which has outstanding combination of performance, effects of three common small molecules H2O, NH3 and H2S on its molecular, crystal and electronic structures, and elastic, optical and thermodynamic properties of the compound were studied by the first-principle calculation and Hirshfeld surface analysis in this work. The results showed that H2O, NH3 and H2S do have significant effects on the structure and property of ICM-102, and different molecules made various influence on all kinds of properties. The low-sensitivity feature of ICM-102 was confirmed, and H2O molecule was found to further increase the stability of ICM-102 crystal obviously by enriching different kinds of close contacts. While the stabilization effect of NH3 and H2S on the ICM-102 was weaker than that of H2O and H2O also improved the density, stiffness, fracture strength and ductility, absorption to purple, blue, green and yellow lights, and thermodynamics parameters of ICM-102, but it decreased the band gap, anisotropy, plasticity, absorption to near ultraviolet and orange, red and infrared lights, and dielectric constant. However, different to H2O, NH3 and H2S reduced stiffness, fracture strength and ductility but increased the band gap of ICM-102. Besides, H2S was found to completely eliminate the region where light cannot be transmitted in the solid crystal ICM-102. This study may be helpful for using small molecules to stabilize the structure and adjust the property of energetic materials.
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The present work was supported by the Natural Science Foundation of Jiangsu (BK20170761, BK20160774), the Natural Science Foundation of Nanjing Institute of Technology (JCYJ201806, CKJA201603), the Jiangsu Key Laboratory Opening Project of Advanced Structural Materials and Application Technology (ASMA201707), Outstanding Scientific and Technological Innovation Team in Colleges and Universities of Jiangsu Province, and Jiangsu Overseas Visiting Scholar Program for University Prominent Young and Middle-aged Teachers and Presidents.
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Conflict of interest
The authors declare no conflicts of interest.
Wang Y, Liu Y, Song S, Yang Z, Qi X, Wang K, Liu Y, Zhang Q, Tian Y (2018) Accelerating the discovery of insensitive high-energy-density materials by a materials genome approach. Nat Commun 9:2444CrossRefGoogle Scholar
Xu Y, Wang Q, Shen C, Lin Q, Wang P, Lu M (2017) A series of energetic metal pentazolate hydrates. Nature 549:78–81CrossRefGoogle Scholar
Zhang C, Sun C, Hu B, Yu C, Lu M (2017) Synthesis and characterization of the pentazolate anion cyclo-N5− in (N5)6(H3O)3(NH4)4Cl. Science 355(6323):374–376CrossRefGoogle Scholar
Xu Y, Lin Q, Wang P, Lu M (2018) Syntheses, crystal structures and properties of a series of 3D metal-inorganic frameworks containing pentazolate anion. Chem-Asian J 13(13):1669–1673CrossRefGoogle Scholar
Xu Y, Tian L, Wang P, Lin Q, Lu M (2019) Hydrogen bonding network: stabilization of the pentazolate anion in two nonmetallic energetic salts. Cryst Growth Des 19(3):1853–1859CrossRefGoogle Scholar
Tappan BC, Brill TB (2003) Thermal decomposition of energetic materials 86 cryogel synthesis of nanocrystalline CL-20 coated with cured nitrocellulose. Propellants Explos Pyrotech 28(5):223–230CrossRefGoogle Scholar
Ding Z, Cao W, Ma X, Hang X, Zhang Y, Xu K, Huang J (2019) Synthesis, structure analysis and thermal behavior of two new complexes: Cu(NH3)4(AFT)2 and Cu(C3H6N2H4)2(AFT)2. J Mol Struct 1175:373–378CrossRefGoogle Scholar
Bogusz R, Rećko J, Magnuszewska P, Lewczuk R (2018) Application of the energetic complex [Cu(TNBI)(NH3)2(H2O)] in heterogeneous solid rocket propellants. Cent Eur J Energ Mater 15(2):391–402CrossRefGoogle Scholar
Wu BD, Yang L, Wang SW, Zhang TL, Zhang JG, Zhou ZN, Yu KB (2011) Preparation, crystal structure, thermal decomposition, and explosive properties of a novel energetic compound [Zn(N2H4)2(N3)2]n: a new high-nitrogen material (N = 65.60%). Z Anorg Allg Chem 637(3–4):450–455CrossRefGoogle Scholar
Liu Z, Zhang T, Zhang J, Wang S (2008) Studies on three-dimensional coordination polymer [Cd2(N2H4)2(N3)4]n: crystal structure, thermal decomposition mechanism and explosive properties. J Hazard Mater 154(1–3):832–838CrossRefGoogle Scholar
Luo JH, Chen LY, Nguyen DN, Guo D, An Q, Cheng MJ (2018) Dual functions of water in stabilizing metal-pentazolate hydrates [M(N5)2(H2O)4]·4H2O (M = Mn, Fe Co, and Zn) high-energy-density materials. J Phys Chem C 122(37):21192–21201CrossRefGoogle Scholar
Zhang L, Chen L, Wang C, Wu JY (2013) Molecular dynamics study of the effect of H2O on the thermal decomposition of α Phase CL-20. Acta Phys-Chim Sin 29(6):1145–1153Google Scholar
Clark SJ, Segall MD, Pickard CJ, Hasnip PJ, Probert MI, Refson K, Payne MC (2005) First principles methods using CASTEP. Z Kristallogr 220:567–570Google Scholar
Hamann DR, Schlüter M, Chiang C (1979) Norm-conserving pseudopotentials. Phys Rev Lett 43(20):1494CrossRefGoogle Scholar
Tkatchenko A, Scheffler M (2009) Accurate molecular van der Waals interactions from ground-state electron density and free-atom reference data. Phys Rev Lett 102(7):073005CrossRefGoogle Scholar
Grimme S (2006) Semiempirical GGA-type density functional constructed with a long-range dispersion correction. J Comput Chem 27(15):1787–1799CrossRefGoogle Scholar
Fischer TH, Almlof J (1992) General methods for geometry and wave function optimization. J Phys Chem 96(24):9768–9774CrossRefGoogle Scholar
Wolff S, Grimwood D, McKinnon J, Turner M, Jayatilaka D, Spackman M (2012) Crystalexplorer (version 3.0). University of Western Australia, CrawleyGoogle Scholar
Zhang W, Zhang J, Deng M, Qi X, Nie F, Zhang Q (2017) A promising high-energy-density material. Nat Commun 8:181CrossRefGoogle Scholar
Tian B, Xiong Y, Chen L, Zhang C (2018) Relationship between the crystal packing and impact sensitivity of energetic materials. CrystEngComm 20(6):837–848CrossRefGoogle Scholar
Ma Y, Meng L, Li H, Zhang C (2017) Enhancing intermolecular interactions and their anisotropy to build low-impact-sensitivity energetic crystals. CrystEngComm 19(23):3145–3155CrossRefGoogle Scholar
Born M, Huang K (1982) Dynamical Theory and Experiment I. Springer-Verlag, BerlinGoogle Scholar
Davidson AJ, Dias RP, Dattelbaum DM, Yoo CS (2011) “Stubborn” triaminotrinitrobenzene: unusually high chemical stability of a molecular solid to 150 GPa. J Chem Phys 135(17):174507CrossRefGoogle Scholar
Pugh SF (1954) XCII. Relations between the elastic moduli and the plastic properties of polycrystalline pure metals. Philos Mag 45(367):823–843CrossRefGoogle Scholar
Saha S, Sinha TP (2000) Electronic structure, chemical bonding, and optical properties of paraelectric BaTiO3. Phys Rev B 62(13):8828CrossRefGoogle Scholar
Zhu W, Xiao J, Xiao H (2006) Comparative first-principles study of structural and optical properties of alkali metal azides. J Phys Chem B 110(20):9856–9862CrossRefGoogle Scholar