Study of elastic anisotropy for 1, 3, 5-trinitro-1, 3, 5-triazacyclohexane by supramolecular structural unit

Wei Fu-Jing; Zhang Wei-Bin; Dong Chuang; Chen Hua

doi:10.7498/aps.72.20221615

Abstract

The relation between elastic property and crystal structure provides a foundation for designing new materials with desired properties and understanding the chemical decomposition and explosion of energetic materials. The supramolecular structural unit is proposed as the smallest chemical unit to quantitatively characterize the elastic anisotropy of 1, 3, 5-trinitro-1, 3, 5-triazacyclohexane (RDX). The supramolecular structural unit refers to the nearest-neighbor coordination polyhedron of one molecule. The supramolecular structural unit of RDX is composed of 15 molecules, and analyzed by the total molecular number density and the density of intermolecular interactions. The elastic modulus model is established on the assumption that 1) the RDX molecule is of sphere and rigid-body; 2) the intermolecular interaction is regarded as a linear spring, i.e. it is described by a bond-spring model; 3) the molecules are close-packed in the series mode. The elastic modulus model based on the supramolecular structural unit demonstrates that the elastic modulus is intrinsically determined by the total molecular number, the equilibrium distance of the molecular pair, the intermolecular force constant, and the angle between the intermolecular non-bonding interaction and the normal to crystal face. The intermolecular force constant is calculated as the second derivative of the intermolecular interaction with respect to the equilibrium centroid distance. The intermolecular interaction is expressed as the summation of van der Waals and electrostatic interactions calculated by COMPASS (condensed-phase optimized molecular potentials for atomistic simulation studies) II forcefield. The calculated elastic moduli are 21.7, 17.1, 20.1, 19.1, and 15.3 GPa for RDX (100), (010), (001), (210), and (021) crystal faces, respectively. The calculation results are consistent with the theoretical values computed by the density functional theory. Excluding RDX(001), the calculated elastic moduli accord with the experimental results measured by the resonant ultrasound spectroscopy (RUS), impulsive stimulated thermal scattering, Brillouin spectroscopy, and nanoindentation methods. The theoretical value (20.1 GPa) of RDX(001) overestimates the experimental values in a range of 15.9–16.6 GPa. The reason can be attributed to the rigid-body approximation for flexible molecules, in which are ignored the motion and deformation of the ring and NO₂ groups when the external loads are applied to RDX(001). The results suggest that the supramolecular structural unit can be the smallest chemical unit to quantitatively characterize the elastic anisotropy of RDX and the elastic anisotropy is mainly due to the angle between the intermolecular interaction and the normal to crystal face.

Keywords:

1, 3, 5-trinitro-1, 3, 5-triazacyclohexane /
supramolecular structural unit /
elastic anisotropy

Authors and contacts

1.
School of Material Science and Engineering, Dalian University of Technology, Dalian 116024, China
2.
Institute of Chemical Materials, China Academy of Engineering Physics, Mianyang 621900, China

Corresponding author: Dong Chuang, dong@dlut.edu.cn ; Chen Hua, chenhua9@caep.cn

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References

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Cited By

图 1 弹性模量模型示意图　(a) 键-弹簧模型; (b) RDX的超分子结构单元; (c) 未变形 (即平衡状态)时的分子对构型; (d) 外界载荷作用下, 发生形变后的分子对构型. 其中, 黄色分子代表RDX超分子结构单元的中心分子

Figure 1. Schematic diagram of the elastic modulus model: (a) Bond-spring model; (b) the supramolecular structural unit of RDX; (c) molecular pair in the un-deformed (i.e., equilibrium position) configuration; (d) molecular pair in the deformed configuration under the external loads. The yellow molecule represents the central molecule of the supramolecular structural unit of RDX.

DownLoad: Full-Size Img PowerPoint

图 2 (a) 5×5×5的RDX超晶胞, 其中A, B, O/C代表超晶胞的晶轴; (b) RDX的总分子数密度和分子间非键能密度曲线

Figure 2. (a) The 5×5×5 supercell structure of RDX, where A, B, and O/C refer to the crystal axis of the supercell; (b) the radial total molecular number density and the density of intermolecular interaction curves of RDX.

DownLoad: Full-Size Img PowerPoint

图 3 (a) RDX的超分子结构单元, 其中黄色分子为中心分子; (b) RDX超分子结构单元内不同分子对的分子间非键能曲线

Figure 3. (a) Supramolecular structural unit of RDX, and the yellow molecule represents the central molecule; (b) the intermolecular interaction curves of molecular pairs extracted from the supramolecular structural unit of RDX.

DownLoad: Full-Size Img PowerPoint

表 1 分子间非键能曲线确定的平衡距离R₀^[12]、分子间作用能E_low和分子间力常数k, 以及真实晶胞中的平衡距离r₀和分子间非键能E₀^[37]

Table 1. Equilibrium distance R₀^[12], the lowest intermolecular interaction E_low, and intermolecular force constant k obtained by intermolecular non-bonded interaction curves, the equilibrium distance r₀ and intermolecular non-bonded interaction E₀^[37] in the actual crystal lattice.

r₀/nm	R₀/nm^[12]	R₀/nm	E_low/(kcal·mol^–1)	E₀/(kcal·mol^–1)^[37]	k/(N·m^–1)
0.4415044	0.42603	0.428	–6.86	–6.25	19.985
0.6447523	0.63385	0.660	–1.57	–2.68	7.211
0.6550915	0.64700	0.640	–3.22	–2.68	6.729
0.6944433	0.68725	0.691	–3.94	–3.35	10.677
0.7291993	0.70889	0.737	–4.46	–5.58	9.546
0.7292055	—	0.710	–6.39	–5.80	18.522
0.8144825	0.76922	0.760	–2.28	—	5.045
0.8146958	—	0.754	–4.76	—	13.018

DownLoad: CSV

表 2 RDX超分子结构单元内分子对的平衡位置R₀、分子间非键能与晶面法线(hkl )的夹角余弦值cosθ和分子间力常数k

Table 2. Equilibrium distance R₀ of the molecular pair, the cosine value of the angle cosθ between the intermolecular non-bonded interactions and the normal to (hkl ), and the intermolecular force constants k within the RDX supramolecular structural unit.

R₀/nm	k/(N·m^–1)	cosθ (021)	cosθ (210)	cosθ (001)	cosθ (100)	cosθ (010)
0.428	19.985	0.0676	–0.1388	–0.7174	–0.9491	0
0.660	7.211	–0.0622	–0.3031	0.8305	0.9491	0
0.660	7.211	–0.8999	–0.3031	–0.8305	–0.2645	0.2695
0.640	6.729	–0.5944	–0.7566	0.3339	–0.4880	0.4972
0.640	6.729	0.9312	0.2048	0.3339	0.6084	–0.7936
0.691	10.677	0.1588	–0.7963	0.315	0.6084	0.7936
0.691	10.677	0.1588	0.7963	0.315	0	–0.5571
0.737	9.546	–0.6853	0.0786	0	0	–0.5571
0.737	9.546	0.6853	0.9423	0	0.6084	0.3011
0.710	18.522	0.6303	0.6743	0.7343	0.6084	0.3011
0.710	18.522	–0.1103	0.6743	–0.7343	–0.8090	–0.4409
0.760	5.045	0.6997	–0.0752	0.9260	0.8090	–0.4409
0.754	13.018	–0.5768	–0.9186	–0.3888	–0.3289	–0.8834
0.754	13.018	–0.5768	0.4389	–0.3888	–0.3289	0.8834

DownLoad: CSV

表 3 由不同实验方法和理论计算得到的RDX多个晶面的弹性模量. 其中, E_RUS, E_ISTS, E_Bri和E_nano分别代表由超声共振谱、脉冲激热散射法、布里渊散射法和纳米压痕法实验测定的弹性模量值; E_DFT和E_cal为密度泛函理论和超分子结构单元法的计算值

Table 3. Elastic moduli of multiple crystal faces for RDX are obtained by experimental and theoretical calculations. E_RUS, E_ISTS, E_Bri, and E_nano refer to the elastic moduli experimentally measured by resonant ultrasound spectroscopy, impulsive stimulated thermal scattering, Brillouin spectroscopy, and nanoindentation approaches, respectively. E_DFT and E_cal represent the elastic moduli theoretically calculated by the density functional theory and the supramolecular structural unit, respectively.

RDX	E_RUS/GPa^[7]	E_ISTS/GPa^[8]	E_Bri/GPa^[9]	E_nano/GPa^[5]	E_DFT/GPa^[15]	E_cal/GPa
(100)	21.5	21.0	21.5	—	25.7	21.7
(010)	17.2	16.4	16.3	—	18.8	17.1
(001)	16.6	15.9	16.2	16.2	20.5	20.1
(210)	20.5	20.0	20.3	21.0	22.8	19.1
(021)	15.5	14.9	14.9	18.2	16.3	15.3

DownLoad: CSV

map

[1]	Mishra M K, Sanphui P, Ramamurty U, Desiraju G 2014 Cryst. Growth. Des. 14 3054 Google Scholar
[2]	Sunil S L, Kiran M, Ramamurty U, Varughese S 2018 Chem. Eur. J. 25 526 Google Scholar
[3]	Armstrong R, Elban W L 2006 Mater. Sci. Technol. 22 381 Google Scholar
[4]	王鹏举, 范俊宇, 苏艳, 赵纪军 2020 69 238702 Google Scholar Wang P J, Fan J Y, Su Y, Zhao J J 2020 Acta Phys. Sin. 69 238702 Google Scholar
[5]	Ramos K J, Hooks D E, Bahr D F 2009 Philos. Mag. 89 2381 Google Scholar
[6]	Haussühl S 2001 Z. Krist-Cryst. Mater. 216 339 Google Scholar
[7]	Schwarz R, Hooks D, Dick J, Archuleta J, Martinez A 2005 J. Appl. Phys. 98 056106 Google Scholar
[8]	Sun B, Winey J, Hemmi N, Dreger Z, Zimmerman K, Gupta Y, Torchinsky D H, Nelson K A 2008 J. Appl. Phys. 104 073517 Google Scholar
[9]	Bolme C A, Ramos K J 2014 J. Appl. Phys. 116 77 Google Scholar
[10]	Weingarten N S, Sausa R C 2015 J. Phys. Chem. A 119 9338 Google Scholar
[11]	Taylor D E 2014 J. Appl. Phys. 116 053513 Google Scholar
[12]	Liu J, Zeng Q, Zhang Y L, Zhang C Y 2016 J. Phys. Chem. C 120 15198 Google Scholar
[13]	Shi Y B, Bai L F, Li J H, Sun G A, Gong J, Ju X 2019 J. Mol. Model. 25 299 Google Scholar
[14]	Zhu S H, Qin H, Zeng W, Liu F S, Tang B, Liu Q J, Li R X, Gan Y D 2020 Philos Mag. 100 1015 Google Scholar
[15]	Fan J Y, Su Y, Zhang Q Y, Zhao J J 2019 Comp. Mater. Sci. 161 379 Google Scholar
[16]	Hang G Y, Yu W L, Wang T, Wang J T, Li Z 2017 J. Mol. Struct. 1141 577 Google Scholar
[17]	Sun H J 1998 J. Phys. Chem. B 102 7338 Google Scholar
[18]	Spackman P R, Grosjean A, Thomas S P, Karothu D P, Naumov P, Spackman M A 2022 Angew. Chem. Int. Ed. 61 e202110716 Google Scholar
[19]	Day G M, Price S L, Leslie M 2001 Cryst. Growth. Des. 1 13 Google Scholar
[20]	Zhang S, Wang Q, Dong C 2021 J. Mater. Inf. 1 8 Google Scholar
[21]	Dong D D, Zhang S, Wang Z J, Dong C, Haeussler P 2016 Mater. Design. 96 115 Google Scholar
[22]	Wang Z R, Qiang J B, Wang Y M, Wang Q, Dong D D, Dong C 2016 Acta Mater. 111 366 Google Scholar
[23]	Ma Y, Wang Q, Jiang B B, Li C L, Hao J M, Li X N, Dong C, Nieh T G 2018 Acta Mater. 147 213 Google Scholar
[24]	Dong D D, Cao Z M, Han G, Dong C 2021 AIP. Adv. 11 035140 Google Scholar
[25]	Chen H, Luo L J, Qiang J B, Wang Y M, Dong C 2014 Philos. Mag. 94 1463 Google Scholar
[26]	Friedel J 1958 II Nuovo. Cimento. 7 287 Google Scholar
[27]	Dong C, Wang Z J, Zhang S, Wang Y M 2019 Int. Mater. Rev. 65 286 Google Scholar
[28]	Li T, Morris K R, Park K 2000 J. Phys. Chem. B 104 2019 Google Scholar
[29]	Bandyopadhya R, Grant D 2002 Pharm. Res. 19 491 Google Scholar
[30]	Zaccone A, Lattuada M, Wu H, Morbidelli M 2007 J. Chem. Phys. 127 174512 Google Scholar
[31]	Weiner J H 1984 J. Appl. Mech. 51 707 Google Scholar
[32]	Gao C, Yang L, Zeng Y, Wang X, Zhang C, Dai R, Wang Z, Zheng X, Zhang Z 2017 J. Phys. Chem. C 121 17586 Google Scholar
[33]	Accelrys. Materials Studio Release Notes, Release 5.5, Accelrys Software. Inc. San Diego 2010, https://www.3ds.com/products-services/biovia/ [2022-8-10]
[34]	Desiraju G R 2013 J. Am. Chem. Soc. 135 9952 Google Scholar
[35]	Bu R P, Xiong Y, Wei X F, Li H Z, Zhang C Y 2019 Cryst. Growth. Des. 19 5981 Google Scholar
[36]	Konovalova I S, Shishkina S V, Bani-Khaled G, Muzyka E N, Boyko A N 2019 Cryst. Eng. Comm. 21 2908 Google Scholar
[37]	Eckhardt C J, Gavezzotti A 2007 J. Phys. Chem. B 111 3430 Google Scholar
[38]	Peng Q, Rahul, Wang G Y, Liu G R, Grimme S, De S 2015 J. Phys. Chem. B 119 5896 Google Scholar

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