Theoretical predict structure and property of the novel CL-20/2,4-DNI cocrystal by systematic search approach
Theoretical predict structure and property of the novel CL-20/2,4-DNI cocrystal by systematic search approach
复制标题
DOI：
10.1016/j.dt.2021.03.027
复制
发表时间：
2022-06-01
影响因子：
5.1
通讯作者：
Li, Wei
中科院分区：
文献类型：
--
作者：
Li, Hao-jie;Liu, Jian-chao;Li, Wei
共混结合了高能量和含能分子间不敏感的优点，获得了性能良好的能量学。然而，如何准确、快速地获得超分子配体，用于预测共晶的结构和性质，仍然是一个具有挑战性的问题。本研究提出了一种预测CL-20/2，4-DNI共晶的有效系统搜索方法，即2，4-DNI以1：1的化学计量比围绕CL-20旋转，并遵循特定的规则（氢键长度：2.2-3.0 A;搜索半径：6.5 A;氢键数目：1-3）。将量子化学与分子力学相结合，得到了8种可能的超分子电子。晶体结构预测表明，共晶中存在P21/c、P212121、Pbca和Pna 21四种结构，CL-20/2，4-DNI共晶可能为P21/c，对应的晶胞参数为Z = 4，a = 8.28 A，B = 12.17 A，c = 20.42 A，a = 90 °，β = 96.94 °，g = 90度，γ =1.9353 g/cm（3）。为了进一步研究CL-20/2，4-DNI共晶的分子间相互作用，采用了分子间相互作用能、静电势、态密度、Hirshfeld表面分析等一系列理论分析方法。C-H/O氢键被证明是共晶形成的主要驱动力。CL-20/2，4-DNI共晶的力学性能和爆轰性能表明，该共晶具有较好的延展性和优良的爆轰性能（9257 m/s，39.27 GPa），是一种很有前途的含能材料。将预测的共晶结构与实验结果进行了比较，验证了系统搜索方法的准确性。实验结果与预测结果的误差小于8.8%，表明系统搜索方法具有极高的可靠性和准确性。系统搜索方法可以成为一种有效搜索超分子配体和结构鉴定的新策略，并有可能通过理论设计促进含能共晶的发展。(C)2021中国园艺学会。Elsevier B. V.代表KeAi Communications Co. Ltd.提供出版服务。
Cocrystallization integrates the merits of high energy and insensitivity between energetic molecules to obtain energetics with satisfying performance. However, how to obtain supramolecular synthons accurately and rapidly for predicting the structure and property of cocrystal remains a challenging problem. In this research, an efficient systematic search approach to predict CL-20/2,4-DNI cocrystal has been proposed that 2,4-DNI revolves around CL-20 with a stoichiometric ratio of 1:1 in accordance with the specified rules (hydrogen bond length: 2.2-3.0 A; search radius: 6.5 A; the number of hydrogen bond: 1-3). Eight possible supramolecular synthons were obtained by combining quantum chemistry with molecular mechanics. Crystal structure prediction indicated that there are four structures in cocrystal, namely P21/c, P212121, Pbca and Pna21, and CL-20/2,4-DNI cocrystal is likely to be P21/c and the corresponding cell parameters are Z = 4, a = 8.28 A, b = 12.17 A, c = 20.42 A, a = 90 degrees, beta = 96.94 degrees, g = 90 degrees, and gamma =1.9353 g/cm(3). To further study the intermolecular interaction of CL-20/2,4-DNI cocrystal, a series of theoretical analyses were employed including intermolecular interaction energy, electrostatic potential (ESP), Density of State (DOS), Hirshfeld surface analysis. The C-H/O hydrogen bonds are demonstrated as the predominant driving forces in the cocrystal formation. The mechanical properties and detonation properties of CL-20/2,4-DNI cocrystal implies that the cocrystal shows better ductility and excellent detonation performances (9257 m/s, 39.27 GPa) and can serve as a promising energetic material. Cocrystal structure predicted was compared with the experimental one to verify the accuracy of systematic search approach. There is a less than 8.8% error between experiment and predict results, indicating the systematic search approach has extremely high reliability and accuracy. The systematic search approach can be a new strategy to search supramolecular synthons and identify structures effectively and does have the potential to promote the development of energetic cocrystal by theoretical design. (C) 2021 China Ordnance Society. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co. Ltd.