First-principle calculations of the electronic, vibrational, and thermodynamic properties of nitrogen-rich salt of 3,6-dinitramino-1,2,4,5-tetrazine [(NH4)2(DNAT)]

IF 2.1 4区 化学 Q4 BIOCHEMISTRY & MOLECULAR BIOLOGY
Si-Jia Lei, Qi-Jun Liu, Fu-Sheng Liu, Zheng-Tang Liu, Wen-Shuo Yuan
{"title":"First-principle calculations of the electronic, vibrational, and thermodynamic properties of nitrogen-rich salt of 3,6-dinitramino-1,2,4,5-tetrazine [(NH4)2(DNAT)]","authors":"Si-Jia Lei,&nbsp;Qi-Jun Liu,&nbsp;Fu-Sheng Liu,&nbsp;Zheng-Tang Liu,&nbsp;Wen-Shuo Yuan","doi":"10.1007/s00894-024-06098-6","DOIUrl":null,"url":null,"abstract":"<div><h3>Context</h3><p>Energy-containing materials such as explosives have attracted considerable interest recently. In the field of high-energy materials, tetrazine and its derivatives can largely meet the requirements of high nitrogen content and oxygen balance. Nitrogen-rich energetic salts are important research subjects. Nitrogen-rich salt of 3,6-dinitramino-1,2,4,5-tetrazine is a high-energy nitrogen-rich material, but there are few related studies. This paper systematically studies the crystal structure and electronic, vibrational, and thermodynamic properties of (NH<sub>4</sub>)<sub>2</sub>(DNAT). The lattice parameters of (NH<sub>4</sub>)<sub>2</sub>(DNAT) are observed to align well with the experimental values. The properties of electrons are analyzed by band structure and density of states (DOS). The phonon dispersion curves indicate that the compound is dynamically stable. The vibrational modes of bonds and chemical groups are described in detail, and the peaks in the Raman and infrared spectra are assigned to different vibration modes. Based on the vibration characteristics, thermodynamic properties such as enthalpy (<i>H</i>), Helmholtz free energy (<i>F</i>), entropy (<i>S</i>), Gibbs free energy (<i>G</i>), constant volume heat capacity (<i>C</i><sub><i>V</i></sub>), and Debye temperature (Θ) are analyzed. This article can pave the way for subsequent work or provide data support to other researchers, promoting further research.</p><h3>Methods</h3><p>In this study, we utilized the density functional theory (DFT) for our calculations. The exchange–correlation potential and van der Waals interactions were characterized based on the GGA-PBE + G function calculation. We obtained Brillouin zone integrals using Monkhorst–Pack <i>k</i>-point grids, with the <i>k</i>-point of the Brillouin zone set to a 2 × 2 × 2 grid. During the self-consistent field operation, we set the total energy convergence tolerance to 5 × 10<sup>−6</sup> eV per atom. The cut-off energy for the calculation was established at 830 eV. Additionally, the states of H (1s<sup>1</sup>), C (2s<sup>2</sup> 2p<sup>2</sup>), N (2s<sup>2</sup> 2p<sup>3</sup>), and O (2s<sup>2</sup> 2p<sup>4</sup>) were treated as valence electrons in our study.</p></div>","PeriodicalId":651,"journal":{"name":"Journal of Molecular Modeling","volume":null,"pages":null},"PeriodicalIF":2.1000,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Molecular Modeling","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s00894-024-06098-6","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"BIOCHEMISTRY & MOLECULAR BIOLOGY","Score":null,"Total":0}
引用次数: 0

Abstract

Context

Energy-containing materials such as explosives have attracted considerable interest recently. In the field of high-energy materials, tetrazine and its derivatives can largely meet the requirements of high nitrogen content and oxygen balance. Nitrogen-rich energetic salts are important research subjects. Nitrogen-rich salt of 3,6-dinitramino-1,2,4,5-tetrazine is a high-energy nitrogen-rich material, but there are few related studies. This paper systematically studies the crystal structure and electronic, vibrational, and thermodynamic properties of (NH4)2(DNAT). The lattice parameters of (NH4)2(DNAT) are observed to align well with the experimental values. The properties of electrons are analyzed by band structure and density of states (DOS). The phonon dispersion curves indicate that the compound is dynamically stable. The vibrational modes of bonds and chemical groups are described in detail, and the peaks in the Raman and infrared spectra are assigned to different vibration modes. Based on the vibration characteristics, thermodynamic properties such as enthalpy (H), Helmholtz free energy (F), entropy (S), Gibbs free energy (G), constant volume heat capacity (CV), and Debye temperature (Θ) are analyzed. This article can pave the way for subsequent work or provide data support to other researchers, promoting further research.

Methods

In this study, we utilized the density functional theory (DFT) for our calculations. The exchange–correlation potential and van der Waals interactions were characterized based on the GGA-PBE + G function calculation. We obtained Brillouin zone integrals using Monkhorst–Pack k-point grids, with the k-point of the Brillouin zone set to a 2 × 2 × 2 grid. During the self-consistent field operation, we set the total energy convergence tolerance to 5 × 10−6 eV per atom. The cut-off energy for the calculation was established at 830 eV. Additionally, the states of H (1s1), C (2s2 2p2), N (2s2 2p3), and O (2s2 2p4) were treated as valence electrons in our study.

Abstract Image

3,6- 二硝氨基-1,2,4,5-四嗪富氮盐 [(NH4)2(DNAT)]的电子、振动和热力学性质的第一性原理计算。
背景:炸药等含能材料近来引起了广泛关注。在高能材料领域,四嗪及其衍生物在很大程度上可以满足高氮含量和氧平衡的要求。富氮高能盐是重要的研究课题。3,6-二硝氨基-1,2,4,5-四嗪富氮盐是一种高能富氮材料,但相关研究较少。本文系统研究了(NH4)2(DNAT)的晶体结构及电子、振动和热力学性质。据观察,(NH4)2(DNAT) 的晶格参数与实验值十分吻合。通过能带结构和状态密度(DOS)分析了电子的特性。声子频散曲线表明该化合物具有动态稳定性。详细描述了键和化学基团的振动模式,并将拉曼光谱和红外光谱中的峰值归属于不同的振动模式。根据振动特征,分析了焓(H)、亥姆霍兹自由能(F)、熵(S)、吉布斯自由能(G)、恒定体积热容(CV)和德拜温度(Θ)等热力学性质。本文可为后续工作铺平道路,或为其他研究人员提供数据支持,促进进一步研究:本研究采用密度泛函理论(DFT)进行计算。基于 GGA-PBE + G 函数计算表征了交换相关势和范德华相互作用。我们使用 Monkhorst-Pack k 点网格获得了布里渊区积分,布里渊区的 k 点设置为 2 × 2 × 2 网格。在自洽场操作过程中,我们将每个原子的总能量收敛容限设定为 5 × 10-6 eV。计算的截止能量设定为 830 eV。此外,在我们的研究中,H(1s1)、C(2s2 2p2)、N(2s2 2p3)和 O(2s2 2p4)的状态被视为价电子。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Journal of Molecular Modeling
Journal of Molecular Modeling 化学-化学综合
CiteScore
3.50
自引率
4.50%
发文量
362
审稿时长
2.9 months
期刊介绍: The Journal of Molecular Modeling focuses on "hardcore" modeling, publishing high-quality research and reports. Founded in 1995 as a purely electronic journal, it has adapted its format to include a full-color print edition, and adjusted its aims and scope fit the fast-changing field of molecular modeling, with a particular focus on three-dimensional modeling. Today, the journal covers all aspects of molecular modeling including life science modeling; materials modeling; new methods; and computational chemistry. Topics include computer-aided molecular design; rational drug design, de novo ligand design, receptor modeling and docking; cheminformatics, data analysis, visualization and mining; computational medicinal chemistry; homology modeling; simulation of peptides, DNA and other biopolymers; quantitative structure-activity relationships (QSAR) and ADME-modeling; modeling of biological reaction mechanisms; and combined experimental and computational studies in which calculations play a major role.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信