高压下硝酸肼结构演化的中远红外光谱和第一性原理计算研究

曾阳阳; 朱刚贝; 王文涛; 白莎; 郑朝阳; 于国洋; 杨延强

doi:10.11858/gywlxb.20230804

高压下硝酸肼结构演化的中远红外光谱和第一性原理计算研究

doi: 10.11858/gywlxb.20230804

1.
中国工程物理研究院流体物理研究所, 四川绵阳　621999
2.
中国科学院大连化学物理研究所, 辽宁大连　116023
3.
西北大学化学与材料学院, 陕西西安　710127

基金项目: 国家自然科学基金（U2030113）；冲击波物理与爆轰物理全国重点实验室基金（2021JCJQLB05712）；中国科学院重点实验室基金（CXJJ-22S034）

详细信息

作者简介:
曾阳阳（1983－），男，博士，助理研究员，主要从事含能材料高温高压理论与实验研究. E-mail：caep2012@163.com

通讯作者:
于国洋（1982－），男，博士，副研究员，主要从事含能材料超快光谱实验研究. E-mail：yuguoyang@caep.cn

中图分类号: O521.2
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出版历程
- 收稿日期: 2023-12-06
- 修回日期: 2023-12-22
- 网络出版日期: 2024-03-14
- 刊出日期: 2024-06-03

Mid- and Far-Infrared Spectroscopic and First-Principles Computational Study of the Structural Evolution of Hydrazine Nitrate under High Pressure

1.
Institute of Fluid Physics, China Academy of Engineering Physics, Mianyang 621999, Sichuan, China
2.
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
3.
College of Chemistry and Materials Science, Northwest University, Xi’an 710127, Shaanxi, China

摘要

摘要: 对于含能材料，6 THz（200 cm⁻¹）以内的晶格振动模式对外部压力变化引起的结构变化非常敏感，因此，中远红外振动光谱可作为研究含能材料高压相变的有力手段。利用基于空气等离子体产生的中远红外超宽带光谱技术，结合金刚石对顶砧，获得了含能材料硝酸肼的高压振动光谱。同时，采用第一性原理方法，计算了硝酸肼的晶体结构和红外光谱，在此基础上对分子间的相互作用进行了分析。综合实验和计算结果，揭示了压力作用下分子间氢键和范德瓦尔斯相互作用对材料中分子结构和堆垛变化的影响，获得了硝酸肼的相变过程。
- 硝酸肼 /
- 中远红外光谱 /
- 第一性原理计算 /
- 高压 /
- 相变
Abstract: For energetic materials, the lattice vibration modes in the 6 THz (200 cm⁻¹) range are very sensitive to structural changes caused by external temperature and pressure changes. Therefore, mid- and far-infrared vibrational spectroscopy can be used as a powerful tool to study high-pressure phase transitions in these materials. We have obtained high-pressure vibrational spectra of hydrazine nitrate, using mid- and far-infrared ultra-broadband spectroscopy, whose broadband was generated by air plasma, combined with a diamond anvil cell (DAC). The crystal structure of hydrazine nitrate, as well as the infrared spectrum, were calculated by using the first principle method. Based on the calculation, the intermolecular interactions were analyzed. Combined with the experimental results, it was revealed that the structural changes under pressure alter the strength of intermolecular hydrogen bonds and van der Waals interactions, which in turn affects the low-frequency vibrational modes. And by analyzing the vibrational spectra, we observed the phase transition process of hydrazine nitrate.
- hydrazine nitrate /
- mid- and far- infrared spectra /
- first principle computation /
- high pressure /
- phase transition

HTML全文

图 1 α相HN晶胞结构^[8]（灰色球为氢原子，红色球为氧原子，蓝色球为氮原子，绿色虚线表示分子间氢键）

Figure 1. Crystal cell structure of α-HN^[8] (The gray balls represent H atoms, the red balls represent O atoms, the blue balls represent N atoms, and the green dashed lines represent intermolecular hydrogen bonds.)

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图 2 α-HN 2×2×2超胞结构中弱相互作用的IRI图示（灰色球为氢原子，红色球为氧原子，蓝色球为氮原子）

Figure 2. IRI representation of weak interactions of α-HN 2×2×2 supercell (The gray balls represent H atoms, the red balls represent O atoms, and the blue balls represent N atoms.)

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图 3 HN的高压红外吸收光谱：(a) 纯HN的远红外谱，(b) HN与KBr混合的中红外谱

Figure 3. High pressure infrared absorption spectra of HN: (a) far-infrared spectra of pure HN; (b) mid-infrared spectra of HN mixed with KBr

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图 4 硝酸基团平动振动模式的吸收峰随压力的变化规律

Figure 4. Effect of pressure on infrared absorption spectra shifts of nitrate libration modes

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图 5 肼离子平动振动模式对应的吸收峰随压力的变化规律

Figure 5. Effect of pressure on infrared absorption spectra shifts of hydrazine libration modes

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表 1 HN晶格参数的计算结果与实验结果比较

Table 1. Calculated crystal lattice parameters of HN compared with experimental data

Method	a/Å	b/Å	c/Å	β/(°)	V/Å³
Expt.^[7]	11.23	11.73	5.17	90.00	681.03
Expt.^[8]	7.9649	5.6569	8.1221	91.34	365.85
Expt.^[9]	8.0150	5.7250	8.1560	92.30	374.00
Calc. (this work)	7.9041	5.7271	8.1447	89.17	368.65
δ(Expt.^[8])/%	−0.8	1.2	0.3	−2.4	0.8
δ(Expt.^[9])/%	−1.4	0.04	−0.1	−3.4	−1.4

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