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沿面放电是破坏绝缘系统性能的原因之一. 聚酰亚胺常用于高频电力设备的气-固绝缘中, 为此利用密度泛函理论, 从原子分子层面探讨了在外电场下聚酰亚胺及其受极性基团OH–影响后的单分子链结构、能级与态密度、静电势、激发态等微观参数对陷阱形成以及沿面放电的影响. 结果表明, 外电场下, 聚酰亚胺分子结构卷曲, 偶极矩增加, 易于积聚电荷形成空间电荷中心, 尤属引入极性基团OH–后变化较明显; 聚酰亚胺分子中, 苯环区域形成空穴陷阱, 酰亚胺环区域形成电子陷阱, 且电子陷阱能级的数量较多, 其中空间电荷陷阱深度随外电场的增加逐渐变深; 聚酰亚胺分子在引入极性基团OH–后激发能降低, 使得分子内部的电子变得容易被激发; 电子与空穴的空间分离度随电场增加而降低, 利于空穴与电子的复合而发出光子.Surface discharge is one of the reasons for insulation failure. Polyimide (PI) is used in gas-solid insulation of high-frequency electric power equipment. Therefore, based on density functional theory, the effects of single molecular chain structure, energy level, density of states, electrostatic potential, excited state and other micro parameters under external electric field on trap formation and surface discharge of both PI and polar- group- OH– affected PI are discussed from the atomic and molecular level. The results show that the structure of PI is crimped and the dipole moment increases under external electric field, which is easy to accumulate charges to form space charge center, especially after the introduction of polar group OH–. In the PI molecules, hole traps are formed in the benzene ring region, and electron traps are formed in the imide ring region. The number of electron trap energy levels is large, in which the space charge trap depth gradually deepens with the increase of external electric field. After the introduction of polar group OH–, the excitation energy of PI molecules decreases, which makes the electrons inside the molecules excited easily. The spatial separation of electrons and holes decreases with the increase of electric field, which is conducive to the recombination of holes and electrons to emit photons.
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Keywords:
- density functional theory /
- trap /
- excited state /
- surface discharge
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图 2 分子优化模型 (a) PI分子单链; (b) PI-OH分子单链
Fig. 2. Molecular optimization model: (a) PI molecular single chain; (b) Pi-OH molecular single chain.
图 5 不同电场下分子态密度图 (a) PI分子; (b) PI-OH分子
Fig. 5. Molecular density of states under different electric fields: (a) Pi molecule; (b) PI-OH molecule.
图 6 分子表面静电势 (a) PI分子; (b) PI-OH分子
Fig. 6. Molecular surface electrostatic potential: (a) PI molecule; (b) PI-OH molecule.
图 7 PI单链分子的轨道跃迁 (a) F=0 a.u.; (b) F = 0.010 a.u.
Fig. 7. Orbital transition of PI single molecule: (a) F = 0 a.u.; (b) F = 0.010 a.u..
表 1 聚酰亚胺片断部分键长与键角
Table 1. Partial bond length and bond angle of polyimide fragments.
N R(13, 14)/nm R(9, 10)/nm R(7, 9)/nm A(13, 14, 15)/(°) A(9, 7, 8)/(°) A(4, 5, 6)/(°) N = 1 1.391 1.422 1.422 121.041 126.108 114.756 N = 2 1.389 1.423 1.422 121.099 126.045 114.894 N = 3 1.389 1.421 1.422 121.115 126.011 114.883 
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表 2 不同外电场下分子的几何结构
Table 2. Molecular geometry under different external electric fields.
F/a.u. PI PI-OH R(50, 55)/nm A(63, 70, 71)/(°) R(46, 51)/nm A(59, 66, 67)/(°) 0 1.411 121.099 1.420 121.162 0.001 1.411 121.330 1.420 121.145 0.002 1.423 121.472 1.421 121.117 0.003 1.424 121.501 1.426 120.049 0.004 1.425 121.534 1.426 119.595 0.005 1.426 121.580 1.427 118.302 0.006 1.428 121.669 1.428 117.915 0.007 1.430 121.707 1.428 116.818 0.008 1.433 121.761 1.429 116.387 0.009 1.436 121.792 1.430 116.008 0.010 1.440 121.917 1.432 115.833
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表 3 不同外电场下分子前线轨道能级的变化
Table 3. Changes of molecular frontier orbital energy levels under different external electric fields.
F/a.u PI PI-OH EH/eV EL/eV EG/eV EH/eV EL/eV EG/eV 0 –7.661 –2.739 4.922 –7.487 –3.018 4.469 0.001 –7.666 –2.765 4.901 –7.451 –3.070 4.381 0.002 –7.674 –2.791 4.883 –7.405 –3.102 4.303 0.003 –7.655 –2.810 4.845 –7.326 –3.146 4.180 0.004 –7.638 –2.817 4.821 –7.285 –3.252 4.033 0.005 –7.602 –2.836 4.766 –7.039 –3.433 3.606 0.006 –7.564 –2.855 4.709 –6.902 –3.546 3.356 0.007 –7.535 –2.871 4.664 –6.645 –3.788 2.857 0.008 –7.502 –2.891 4.611 –6.438 –3.938 2.500 0.009 –7.495 –2.914 4.581 –6.259 –4.067 2.192 0.010 –7.499 –2.939 4.560 –6.116 –4.202 1.914
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表 4 电场下空间电荷陷阱深度的变化
Table 4. Changes of space charge trap depth under electric field.
E/eV F/a.u. 0 0.001 0.002 0.003 0.004 0.005 0.006 0.007 0.008 0.009 0.010 PI EEA(a) 2.834 2.765 2.679 2.594 2.498 2.388 2.264 2.126 1.974 1.806 1.622 EEA(b) 2.721 2.639 2.204 2.116 1.899 1.701 1.509 1.279 1.006 0.718 0.408 Etrap 0.113 0.126 0.475 0.479 0.599 0.687 0.755 0.847 0.968 1.089 1.214 PI-OH EEA(a) 2.965 2.864 2.776 2.643 2.488 2.330 2.127 1.932 1.687 1.170 0.898 EEA(b) 2.639 2.503 2.258 2.008 1.798 1.571 1.329 1.063 0.781 0.482 0.164 Etrap 0.326 0.361 0.518 0.635 0.691 0.758 0.799 0.869 0.906 0.688 0.734
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表 5 PI和PI-OH单链分子的前8个激发能
Table 5. Top 8 excitation energies of PI and PI-OH single molecules.
Eex/eV N = 1 N = 2 N = 3 N = 4 N = 5 N = 6 N = 7 N = 8 PI 3.369 3.476 3.770 3.813 3.821 3.912 3.913 3.990 PI-OH 3.091 3.325 3.381 3.727 3.730 3.897 3.942 3.951
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表 6 激发态S(0)→S(1)的各类参数
Table 6. Various parameters of excited state S(0)→S(1).
F/a.u. Sr/a.u. D/Å t/Å Orbital contribution(hole) Orbital contribution(electron) 0 0.383 3.998 1.665 MO 195-12.33% MO 197-76.94% MO 198-95.01% 0.010 0.409 3.628 1.234 MO 197-77.56% MO198-94.7% 注: MO代表分子轨道.
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[1] 黄旭炜, 刘涛, 舒想, 李庆民, 王忠东 2020 高电压技术 46 215
Google Scholar
Huang X W, Liu T, Shu X, Li Q M, Wang Z D 2020 High Voltage Eng. 46 215
Google Scholar
[2] 胡一卓, 董明, 谢佳成, 何文林, 汪可, 李金忠 2020 电网技术 44 1276
Google Scholar
Hu Y Z, Dong M, Xie J C, He W L, Wang K, Li J Z 2020 Power System Technology 44 1276
Google Scholar
[3] 董国静, 刘涛, 李庆民 2020 电工技术学报 35 2006
Google Scholar
Dong G J, Liu T, Li Q M 2020 Trans. China Electrotechnical. Soc. 35 2006
Google Scholar
[4] 刘涛, 韩帅, 李庆民, 鲁旭, 黄旭炜 2016 电工技术学报 31 199
Google Scholar
Liu T, Han S, Li Q M, Lu X, Huang X W 2016 Trans. China Electrotechnical. Soc. 31 199
Google Scholar
[5] 张开放, 张黎, 李宗蔚, 赵彤, 邹亮 2019 电工技术学报 34 3275
Google Scholar
Zhang K F, Zhang L, Li Z W, Zhao T, Zhou L 2019 Trans. China Electrotechnical. Soc. 34 3275
Google Scholar
[6] 罗杨, 吴广宁, 刘继午, 曹开江, 彭佳, 张依强, 朱光亚 2013 中国电机工程学报 33 187
Google Scholar
Luo Y, Wu G Y, Liu J W, Cao K J, Peng J, Zhang Y Q, Zhu G Y 2013 Chin. Soc. Elec. Eng. 33 187
Google Scholar
[7] 赵义焜, 张国强, 韩冬, 杨富尧, 刘洋 2019 电工技术学报 34 3464
Google Scholar
Zhao Y K, Zhang G Q, Han D, Yang F Y, Liu Y 2019 Trans. China Electrotechnical. Soc. 34 3464
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[8] 田付强, 彭潇 2017 电工技术学报 32 3
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[10] 刘涛, 董国静, 李庆民, 任瀚文, 王健, 王忠东 2020 高电压技术 46 2504
Google Scholar
Liu T, Dong G J, Li Q M, Ren H W, Wang J, Wang Z D 2020 High Voltage Eng. 46 2504
Google Scholar
[11] Boufayed F, Teyssedre G, Laurent C, Roy Le S, Dissado L A, Ségur P, Montanari G C 2006 J. Appl. Phys. 100 104
Google Scholar
[12] 罗杨, 吴广宁, 曹开江, 辛正亮, 张依强, 徐慧慧 2012 高电压技术 38 2707
Google Scholar
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Google Scholar
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[15] 李亚莎, 谢云龙, 黄太焕, 徐程, 刘国成 2018 物理学报 67 183101
Google Scholar
Li Y S, Xie Y L, Huang T H, Xu C, Liu G C 2018 Acta Phys. Sin. 67 183101
Google Scholar
[16] 李亚莎, 孙林翔, 周筱, 陈凯, 汪辉耀 2020 物理学报 69 013101
Google Scholar
Li Y S, Sun L X, Zhou X, Chen K, Wang H Y 2020 Acta Phys. Sin. 69 013101
Google Scholar
[17] 李进, 赵仁勇, 杜伯学, 苏金刚, 韩晨磊, 高田达雄 2020 高电压技术 46 772
Google Scholar
Li J, Zhao R Y, Du B X, Su J G, Han C L, Takada T 2020 High Voltage Eng. 46 772
Google Scholar
[18] Frish M J, Trucks G W, Schlegal H B 2010 Gaussian 09 (Revision B01) (Walling ford: Gaussian Inc. )
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Mei J S, Yang H J, Yin J H, Lei Q Q 2006 Journal of Harbin University of Science and Technology 11 50
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Google Scholar
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Li H, Xu L, Liu T, Yang Z Y 2021 Electric Power Eng. Technology 5 54
Google Scholar
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Zhang X T, Wu G N, Yang Y, Wu X H, Lei Y X, Zhong X 2018 High Voltage Eng. 44 3097
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[24] LU T, Chen F 2012 J. Comput. Chem. 33 580
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Google Scholar
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Lin J Q, Li L D, He X X, Yang W L, Chi Q G, Zhang C H, Xie Z B, Lei Q Q 2017 Electric Machines and Control 21 89
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Google Scholar
Li S T, Huang Q F, Sun J, Zhang T, Li J Y 2010 Acta Phys. Sin. 59 422
Google Scholar
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Huang B R, Wang W W, Li S T, Li X Y, Jiang Q H, Nie Y J, Deng Y K 2021 J. Electrical Eng. 16 25
Google Scholar
[30] 罗龙波, 叶信合, 易江, 李科, 刘向阳 2021 高分子学报 52 363
Google Scholar
Luo L B, Ye X H, Yi J, Li K, Liu X Y 2021 Acta Polymerica Sinica 52 363
Google Scholar
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