Surface discharge of bulk materials investigated from change of charge trap characteristics of polyimide single molecular chain

Li Ya-Sha; Xia Yu; Liu Shi-Chong; Qu Cong

doi:10.7498/aps.71.20211611

Abstract

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.

Keywords:

Authors and contacts

College of Electrical and New Energy, China Three Gorges University, Yichang 443002, China

Corresponding author: Xia Yu, 1106283537@qq.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51577105).

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References

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图 1 PI分子结构式

Figure 1. Molecular formula of PI.

DownLoad: Full-Size Img PowerPoint

图 2 分子优化模型　(a) PI分子单链; (b) PI-OH分子单链

Figure 2. Molecular optimization model: (a) PI molecular single chain; (b) Pi-OH molecular single chain.

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图 3 分子偶极矩的变化

Figure 3. Changes of molecular dipole moments.

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图 4 轨道云图与能级分布图

Figure 4. Orbital cloud diagram and energy level distribution diagram.

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图 5 不同电场下分子态密度图　(a) PI分子; (b) PI-OH分子

Figure 5. Molecular density of states under different electric fields: (a) Pi molecule; (b) PI-OH molecule.

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图 6 分子表面静电势　(a) PI分子; (b) PI-OH分子

Figure 6. Molecular surface electrostatic potential: (a) PI molecule; (b) PI-OH molecule.

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图 7 PI单链分子的轨道跃迁　(a) F=0 a.u.; (b) F = 0.010 a.u.

Figure 7. Orbital transition of PI single molecule: (a) F = 0 a.u.; (b) F = 0.010 a.u..

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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

DownLoad: CSV

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
F/a.u.	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
F/a.u	E_H/eV	E_L/eV	E_G/eV	E_H/eV	E_L/eV	E_G/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

DownLoad: CSV

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.
E/eV		0	0.001	0.002	0.003	0.004	0.005	0.006	0.007	0.008	0.009	0.010
PI	E_EA(a)	2.834	2.765	2.679	2.594	2.498	2.388	2.264	2.126	1.974	1.806	1.622
	E_EA(b)	2.721	2.639	2.204	2.116	1.899	1.701	1.509	1.279	1.006	0.718	0.408
	E_trap	0.113	0.126	0.475	0.479	0.599	0.687	0.755	0.847	0.968	1.089	1.214
PI-OH	E_EA(a)	2.965	2.864	2.776	2.643	2.488	2.330	2.127	1.932	1.687	1.170	0.898
	E_EA(b)	2.639	2.503	2.258	2.008	1.798	1.571	1.329	1.063	0.781	0.482	0.164
	E_trap	0.326	0.361	0.518	0.635	0.691	0.758	0.799	0.869	0.906	0.688	0.734

DownLoad: CSV

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.

	E_ex/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

DownLoad: CSV

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.

DownLoad: CSV

[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
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[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 Google Scholar
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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 Luo Y, Wu G Y, Cao K J, Xin Z L, Zhang Y Q, Xu H H 2012 High Voltage Eng. 38 2707 Google Scholar
[13]	鲁旭, 韩帅, 李庆民, 黄旭炜, 王学磊, 王高勇 2016 电工技术学报 31 14 Google Scholar Lu X, Han S, Li Q M, Huang X W, Wang X L, Wang G Y 2016 Trans. China Electrotechnical. Soc. 31 14 Google Scholar
[14]	Sarathi R, Thangabalan B, Harid N, Griffiths H 2020 IET Nanodielectrics 3 44
[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. )
[19]	梅金硕, 杨红军, 殷景华, 雷清泉 2006 哈尔滨理工大学学报 11 50 Google Scholar Mei J S, Yang H J, Yin J H, Lei Q Q 2006 Journal of Harbin University of Science and Technology 11 50 Google Scholar
[20]	吴旭辉, 吴广宁, 杨雁, 张兴涛, 雷毅鑫, 钟鑫, 朱健 2018 中国电机工程学报 38 3410 Google Scholar Wu X H, Wu G N, Yang Y, Zhang X T, Lei Y X, Zhong X, Zhu J 2018 Chin. Soc. Elec. Eng. 38 3410 Google Scholar
[21]	李欢, 徐磊, 刘涛, 杨章勇 2021 电力工程技术 5 54 Google Scholar Li H, Xu L, Liu T, Yang Z Y 2021 Electric Power Eng. Technology 5 54 Google Scholar
[22]	张兴涛, 吴广宁, 杨雁, 吴旭辉, 雷毅鑫, 钟鑫 2018 高电压技术 44 3097 Google Scholar Zhang X T, Wu G N, Yang Y, Wu X H, Lei Y X, Zhong X 2018 High Voltage Eng. 44 3097 Google Scholar
[23]	Lu T, Chen F W 2012 J. Mol. Graph Model. 38 31 Google Scholar
[24]	LU T, Chen F 2012 J. Comput. Chem. 33 580 Google Scholar
[25]	查俊伟, 田娅娅, 刘雪洁, 董晓迪, 郑明胜 2021 高电压技术 47 1759 Google Scholar Cha J W, Tian Y Y, Liu X J, Dong X D 2021 High Voltage Eng. 47 1759 Google Scholar
[26]	廖瑞金, 陆云才, 杨丽君, 李剑, 孙才新 2006 绝缘材料 39 51 Google Scholar Liao R J, Lu Y C, Yang L J, Li J, Sun C X 2006 Insulating Materials 39 51 Google Scholar
[27]	林家齐, 李兰地, 何霞霞, 杨文龙, 迟庆国, 张昌海, 谢志滨, 雷清泉 2017 电机与控制学报 21 89 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
[28]	李盛涛, 黄奇峰, 孙健, 张拓, 李建英 2010 物理学报 59 422 Google Scholar Li S T, Huang Q F, Sun J, Zhang T, Li J Y 2010 Acta Phys. Sin. 59 422 Google Scholar
[29]	黄炳融, 王威望, 李盛涛, 李欣原, 蒋起航, 聂永杰, 邓云坤 2021 电气工程学报 16 25 Google Scholar 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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Vol. 71, Issue 5 - 2022-03-05

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