Surface structure design of boron nitride nanotubes and mechanism of their regulation on properties of epoxy composite dielectric

Ren Jun-Wen; Jiang Guo-Qing; Chen Zhi-Jie; Wei Hua-Chao; Zhao Li-Hua; Jia Shen-Li

doi:10.7498/aps.73.20230708

Abstract

Adding nanofillers into epoxy resin matrices is a common method to achieve their multi-function. Boron nitride nanotubes (BNNTs) with one-dimensional nanostructures have attracted much attention because of their ultra-high thermal conductivity, wide energy level band gap, high aspect ratio and mechanical strength. Yet, the strong π-π non-covalent bonding and lip-lip interactions make BNNTs prone to agglomeration in the epoxy resin matrix. Moreover, the different physicochemical properties of BNNTs and epoxy resins as well as the chemical inertness of BNNTs surface lead to the lack of effective interfacial interaction between BNNTs and epoxy resin matrix. Therefore, the performance of the epoxy composite dielectric is not enhanced by simple blending solely, but will even have the opposite effect. To address the problems of BNNTs, in this study, the surface structure of BNNTs is constructed from the perspective of interface modulation by using sol-gel method to coat mesoporous silica (mSiO₂) on BNNTs’ surface and further introducing silane coupling agent (KH560). The results indicate that the surface structure of BNNTs can optimize the level of interfacial interaction between BNNTs and epoxy resin matrix, which leads to stronger interfacial connection and elimination of internal pore phenomenon. The dielectric constant and loss of the composite dielectric prepared in this way are further reduced, reaching 4.1 and 0.005 respectively at power frequency, which is significantly lower than that of pure epoxy resin. At the same time, the mechanical toughness (3.01 MJ/m³) and thermal conductivity (0.34 W/(m⋅K)) are greatly improved compared with the counterparts of pure epoxy resin. In addition, the unique nano-mesoporous structure of mSiO₂ endows the composite dielectric with a large number of deep traps, which effectively hinders the migration of electrons, thereby improving the electrical strength of the composite dielectric, and the breakdown field strength reaches 95.42 kV/mm. Furthermore, the interfacial mechanism of BNNTs’ surface structure on dielectric relaxation and trap distribution of composite dielectrics is systematically studied by Tanaka multinuclear model. The above results indicate that the good interfacial interaction between BNNTs and epoxy resin matrix is crucial in establishing the micro-interface structure and improving the macroscopic properties of composite dielectrics. This study presents a novel idea for the multifunctionalities of epoxy resin, and also provides some experimental data support for revealing the correlation among surface properties of nano-fillers, microstructure and macroscopic properties of composite dielectric.

Keywords:

Authors and contacts

College of Electrical Engineering, Sichuan University, Chengdu 610065, China

Corresponding author: Jia Shen-Li, jiashenli@scu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 52107020), the Key R&D Projects in Sichuan Province, China (Grant No. 2023YFG0236), the State Key Laboratory of Electrical Insulation of Power Equipment Open Fund, China (Grant No. EIPE23210), and the China Postdoctoral Science Foundation (Grant No. 2018M643475).

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References

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Cited By

图 1 Tanaka多核模型示意图

Figure 1. Schematic diagram of Tanaka multicore model.

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图 2 BNNTs@mSiO₂-KH560纳米颗粒的制备及表征　(a) BNNTs@mSiO₂-KH560纳米颗粒的制备流程; (b)—(d) BNNTs@mSiO₂-KH560的TEM图像; (e) BNNTs与BNNTs@mSiO₂-KH560在5°—90°的XRD图谱; (f)—(h) BNNTs与BNNTs@mSiO₂-KH560的XPS图谱; (i) BNNTs与BNNTs@mSiO₂-KH560的FT-IR图谱

Figure 2. Preparation and characterization of BNNTs@mSiO₂-KH560 nanoparticles: (a) Preparation process of BNNTs@mSiO₂-KH560 nanoparticles; (b)–(d) TEM images of BNNTs@mSiO₂-KH560; (e) XRD patterns of BNNTs and BNNTs@mSiO₂-KH560 at 5°–90°; (f)–(h) XPS patterns of BNNTs and BNNTs@mSiO₂-KH560; (i) FT-IR patterns of BNNTs and BNNTs@mSiO₂-KH560.

DownLoad: Full-Size Img PowerPoint

图 3 (a)—(d) 不同BNNTs含量的复合电介质SEM图像; (e)—(h)不同BNNTs@mSiO₂-KH560含量的复合电介质SEM图像

Figure 3. (a)–(d) SEM images of composite dielectric with different BNNTs contents; (e)–(h) SEM images of composite dielectric with different BNNTs@mSiO₂-KH560 contents.

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图 4 复合电介质的介电性能　(a) 不同BNNTs含量的复合电介质介电常数、介质损耗因数频谱图; (b) 不同BNNTs@mSiO₂-KH560含量的复合电介质介电常数、介质损耗因数频谱图

Figure 4. Dielectric properties of composite dielectric: (a) Dielectric constant, dielectric loss spectrum of composite dielectric with different BNNTs contents; (b) dielectric constant, dielectric loss spectrum of composite dielectric with different BNNTs@mSiO₂-KH560 contents.

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图 5 (a)—(c) 不同填料复合电介质的Cole-Cole图; (d)—(f) 不同填料复合电介质介电常数两项式Cole-Cole方程拟合图

Figure 5. (a)–(c) Cole-Cole diagram of composite dielectric with different fillers; (d)–(f) two-term Cole-Cole equation fit diagram of dielectric constant of composite dielectric with different fillers.

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图 6 不同填料复合电介质的介质损耗因数温谱图

Figure 6. Temperature spectrum of dielectric loss factor of composite dielectric with different fillers.

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图 7 复合电介质电击穿性能和去极化热刺激电流曲线　(a) 不同填料含量的复合电介质电击穿测试威布尔概率分布图; (b) 复合电介质电击穿通道示意图; (c) 复合电介质良好界面结合阻碍放电发展示意图; (d) 不同填料复合电介质全温谱去极化热刺激电流曲线; (e) 不同填料复合电介质β峰去极化热刺激电流曲线

Figure 7. Electrical breakdown performance and depolarization heat stimulation current curves of composite dielectrics: (a) Weibull probability distribution diagram for electrical breakdown test of composite dielectric with different filler contents; (b) schematic diagram of composite dielectric electrical breakdown channel; (c) schematic diagram of composite dielectric possessing excellent interface combination hinders the intention of discharge emitting; (d) depolarization heat stimulation current curves with full temperature spectrum of composite dielectrics with different fillers; (e) β peak depolarization heat stimulation current curves of composite dielectrics with different fillers.

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图 8 不同填料复合电介质的韧性与导热性能　(a) 不同填料复合电介质的应力-应变曲线; (b) 不同填料复合电介质的杨氏模量; (c), (d) 不同填料复合电介质的导热系数及其增长率

Figure 8. Toughness and thermal conductivity of composite dielectric with different fillers: (a) Stress-strain curve of composite dielectric with different fillers; (b) Young’s modulus of composite dielectric with different fillers; (c), (d) thermal conductivity and its corresponding growth rate of composite dielectric with different fillers.

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表 1 两项式Cole-Cole方程拟合参数表

Table 1. Table of parameters for fitting the two-term Cole-Cole equation.

复合电介质	温度/℃	$ {\omega _1} $/Hz	$ {\gamma _1} $	$ {\omega _2} $/Hz	$ {\gamma _2} $	$ {\varepsilon _\infty } $	$ {\varepsilon _{\text{s}}} $
Epoxy	150	0.32	0.79	8000	0.60	3.50	22.0
	140	0.3	0.91	600	0.60	3.75	10.0
	130	0.34	0.99	50	0.45	3.6	7.0
BNNTs	150	0.5	0.9	8000	0.60	4.60	22.0
	140	0.5	0.95	5000	0.60	4.60	16.5
	130	0.38	0.97	1500	0.50	4.45	10.0
BNNTs@mSiO₂-KH560	150	0.25	0.9	8000	0.60	4.90	28.0
	140	0.13	0.85	1000	0.45	4.50	24.0
	130	0.05	0.65	260	0.45	4.30	15.0

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表 2 复合电介质的标准击穿场强和形状参数

Table 2. Standard breakdown field strength and shape parameters of composite dielectric.

复合电介质	标准击穿场强/ (kV·mm^–1)	形状参数
Epoxy	26.02	4.31
BNNTs-0.5	20.92	4.30
BNNTs-3	36.04	22.89
BNNTs@mSiO₂-KH560-0.5	29.69	6.25
BNNTs@mSiO₂-KH560-1	42.90	7.35
BNNTs@mSiO₂-KH560-2	69.50	6.73
BNNTs@mSiO₂-KH560-3	95.42	6.67

DownLoad: CSV

表 3 复合电介质的陷阱深度及密度

Table 3. Trap depth and density of composite dielectric.

复合电介质	$ \alpha $ 陷阱		$ \beta $ 陷阱		$ Q $/pC
复合电介质	$ E $/eV	$ {Q_\alpha } $/pC	$ E $/eV	$ {Q_\beta } $/pC	$ Q $/pC
Epoxy	0.14	134	—	—	134
BNNTs	0.07	94	—	—	94
BNNTs@mSiO₂-KH560	0.20	652	0.82	0.32	652.32

DownLoad: CSV

表 4 复合电介质的韧性

Table 4. Toughness of composite dielectric.

复合电介质	韧性/(MJ·m^–3)
Epoxy	1.01
BNNTs-0.5	1.02
BNNTs-1	1.04
BNNTs-2	1.37
BNNTs-3	1.83
BNNTs@mSiO₂-KH560-0.5	1.78
BNNTs@mSiO₂-KH560-1	2.21
BNNTs@mSiO₂-KH560-2	2.61
BNNTs@mSiO₂-KH560-3	3.01

DownLoad: CSV

map

[1]	张志斌, 任明, 宋波, 陈荣发, 余家赫, 范文杰, 董明 2022 中国电机工程学报 42 1690 Google Scholar Zhang Z B, Ren M, Song B, Chen R F, Yu J H, Fan W J, Dong M 2022 Proc. CSEE 42 1690 Google Scholar
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[3]	Yuan S J, Peng Z Q, Rong M Z, Zhang M Q 2022 Mater. Chem. Front. 6 1137 Google Scholar
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[5]	Bertasius P, Shneider M, Macutkevic J, Samulionis V, Banys J, Zak A 2019 J. Nanomater Pt. 4 5761439 Google Scholar
[6]	Golberg D, Bando Y, Tang C, Zhi C 2007 Adv. Mater. 19 2413 Google Scholar
[7]	Pan Z, Tao Y, Zhao Y, Fitzgerald M L, McBride J R, Zhu L, Li D 2021 Nano Lett. 21 7317 Google Scholar
[8]	Zhang S, Chen W J, Zhao Y, Yang K, Du B, Ding L J, Yang W, Wu S Z 2021 Compos. B. Eng. 223 109106 Google Scholar
[9]	Huang X Y, Zhi C Y, Jiang P K, Golberg D, Bando Y, Tanaka T 2013 Adv. Funct. Mater. 23 1824 Google Scholar
[10]	Lewis T J 2004 IEEE Trans. Dielectr. Electr. Insul. 11 739 Google Scholar
[11]	Tanaka T 2005 IEEE Trans. Dielectr. Electr. Insul. 12 914 Google Scholar
[12]	Tanaka T, Kozako M, Fuse N, Ohki Y 2005 IEEE Trans. Dielectr. Electr. Insul. 12 669 Google Scholar
[13]	韩延东, 韩明勇, 杨文胜 2021 高等学校化学学报 42 965 Google Scholar Han Y D, Han M Y, Yang W S 2021 Chem. Res. Chin. Univ. 42 965 Google Scholar
[14]	杨国清, 戚相成, 高青青, 王德意 2022 高电压技术 48 689 Google Scholar Yang G Q, Qi X C, Gao Q Q, Wang D Y 2022 High Volt. Eng. 48 689 Google Scholar
[15]	Amin M S, Molin T E, Tampubolon C, Kranbuehl D E, Schniepp H C 2020 Chem. Mater. 32 9090 Google Scholar
[16]	Li B, Zeng H C 2018 ACS Appl. Mater. Interfaces 10 29435 Google Scholar
[17]	李鹏新, 崔浩喆, 邢照亮, 郭宁, 闵道敏 2022 电工技术学报 37 291 Google Scholar Li P X, Cui H Z, Xing Z L, Guo N, Min D M 2022 Trans. CES. 37 291 Google Scholar
[18]	查俊伟, 黄文杰, 杨兴, 万宝全, 郑明胜 2023 高电压技术 49 1055 Google Scholar Zha J W, Huang W J, Yang X, Wan B Q, Zheng M S 2023 High Volt. Eng. 49 1055 Google Scholar
[19]	Zhao L H, Yan L, Wei C M, Li Q H, Huang X L, Wang Z L, Fu M L, Ren J W 2020 J. Phys. Chem. C 124 12723 Google Scholar
[20]	Feng Z Q, Liu X H, Zhang W C, Zeng J J, Liu J M, Chen B F, Lin J M, Tan L Q, Liang L Y 2022 J. Mater. Sci. 57 1156 Google Scholar
[21]	高铭泽, 张沛红 2016 65 247802 Google Scholar Gao M Z, Zhang P H 2016 Acta Phys. Sin. 65 247802 Google Scholar
[22]	邹阳, 林锦煌, 何津, 翁祖辰, 金涛 2023 电工技术学报 38 622 Google Scholar Zhou Y, Lin J H, He J, Wen Z C, Jin T 2023 Trans. CES. 38 622 Google Scholar
[23]	张涛, 江世杰, 张宁, 任乔林, 肖洒 2022 高电压技术 48 1452 Google Scholar Zhang T, Jiang S J, Zhang N, Ren Q L, Xiao S 2022 High Volt. Eng. 48 1452 Google Scholar
[24]	Heileman K, Daoud J, Tabrizian M 2013 Biosens. Bioelectron. 49C 348 Google Scholar
[25]	Achour M E, Brosseau C, Carmona F 2008 J. Appl. Phys. 103 1277 Google Scholar
[26]	成鹏飞, 王辉, 李盛涛 2013 62 057701 Google Scholar Cheng P F, Wang H, Li S T 2013 Acta Phys. Sin. 62 057701 Google Scholar
[27]	Ibragimov T D, Ramazanova I S, Yusifova U V, Rzayev R M 2023 Integr. Ferroelectr. 231 1 Google Scholar
[28]	肖异瑶, 周求宽, 宴年平, 王子悦, 武康宁, 李欢, 李建英 2017 绝缘材料 50 36 Google Scholar Xiao Y Y, Zhou Q K, Yan N P, Wang Z Y, Wu K N, Li H, Li J Y 2017 Insul. Mater. 50 36 Google Scholar
[29]	Siddabattuni S, Schuman T P, Dogan F 2011 Mater. Sci. Eng. B 176 1422 Google Scholar
[30]	张镱议, 李杭东, 郑明胜, 查俊伟, 陈松, 祝晚华, 青双桂 2022 高电压技术 48 4264 Google Scholar Zhang Y Y, Li H D, Zheng M S, Zha J W, Chen S, Zhu W H, Qing S G 2022 High Volt. Eng. 48 4264 Google Scholar
[31]	Tu Y P, Zhou F W, Cheng Y, Jiang H, Wang C, Bai F J, Lin J 2018 IEEE Trans. Dielectr. Electr. Insul. 25 1275 Google Scholar
[32]	Tian F Q, Zhang L, Zhang J L, Peng X 2017 Compos. B. Eng. 114 93 Google Scholar
[33]	Chen Y, Cheng Y H, Wu K, Nelson J K, Dissado L A, Li S G 2009 IEEE Trans. Plasma. Sci. 37 195 Google Scholar
[34]	Yang K, Chen W J, Zhao Y S, He Y, Chen X, Du B, Yang W, Zhang S, Fu Y F 2021 ACS Appl. Mater. Interfaces 13 25850 Google Scholar
[35]	查俊伟, 肖梦雨, 万宝全, 郑明胜 2023 绝缘材料 56 1 Google Scholar Zha J W, Xiao M Y, Wan B Q, Zheng M S 2023 Insul. Mater. 56 1 Google Scholar
[36]	Zhang X D, Zhang Z T, Wang H Z, Cao B Y 2023 ACS Appl. Mater. Interfaces 15 3534 Google Scholar
[37]	Tang D M, Ren C L, Wei X L, Wang M S, Liu C, Bando Y, Golberg D 2011 ACS Nano 5 7362 Google Scholar
[38]	Zeng X, Sun J, Yao Y, Sun R, Xu J B, Wong C P 2017 ACS Nano 11 5167 Google Scholar
[39]	Chang H B, Lu M X, Arias-Monje P J, Luo J, Park C, Kumar S 2019 ACS Appl. Nano Mater. 2 6670 Google Scholar
[40]	查俊伟, 王帆 2022 71 233601 Google Scholar Zha J W, Wang F 2022 Acta Phys. Sin. 71 233601 Google Scholar

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Vol. 73, Issue 2 - 2024-01-20

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