Design, fabrication, and high-temperature dielectric energy storage performance of thermoplastic polyimide/aluminum oxide sandwich-structured flexible dielectric films

Zhuo Jun-Tian; Lin Ming-Hao; Zhang Qi-Yan; Huang Shuang-Wu

doi:10.7498/aps.73.20240838

Abstract

Dielectric capacitors are essential components in advanced electronic and power systems due to their high power densities, fast charge-discharge rates, low losses, and excellent cycling stabilities. Polymer dielectrics, such as biaxially oriented polypropylene (BOPP), are preferred dielectric materials for high-voltage capacitors because of their high breakdown strength, flexibility, and easy processing. However, their relatively low thermal stability limits their applications in high-temperature environments, such as in electric vehicles and photovoltaic power generation systems. In this study, sandwich-structured dielectric films are prepared by using physical vapor deposition (PVD) to deposit aluminum oxide (Al₂O₃) layers onto thermoplastic polyimide (TPI) films to achieve high capacitive energy storage at high temperatures. The TPI films are chosen for their high glass transition temperature (T_g), while Al₂O₃ layers are deposited to enhance the Schottky barrier, thereby suppressing electrode charge injection, reducing leakage current, and improving breakdown strength at high temperatures. Various characterization techniques are employed to assess the microstructure, dielectric properties, and energy storage performance of the prepared Al₂O₃/TPI/Al₂O₃ sandwich-structured films. The results demonstrate that the Al₂O₃ coating exhibits excellent interfacial adhesion with TPI films, successfully inhibiting charge injection and thereby reducing leakage current. For instance, at 150 °C and 250 MV/m, the leakage current density of TPI film is 3.19×10^–7 A/cm², whereas for Al₂O₃/TPI/Al₂O₃ sandwich-structured film, its leakage current density is 2.77×10^–8 A/cm², a decrease of one order of magnitude. The suppression of charge injection and reduction of leakage current contribute to outstanding discharge energy density (U_d) and charge-discharge efficiency (η) at high temperatures. Specifically, at high temperatures of 150 and 200 °C, the U_d reaches 4.06 and 2.72 J/cm³, respectively, with η > 90%, i.e. increasing 98.0% and 349.4% compared with those of pure TPI films. Furthermore, the PVD process used for fabricating these sandwich-structured films is highly compatible with existing methods of producing metal electrodes in capacitors, offering significant advantages in production efficiency and cost control. This study suggests that the Al₂O₃/TPI/Al₂O₃ sandwich-structured films, prepared by using the PVD process and exhibiting exceptional high-temperature capacitive energy storage performance, are highly promising for applications in environments with high temperatures and high electric fields.

Keywords:

Authors and contacts

1.
State Key Laboratory of Radio Frequency Heterogeneous Integration, Shenzhen University, Shenzhen 518060, China
2.
College of Electronics and Information Engineering, Shenzhen University, Shenzhen 518060, China

Corresponding author: Zhang Qi-Yan, zhangqy15@tsinghua.org.cn

Funds: Project supported by the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 52203096) and the Shenzhen Science and Technology Innovation Program, China (Grant Nos. RCBS20221008093110036, ZDSYS20220527171402005).

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References

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Cited By

图 1 (a) 三明治结构电介质薄膜的结构示意图; (b) Al₂O₃/TPI/Al₂O₃三明治结构薄膜的实物图; (c) TPI沉积氧化铝镀层前后的DSC升温曲线; 不同镀层厚度Al₂O₃/TPI/Al₂O₃薄膜的SEM图 (d) 100 nm; (e) 200 nm; (f) 300 nm; (g) Al₂O₃/TPI/ Al₂O₃薄膜的表面SEM照片及EDS分析图片; (h) Al₂O₃/TPI/ Al₂O₃薄膜表面AFM三维照片; (i) 纯TPI薄膜表面AFM三维照片

Figure 1. (a) Schematic diagram of the sandwich-structured dielectric films; (b) photograph of TPI coated with aluminum oxide layer; (c) DSC heating curves of TPI films before and after Al₂O₃ deposition; scanning electron microscope (SEM) images of TPI films with Al₂O₃ coating layers of (d) 100, (e) 200, and (f) 300 nm thickness; (g) SEM images and EDS analysis of the Al₂O₃/TPI/Al₂O₃ films; 3D AFM images of the surface of (h) the Al₂O₃/TPI/Al₂O₃ films and (i) pristine TPI films.

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图 2 (a) 常温和(b) 200 ℃温度下TPI及其三明治结构薄膜的介电常数与介电损耗随频率的变化; (c) 10 kHz下样品的介电常数和介电损耗随Al₂O₃镀层厚度的变化; (d) TPI及其三明治结构薄膜在10 kHz下介电常数与介电损耗随温度的变化图

Figure 2. Dielectric constant and dielectric loss of TPI and its sandwich-structured films as a function of frequency at (a) Room temperature and (b) 200 ℃; (c) dielectric constant and dielectric loss at 10 kHz as a function of Al₂O₃ coating thickness; (d) dielectric constant and dielectric loss of TPI and its sandwich-structured films as a function of temperature at 10 kHz.

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图 3 (a) 150和(b) 200 ℃下TPI薄膜在沉积Al₂O₃镀层前后漏电流密度随电场强度的变化; (c) 不同温度下TPI薄膜沉积Al₂O₃前后的电导率对比; (d) 密度泛函理论计算得到的TPI与Al₂O₃能带示意图; (e) 电极Au与电介质TPI界面处能带结构图; (f) 电极Au与镀层Al₂O₃界面处能带结构图

Figure 3. Leakage current density of TPI films before and after Al₂O₃ deposition at (a) 150 and (b) 200 ℃; (c) comparation of electrical conductivity for TPI films before and after Al₂O₃ deposition at 150 and 200 ℃; (d) energy band diagram of TPI and Al₂O₃ obtained from density functional theory (DFT) calculations; (e) energy band structure at the interface between the Au electrode and the TPI dielectric; (f) energy band structure at the interface between the Au electrode and the Al₂O₃ coating.

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图 4 (a) 150和 (b) 200 ℃下TPI和TPI-200 nm Al₂O₃薄膜的韦伯分布击穿强度; (c) 不同温度下TPI和TPI-200 nm Al₂O₃薄膜击穿强度的对比

Figure 4. Weibull distribution of breakdown strength for TPI and TPI-200 nm Al₂O₃ films at (a) 150 and 200 ℃; (c) comparation of the weibull breakdown strength for TPI and TPI-200 nm Al₂O₃ films at different temperatures.

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图 5 (a) 纯TPI薄膜和(b) TPI-200 nm Al₂O₃薄膜在温度为150 ℃时的电位移-电场强度(D-E)曲线; (c) 纯TPI薄膜和(d) TPI-200 nm Al₂O₃薄膜在温度为200 ℃时的D-E曲线

Figure 5. D-E loops of (a) pristine TPI and (b) TPI-200 nm Al₂O₃ films at 150 ℃; D-E loops of (c) pristine TPI and (d) TPI-200 nm Al₂O₃ films at 200 ℃.

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图 6 (a) 150 ℃ 和(b) 200 ℃温度下放电能量密度(U_e)和充放电效率随电场强度的变化曲线; (c) 不同温度下TPI-200 nm Al₂O₃和TPI电介质薄膜在90%效率时的放电能量密度对比; (d) 不同温度下TPI-200 nm Al₂O₃和TPI电介质薄膜在电场强度350 MV/m下能量密度损失的对比

Figure 6. Discharge energy density (U_e) and charge-discharge efficiency (η) at different electric fields at (a) 150 ℃ and (b) 200 ℃; (c) comparation of the discharge energy density at 90% efficiency for TPI-200 nm Al₂O₃ and TPI films at 150 and 200 ℃; (d) comparation of energy density loss at 350 MV/m for TPI-200 nm Al₂O₃ and TPI films at 150 and 200 ℃.

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map

[1]	查俊伟, 查磊军, 郑明胜 2023 72 018401 Google Scholar Zha J W, Zha L J, Zheng M S 2023 Acta Phys. Sin. 72 018401 Google Scholar
[2]	Zhang M, Lan S, Yang B B, Pan H, Liu Y Q, Zhang Q H, Qi J L, Chen D, Su H, Yi D, Yang Y Y, Wei R, Cai H D, Han H J, Gu L, Nan C W, Lin Y H 2024 Science 384 185 Google Scholar
[3]	Luo H, Wang F, Guo R, Zhang D, He G H, Chen S, Wang Q 2022 Adv. Sci. 9 2202438 Google Scholar
[4]	Chen J, Pei Z T, Chai B, Jiang P K, Ma L, Zhu L, Huang X Y 2023 Adv. Mater. 2308670 Google Scholar
[5]	Ho J, Jow T R 2012 IEEE Trans. Dielect. Electr. Insul. 19 990 Google Scholar
[6]	Zhang Q, Chen X, Zhang B, Zhang T, Lu W, Chen Z, Liu Z, Kim S H, Donovan B, Warzoha R J, Gomez E D, Bernholc J, Zhang Q M 2021 Matter 4 2448 Google Scholar
[7]	Li Q, Yao F Z, Liu Y, Zhang G, Wang H, Wang Q 2018 Annu. Rev. Mater. Res. 48 219 Google Scholar
[8]	Ho J S, Greenbaum S G 2018 ACS Appl. Mater. Interfaces 10 29189 Google Scholar
[9]	Zhang Q, Chen X, Zhang T, Zhang Q M 2019 Nano Energy 64 103916 Google Scholar
[10]	Zhang Q, Li D, Zhong Y, Hu Y, Huang S, Dong S, Zhang Q 2024 Energy Environ. Sci. In Press Google Scholar
[11]	Wang R, Zhu Y, Fu J, Yang M, Ran Z, Li J, Li M, Hu J, He J, Li Q 2023 Nat. Commun. 14 2406 Google Scholar
[12]	Zhang T, Chen X, Thakur Y, Lu B, Zhang Q, Runt J, Zhang Q M 2020 Sci. Adv. 6 eaax6622 Google Scholar
[13]	董久锋, 邓星磊, 牛玉娟, 潘子钊, 汪宏 2020 69 217701 Google Scholar Dong J F, Deng X L, Niu Y J, Pan Z Z, Wang H 2020 Acta Phys. Sin. 69 217701 Google Scholar
[14]	Li Q, Chen L, Gadinski M R, Zhang S, Zhang G, Li H U, Iagodkine E, Haque A, Chen L Q, Jackson T N, Wang Q 2015 Nature 523 576 Google Scholar
[15]	Pei J, Yin L, Zhong S, Dang Z 2023 Adv. Mater. 35 2203623 Google Scholar
[16]	Wu F, Xie A, Jiang L, Mukherjee S, Gao H, Shi J, Wu J, Shang H, Sheng Z, Guo R, Wu L, Liu J, Suss M E, Terzis A, Li W, Zeng H 2023 Adv. Funct. Mater. 33 2212861 Google Scholar
[17]	Min D, Ji M, Li P, Gao Z, Liu W, Li S, Liu J 2021 IEEE Trans. Dielectr. Electr. Insul. 28 2011 Google Scholar
[18]	Li H, Ai D, Ren L, Yao B, Han Z, Shen Z, Wang J, Chen L, Wang Q 2019 Adv. Mater. 31 1900875 Google Scholar
[19]	Li Q, Cheng S 2020 IEEE Electr. Insul. Mag. 36 7 Google Scholar
[20]	Rui G C, Bernholc J, Zhang S H, Zhang Q M 2024 Adv. Mater. 2311739 Google Scholar
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[22]	Zhou Y, Zhu Y, Xu W, Wang Q 2023 Adv. Energy Mater. 13 2203961 Google Scholar
[23]	Li Z, Zhang Y, Pan Z, Fan X, Li P, Chen W, Liu J, Li W 2024 ACS Appl. Mater. Interfaces 16 10756 Google Scholar
[24]	Ai D, Li H, Zhou Y, Ren L, Han Z, Yao B, Zhou W, Zhao L, Xu J, Wang Q 2020 Adv. Energy Mater. 10 1903881 Google Scholar
[25]	Tan D Q 2020 Adv. Funct. Mater. 30 1808567 Google Scholar
[26]	Zhang T, Sun H, Yin C, Jung Y H, Min S, Zhang Y, Zhang C, Chen Q, Lee K J, Chi Q 2023 Prog. Mater. Sci. 140 101207 Google Scholar
[27]	Zhou Y, Li Q, Dang B, Yang Y, Shao T, Li H, Hu J, Zeng R, He J, Wang Q 2018 Adv. Mater. 30 1805672 Google Scholar
[28]	Li H, Chang B S, Kim H, Xie Z, Lainé A, Ma L, Xu T, Yang C, Kwon J, Shelton S W, Klivansky L M, Altoé V, Gao B, Schwartzberg A M, Peng Z, Ritchie R O, Xu T, Salmeron M, Ruiz R, Sharpless K B, Wu P, Liu Y 2023 Joule 7 95 Google Scholar
[29]	Cheng S, Zhou Y, Hu J, He J, Li Q 2020 IEEE Trans. Dielectr. Electr. Insul. 27 498 Google Scholar
[30]	Cheng S, Zhou Y, Li Y S, Yuan C, Yang M C, Fu J, Hu J, He J L 2021 Energy Storage Mater. 42 445 Google Scholar
[31]	Wu X, Song G, Zhang X, Lin X, Ivry Y, Tan D Q 2022 Chem. Eng. J. 450 137940 Google Scholar
[32]	Azizi A, Gadinski M R, Li Q, AlSaud M A, Wang J, Wang Y, Wang B, Liu F, Chen L, Alem N, Wang Q 2017 Adv. Mater. 29 1701864 Google Scholar
[33]	李雨凡, 薛文清, 李玉超, 战艳虎, 谢倩, 李艳凯, 查俊伟 2024 73 027702 Google Scholar Li Y F, Xue W Q, Li Y C, Zhan Y H, Xie Q, Li Y K, Zha J W 2024 Acta Phys. Sin. 73 027702 Google Scholar
[34]	Pan L, Wang F, He Y, Du G 2022 2022 IEEE International Conference on High Voltage Engineering and Applications (ICHVE) Chongqing, China , 2022-09-25, 2022 pp1–4
[35]	Li J, Ren G K, Chen J, Chen X, Wu W, Liu Y, Chen X, Song J, Lin Y H, Shi Y 2022 JOM 74 3069 Google Scholar
[36]	Bao Z, Du X, Ding S, Chen J, Dai Z, Liu C, Wang Y, Yin Y, Li X 2022 ACS Appl. Energy Mater. 5 3119 Google Scholar
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