Research progress of flexible energy storage dielectric materials with sandwiched structure

Li Yu-Fan; Xue Wen-Qing; Li Yu-Chao; Zhan Yan-Hu; Xie Qian; Li Yan-Kai; Zha Jun-Wei

doi:10.7498/aps.73.20230614

Abstract

Polymer dielectric materials show wide applications in smart power grids, new energy vehicles, aerospace, and national defense technologies due to the ultra-high power density, large breakdown strength, flexibility, easy processing, and self-healing characteristics. With the rapid development of integration, miniaturization and lightweight production of electronic devices, it is required to develop such a storage and transportation dielectric system with larger energy storage density, higher charge and discharge efficiency, good thermostability and being environmentally friendly. However, the contradiction between dielectric constant and breakdown strength of dielectric materials is the key factor and bottleneck to obtain a high performance dielectric material. It is accepted that controlling charge distribution and inhibiting charge carrier injection are important to improve the energy storage characteristics of polymer dielectrics. In recent years, the materials with sandwiched or stacking structures have demonstrated outstanding advantages in inhibiting charge injection and promoting polarization, allowing polymer dielectrics to have increased permittivity and breakdown strength at the same time. Therefore, from the perspectives of material composition, structural design, and preparation methods, this study reviews the research progress of polymer dielectric films with sandwiched structure in improving the energy storage performance. The influence of dielectric polarization, charge distribution, charge injection, interfacial barrier and electrical dendrite growth on the energy storage performance and the synergistic enhancement mechanisms in such sandwich-structured dielectric materials are systematically summarized, showing good development and vast application prospects.In brief, introducing easy polarization, wide-gap and deep-trap nanofillers has greater designability and regulation in the dielectric and breakdown properties. In addition, using the hard layer as the outer layer can reduce charge injection more effectively, resulting in a high breakdown resistance performance that is easy to achieve. The sandwiched structure design also possesses advantages over other methods in maintaining good flexibility and dielectric stability of dielectric materials, thus having become a hot-topic research area in recent years. In the future, it is necessary to combine low conductivity and high thermal conductivity of dielectric polymers to realize high temperature energy storage and efficiency. Researches on recyclable, self-repairing sandwiched insulating films are good for the service life and safety of electronic components and will further expand the application scope of dielectric polymers. Finally, effective evaluation of dielectric with sandwiched structure and energy storage performances through simulation and theoretical modeling is very helpful in revealing the breakdown mechanism and thermal failure mechanism, and also in theoretically guiding the design of polymer dielectric materials.

Keywords:

Authors and contacts

1.
Department of Materials Science and Engineering, Liaocheng University, Liaocheng 252059, China
2.
School of Chemistry and Biological Engineering, University of Science and Technology Beijing, Beijing 100083, China

Corresponding author: Li Yu-Chao, liyuchao@lcu.edu.cn ; Zha Jun-Wei, zhajw@ustb.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52177020, 52277022) and the College Student Innovation and Entrepreneurship Training Program, China (Grant No. CXCY2022184).

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图 1 (a) 介质材料极化储能过程^[5]; (b) 介电材料的D-E曲图^[6]

Figure 1. Schematic diagram of (a) polarization^[5] and (b) D-E loop of dielectric materials^[6].

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图 2 BN和TiO₂协同提升三明治结构电介质材料储能机理^[19]

Figure 2. Synergistic enhancement of energy storage mechanism of sandwich structure composite by BN and TiO₂^[19].

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图 3 三明治结构　(a) 全有机P(VDF-HFP)-PMMA-P(VDF-HFP)薄膜^[21]; (b) 有机/无机PVDF-BT/PVDF-PVDF薄膜^[22]; (c) BN, Sr₂Nb₂O₇协同增强PMMA/PVDF电介质薄膜^[23]; (d) PI-Al₂O₃-PI薄膜示意图^[25]

Figure 3. Diagram of sandwich structure: (a) All-organic composite film of P(VDF-HFP)-PMMA-P(VDF-HFP)^[21], (b) organic/inorganic composite film of PVDF-BT/PVDF-PVDF^[22], (c) BN, Sr₂Nb₂O₇ synergistically reinforced PMMA/PVDF dielectric film^[23] and (d) PI-Al₂O₃-PI composite film^[25].

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图 4 (a) 对称型A-B-A和B-A-B三明治结构电介质材料示意图; (b) 不同结构电介质材料的储能密度^[45]; (c) 相场模拟不同结构复合电介质材料的失效概率与场强关系^[59]

Figure 4. (a) Schematics of symmetric A-B-A and B-A-B types of sandwich structure; (b) different energy storage density ^[45] and (c) failure probability versus electric field ^[59] of A-B-A and B-A-B types of structure.

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图 5 (a) 五层结构PVDF-SNBT/PVDF-PVDF复合薄膜结构示意图^[62]; (b) 对称梯度结构BZCT/PVDF多层膜材料示意图^[66]; (c) 非对称梯度结构PEI-PEI/P(VDF-HFP)-P(VDF-HFP)薄膜示意图^[67]

Figure 5. Schematic of (a) a five-layer dielectric composite film^[62], (b) a symmetrically gradient dielectric film^[66] , and (c) an asymmetrically gradient PEI-PEI/P(VDF-HFP)-P(VDF-HFP) film^[67].

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图 6 (a) 流延工艺^[21]及其(b) PMMA/PVDF-BCZT/PVDF-PMMA/PVDF薄膜扫描电镜图 ^[68]; (c) 旋涂工艺及其(d) BT@HPC/PVDF-PVDF-BT@HPC/PVDF薄膜扫描电镜图^[42]

Figure 6. Sandwich structure composite films prepared by (a) flow casting^[21] and (b) representative SEM image of PMMA/PVDF-BCZT/PVDF-PMMA/PVDF dielectric film ^[68], (c) spin coating process and (d) representative SEM image of BT@HPC/PVDF-PVDF-BT@HPC/PVDF film^[42].

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图 7 (a) 热压法制备FPE-P(VDF-HFP)-FPE三明治结构薄膜的制备过程和扫描电镜图^[36]; (b) 静电纺丝制备P(VDF-HFP)和BT/P(VDF-HFP)多层膜结构及其扫描电镜图^[71]

Figure 7. (a) Hot-compression molding process of FPE-P(VDF-HFP)-FPE sandwich film and SEM image^[36]_; (b) electrostatic spinning preparation of P(VDF-HFP) and BT/P(VDF-HFP) multilayer film and its SEM image^[71].

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表 1 不同材料构成A-B-A型三明治电介质材料的介电性能

Table 1. Dielectric properties of A-B-A type sandwich dielectric materials

材料构成	A层(含量, 厚度)	B层(含量, 厚度)	A-B-A三明治(25 ℃, 1 kHz)
材料构成	A层(含量, 厚度)	B层(含量, 厚度)	$\varepsilon_{\mathrm{r}} $	tanδ	E/(MV·m^–1)	U/(J·cm^–3)	η/%	制备方法	U/U_基体	文献
全有机复合	PVDF (3 μm)	P(VDF-TrFE-CTFE) (3 μm)	12.06	0.35	599	20.86	60	溶液涂膜	1.3	[20]
	P(VDF-HFP) (6.5 μm)	PMMA (6 μm)	7	0.03	440	20.3	84	溶液浇筑	1.3	[21]
	PVDF (4 μm)	P(VDF-TrFE)-PVDF (70% PVDF, volume percent, 10 μm)	12	0.03	582	23.4	65.5	溶液浇筑	1.5	[26]
	P(VH-HFP) (3 μm)	P(VDF-HFP)-PMMA (25% PMMA, weight percent, 4 μm)	9	0.25	680	28	74	热压、拉伸	1.8	[27]
	P(VDF-TrFE-CFE) (4 μm)	PMMA (13 μm)	5	0.05	399.1	9.7	78	静电纺丝、热压	1.7	[28]
	P(VDF-TrFE-CFE) (2 μm)	PVDF (2 μm)	10.2	0.02	550.9	18.3	60	溶液涂覆	2.44	[29]
	PMMA-P(VDF-TrFE-CFE) (20% PMMA, weight percent, 4 μm)	DE-P(VDF-TrFE-CFE) (15% DE, weight percent, 4 μm)	7	0.05	790	20.1	66	溶液浇筑	2.5	[30]
	Parylene (1 μm)	PI (17 μm)	5.04	0.43	460	4.72	44.8	CVD	2.9	[31]
	DE-P(VDF-HFP) (30% DE, weight percent, 2.5 μm)	PMMA (14.5μm)	—	—	300	11.8	89	溶液浇筑	1.45	[32]
	PEI (4.5 μm)	P(VDF-TrFE-CFE) (3 μm)	~7	0.03	504	8	81	溶液浇筑	2.6	[33]
	P(VDF-TrFE-CFE) (3.4 μm)	PEI (6.7 μm)	~5	0.01	275	4	80	溶液浇筑	1.3	[33]
	PVDF (6.5 μm)	DE (4 μm)	10.4	0.03	438	20.92	72	溶液浇筑	1.3	[34]
	PET (2 μm)	P(VDF-HFP) (5 μm)	4.5	0.01	583.2	8.2	86.4	溶液浇筑	1.17	[35]
	Fluorene polyester (7 μm)	P(VDF-HFP) (4 μm)	4	0.014	564	8	86.7	溶液浇筑、热压	1.1	[36]
	PMMA (4 μm)	P(VDF-TrFE-CFE) (9 μm)	4.5	0.05	—	7.03	78	溶液浇筑	1.55	[37]
	PVDF (9 μm)	P(VDF-TrFE-CFE) (16 μm)	16	0.03	408	8.7	60	溶液浇筑、热压	2	[38]
有机/无机杂化	BN/PVDF (2%, weight percent, 4 μm)	TiO₂/PVDF (3%, weight percent, 4 μm)	11.42	0.03	369.9	10.17	56	溶液浇筑、热压	5	[19]
	PVDF (3 μm)	BT@SiO2@PDA/PVDF (3 μm)	12	0.023	634	15.3	64	溶液浇筑	3.85	[24]
	BT/PVDF (3%, weight percent, 4 μm)	PVDF (4 μm)	13.3	<0.025	505	15	60	溶液浇筑	1.6	[22]
	PVDF (4 μm)	BT/PVDF (3%, 4 μm)	12.9	<0.025	519.7	19.1	68.6	溶液浇筑	2.3	[22]
	BT/PVDF (20%, volume percent, 5 μm)	BT/PVDF (1%, volume percent, 10 μm)	17.5	0.05	470	18.8	—	溶液浇筑	4.5	[39]
	BT/P(VDF-HFP) (10%, weight percent, 5 μm)	BNNs (3 μm)	10.99	0.05	414.76	8.37	50	溶液浇筑	2.26	[40]
	h-BN (70 nm)	PVDF (12 μm)	~9.5	0.024	464.7	19.26	52.2	CVD、热压	2.7	[41]
	BT@HPC/PVDF (1%, weight percent, 5 μm)	PVDF (5 μm)	15	0.02	360	10.2	77	旋涂	5.1	[42]
	h-BN (2 μm)	PC (12 μm)	3.15	0.015	—	5.01	80.82	静电纺丝、热压	1.16	[43]
	P(VDF-CTFE)/PMMA (3 μm)	Ag@SrTiO₃/P(VDF-CTFE) (1.5%, weight percent, 5 μm)	7.2	0.041	635.4	24.6	86.3	溶液浇筑	6.15	[44]
	PVDF (8 μm)	BST/PVDF (40%, volume percent, 14μm)	~15	0.025	230.8	7.56	68.59	溶液浇筑、热压	1.89	[45]
	BST/PVDF (20%, volume percent, 8 μm)	PVDF (8 μm)	17.3	0.025	224.5	10.54	72.02	溶液浇筑、热压	2.63	[45]
	PMMA (6.6 μm)	P(VDF-HPF)/GO (2%, weight percent, 12 μm)	10	0.01	286	10.17	77	溶液浇筑	6.78	[46]
	BN/PVDF (8 μm)	BT/PVDF (8 μm)	12	0.02	370	6.2	55	溶液浇筑	1.55	[47]
	BT-np/PVDF (10%, volume percent, 3.5 μm)	BT-nf/PVDF (2%, volume percent, 5.5 μm)	10.5	0.015	453	9.72	—	逐层流延	2.43	[48]
	BT/PMMA (1%, weight percent, 5 μm)	BT/PMMA(9%, weight percent, 10 μm)	7.15	0.05	501.4	6.08	—	溶液浇筑	4.05	[49]
	P(VDF-HFP) (5 μm)	Ag@BN/PEI (5%, weight percent, 5 μm)	5.9	0.018	510	11	80	热压法	—	[50]
	PVDF (5 μm)	NBT@TO/PVDF (6%, weight percent, 10 μm)	12	0.025	304	15.42	66.12	逐层浇筑	3.8	[51]
	PVDF (10 μm)	PPy/TiO₂ (30%, weight percent, 20 μm)	16	0.02	99	2.68	66.7	静电纺丝、热压	1.1	[52]
	BZCT/PVDF (3 l%, volume percent, 10 μm)	Fe₃O₄@BNNS/PVDF (5%, volume percent, 10 μm)	16	0.03	350	8.9	—	溶液浇筑、热压	2.3	[53]
	BN/PVDF (10 %, weigh percent, 4 μm)	BST/PVDF (8%, weigh percent, 8 μm)	12	0.025	588	20.5	60	溶液浇筑	4	[54]
注: Na_0.5Bi_0.5TiO₃@TiO₂=NBT@TO, hollow porous carbon=HPC, BT-np (nf)= BT纳米颗粒(纳米片), Polypyrrole=PPy, 0.5 Ba(Zr_0.2Ti_0.8)O₃-0.5(Ba_0.7Ca_0.3)TiO₃=BZCT, polyacrylate elastomer=DE.

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