硅酸盐学报

Sr_0.7Bi_0.2TiO₃改性Bi_0.5Na_0.5TiO₃基薄膜电储能特性的优化

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王鑫 ¹^,² , 郝华 ¹^,² , 李东旭 ² , 曹明贺 ² , 尧中华 ¹^,² , 甘小燕 ¹^,² , 刘韩星 ¹^,²

硅酸盐学报 | 电介质储能材料专刊—研究论文 2024,52(4): 1374-1383

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硅酸盐学报 |电介质储能材料专刊—研究论文 2024 , 52 (4) : 1374 -1383

Sr_0.7Bi_0.2TiO₃改性Bi_0.5Na_0.5TiO₃基薄膜电储能特性的优化

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王鑫¹^,², 郝华¹^,², 李东旭², 曹明贺², 尧中华¹^,², 甘小燕¹^,², 刘韩星¹^,²

作者信息

^1．武汉理工大学三亚科教创新园，海南三亚 572000

^2．武汉理工大学材料科学与工程学院，材料科学与工程国际化示范学院（材料与微电子学院），材料复合新技术国家重点实验室，武汉 430070

通讯作者:

刘韩星（1963—），男，博士，教授。

作者简介:

王鑫（1995—），男，博士研究生。

Optimization of Electric Energy Storage Performance of Sr_0.7Bi_0.2TiO₃ Modified Bi_0.5Na_0.5TiO₃-Based Films

Xin WANG¹^,², Hua HAO¹^,², Dongxu LI², Minghe CAO², Zhonghua YAO¹^,², Xiaoyan GAN¹^,², Hanxing LIU¹^,²

Affiliations

^1.Sanya Science and Education Innovation Park, Wuhan University of Technology, Sanya 572000, Hainan, China

^2.State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, School of Material Science and Engineering, International School of Material Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Corresponding Author:

LIU Hanxing (1963-), male, Ph.D., Professor. E-mail: lhxhp@whut.edu.cn

WANG Xin (1995-), male, Doctoral candidate. E-mail: hsin@whut.edu.cn

出版时间: 2024-04-20 doi: 10.14062/j.issn.0454-5648.20230833

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摘要

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无铅（Bi_0.5Na_0.5）TiO₃（BNT）基弛豫铁电薄膜以其高Curie温度和大极化在介质储能中受到广泛关注，然而较低的击穿电场限制了它们的应用。选择Sr_0.7Bi_0.2TiO₃（SBT）作为固溶组元，通过组分调控提高薄膜击穿强度，优化储能性能。结果表明：BNT-xSBT薄膜均为单一钙钛矿结构，没有明显的第二相。随SBT含量增加，晶胞参数先增大后降低，介电常数略微下降，介电损耗保持稳定，击穿强度先上升后降低。最终，在最优组分样品BNT-0.40SBT中获得了3 622.25 kV/cm的高击穿强度和85.99 J/cm³的高储能密度。这种优异的能量存储密度和出色的稳定性，表明样品BNT-0.40SBT是脉冲功率和电力电子应用电容器的有前途的候选者。

关键词

电介质电容器 / 薄膜 / 击穿强度 / 储能性能

Abstract

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Introduction

The environmentally friendly dielectric capacitors based on lead-free relaxation ferroelectrics have attracted recent attention. The material (Bi_0.5Na_0.5)TiO₃ (BNT) exhibits an intrinsic high saturation polarization due to the hybridization between Bi 6s and O 2p orbitals, surpassing conventional lead-free relaxor ferroelectrics. However, a low breakdown strength (BDS) of BNT results in a relatively poor energy storage performance, restricting its further applications. Therefore, improving the BDS of BNT-based materials is a necessity towards achieving a high energy storage density, and one effective measure is a compositional modification. Sr_0.7Bi_0.2TiO₃ (SBT) as an emerging relaxor ferroelectric material has a higher dielectric constant due to the ion substitution-induced local charge imbalance and dipole fluctuations in nanoscale. It is anticipated that introducing SBT as a solid solution component into BNT matrix films can enhance the BDS of the films, optimizing their energy storage performance. In this paper, the impact of SBT/BNT solid solution ratio on phase structure, microstructure, dielectric, and energy storage properties of the SBT modified BNT-based film was investigated.

Methods

The precursor solutions for (1-x)(Bi_0.5Na_0.5)TiO₃-xSr_0.7Bi_0.2TiO₃ (BNT-xSBT, x=0.30, 0.35, 0.40, 0.45, and 0.50) were prepared by a sol-gel method. The precursor solutions prepared were aged via static aging for 24 h before spin-coating. Subsequently, the films were heat-treated on a hot plate and rapidly annealed at 630 ℃ for 2 min. The film preparation process, including spin-coating, heat treatment, and rapid annealing, was repeated for 8 times to complete the film fabrication.

The crystal structure of the films was analyzed by a model PANalytical X'Pert PRO X-ray diffractometer (XRD). The surface and cross-sectional morphologies of the samples were determined a model Ultra Plus scanning electron microscope (SEM). To evaluate the electrical properties of the samples, platinum electrodes with a diameter of 0.2 mm were deposited on the film surface using magnetron sputtering. The leakage current density of the films was obtained by a model 6517A electrostatic/high-resistance meter. The ferroelectric properties of the samples were tested by a model PolyK CPE1801 ferroelectric workstation. The dielectric properties of the samples were analyzed by a model 4294A precision impedance analyzer.

Results and discussion

All the BNT-xSBT films exhibit a single pseudocubic phase structure. The unit cell volume initially increases and then decreases as the SBT content increases, which is affected by a combined effect of Sr²⁺ doping at the A-site and vacancies. The films demonstrate a well-crystallinity, clear grain boundaries, good adhesion to the substrate, and a thickness of approximately 140 nm. The introduction of SBT results in a reduction in the dielectric constant of the film, improving the temperature stability of the dielectrics. At 2 000 kV/cm, the maximum polarization (P_max) and remnant polarization (P_r) of the films both decrease as the SBT content increases, which is consistent with the dielectric performance. The incorporation of an appropriate amount of SBT increases the BDS of the films from 2 975 kV/cm for BNT-0.3SBT to 3 622 kV/cm for BNT-0.40SBT, which is consistent with the leakage current density. Therefore, the optimal composition BNT-0.40SBT film achieves a high recoverable energy storage density (W_rec) of 85.99 J/cm³ and an efficiency of 74% at the breakdown electric field (E_b). This film demonstrates some advantages, compared to other film capacitors. In addition, the BNT-0.40SBT film exhibits a superior high-frequency stability, a heat resistance, and a fatigue resistance, showing a promising potential for applications in dielectric capacitors.

Conclusions

All the films exhibited a well-crystallinity, having a single perovskite phase. With the introduction of SBT, the unit cell volume initially increased and the decreased, and the BDS firstly increased and then decreased. The dielectric constant and polarization intensity gradually decreased, while dielectric loss remained stable. The optimal component BNT-0.40SBT film achieved a high BDS of 3 622.25 kV/cm and a high energy storage density (W_rec) of 85.99 J/cm³. The superior energy storage density and stability indicated that BNT-0.40SBT thin films could be promising candidates for pulse power and power electronics applications in capacitors.

Key words

dielectric capacitor / thin films / breakdown strength / energy storage properties

引用本文

王鑫, 郝华, 李东旭, 曹明贺, 尧中华, 甘小燕, 刘韩星. Sr_0.7Bi_0.2TiO₃改性Bi_0.5Na_0.5TiO₃基薄膜电储能特性的优化. 硅酸盐学报, 2024 , 52 (4) : 1374 -1383 . DOI: 10.14062/j.issn.0454-5648.20230833

Xin WANG, Hua HAO, Dongxu LI, Minghe CAO, Zhonghua YAO, Xiaoyan GAN, Hanxing LIU. Optimization of Electric Energy Storage Performance of Sr_0.7Bi_0.2TiO₃ Modified Bi_0.5Na_0.5TiO₃-Based Films[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (4) : 1374 -1383 . DOI: 10.14062/j.issn.0454-5648.20230833

基金

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武汉理工大学三亚科教创新园开放基金(2022KF0008)
国家重点研发计划项目(2023YFB3812200)
广东省基础与应用基础研究基金项目(2022b1515120041)

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2024年第52卷第4期

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文章信息

doi: 10.14062/j.issn.0454-5648.20230833

接收时间：2023-11-01
首发时间：2026-10-22
出版时间：2024-04-20

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出版历史

收稿日期：2023-11-01
修回日期：2023-11-13

基金

武汉理工大学三亚科教创新园开放基金(2022KF0008)

国家重点研发计划项目(2023YFB3812200)

广东省基础与应用基础研究基金项目(2022b1515120041)

作者信息

^1．武汉理工大学三亚科教创新园，海南三亚 572000

^2．武汉理工大学材料科学与工程学院，材料科学与工程国际化示范学院（材料与微电子学院），材料复合新技术国家重点实验室，武汉 430070

通讯作者:

刘韩星（1963—），男，博士，教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230833

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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