硅酸盐学报

Bi_0.5Na_0.5TiO₃基铁电陶瓷的弛豫特征与储能性能

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王思民 ¹^,²^,³ , 葛广龙 ¹ , 钱进 ¹ , 林锦锋 ¹ , 李国辉 ¹ , 刘志甫 ²^,³ , 翟继卫 ¹

硅酸盐学报 | 电介质储能材料专刊—研究论文 2024,52(4): 1173-1182

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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) : 1173 -1182

Bi_0.5Na_0.5TiO₃基铁电陶瓷的弛豫特征与储能性能

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王思民¹^,²^,³, 葛广龙¹, 钱进¹, 林锦锋¹, 李国辉¹, 刘志甫²^,³, 翟继卫¹

作者信息

^1．同济大学材料科学与工程学院，功能材料研究所，上海 201804

^2．中国科学院上海硅酸盐研究所，无机功能材料与器件重点实验室，上海 200050

^3．中国科学院大学，材料科学与光电工程研究中心，北京 100049

通讯作者:

翟继卫（1963—），男，博士，教授。

作者简介:

王思民（1997—），男，博士研究生。

Relaxation Characteristics and Energy Storage Properties of Bi_0.5Na_0.5TiO₃-Based Ferroelectric Ceramics

Simin WANG¹^,²^,³, Guanglong GE¹, Jin QIAN¹, Jinfeng LIN¹, Guohui LI¹, Zhifu LIU²^,³, Jiwei ZHAI¹

Affiliations

^1.Functional Materials Research Laboratory, School of Materials Science and Engineering, Tongji University, Shanghai 201804, China

^2.The Key Lab of Inorganic Functional Materials and Devices, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

^3.Center of Materials Science and Optoelectronics Engineering, University of the Chinese Academy of Sciences, Beijing 100049, China

Corresponding Author:

ZHAI Jiwei (1963-), male, Ph.D., Professor. E-mail: apzhai@tongji.edu.cn

WANG Simin (1997-), male, Doctoral candidate. E-mail: wangsimin191@mails.ucas.ac.cn

出版时间: 2024-04-20 doi: 10.14062/j.issn.0454-5648.20230736

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摘要

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电介质陶瓷电容器作为信息社会电子器件的核心器件之一，具有可靠性高、耐高温高压和优异的储能特性，尤其是凭借其较高的功率密度，广泛用于先进脉冲功率系统之中。Bi_0.5Na_0.5TiO₃（BNT）作为无铅铁电陶瓷的典型代表已受到广泛研究。然而，其较大的剩余极化和较低的击穿场强限制了BNT陶瓷在储能领域的应用和发展。本工作通过调控弛豫特征，制备了具有较高储能特性的BNT基介质陶瓷。首先，通过掺杂（Al_0.5Nb_0.5）⁴⁺降低陶瓷的晶粒尺寸实现了击穿场强的提高，同时也对弛豫特性的增强有一定贡献。其次，通过调控Sr和Ca的比例可以进一步提高材料的弛豫特性，实现储能密度的提高。当Ca离子取代量达到0.15时，陶瓷获得了最优的综合性能，在630 kV/cm的电场下，其储能密度为6.4 J/cm³，储能效率达到85%。当电压为300 kV/cm时，其功率密度和工作电流密度分别可以达到154.4 MW/cm³和1 029.6 A/cm²，并且其储能性能在20 ℃到110 ℃温度范围内具有良好温度稳定性（3.4±0.12）J/cm³，79.0%±7.4%，在1 Hz到100 Hz频率范围内具有良好的频率稳定性（3.30±0.01）J/cm³，81.0%±5.5%。

关键词

钛酸铋钠陶瓷 / 弛豫性 / 储能密度 / 储能效率

Abstract

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Introduction

Energy storage technology plays a vital role in advanced electronic and power systems. Ceramic dielectric capacitors show a great potential in electronics, pulse power, and defibrillators due to their ultrahigh power density, fast charging/discharging speed, and superior reliability. Increasing the energy storage density of dielectric capacitors will boost the development of powder devices towards miniaturization, lightweight, and low cost. It is thus crucial to improve the energy storage density of dielectric capacitor. In general, high energy storage properties (ESP) are closely related to a larger maximum polarization (P_m), a smaller remnant polarization (P_r), and a larger breakdown strength (E_b). The recoverable energy storage density (W_rec) and energy storage efficiency (η) are the crucial parameters to evaluate their ESP.

This paper designed and prepared a series of (Bi_0.5Na_0.5)_0.65(Sr_1-_xCa_x)_0.35Ti_0.96(Al_0.5Nb_0.5)_0.04O₃ (BNST-xC) ceramics (x=0.05, 0.10, 0.15, 0.20). The effect of relaxation characteristics on the energy storage characteristics of BNT ferroelectric ceramics was investigated.

Methods

The BNST-xC ceramics were fabricated via conventional solid-state reaction and subsequent tape-casting. The oxides and carbonates as raw materials were weighed according to a stoichiometric ratio and ground in a planetary mill with a nylon grinding chamber for 12 h. After drying, the powders were calcined at 850 ℃ for 6 h and then ground for 12 h. Subsequently, the synthesized BNST-xC powders were mixed with glycerol trioleate, ethanol absolute, butanone, dibutyl phthalate, polyvinyl butyral, and polyethylene glycol to obtain a slurry. The uniformly mixed slurry was tape-casted on the surface of vacuum adsorbed PET release film using a model MSK-AFA-Ⅳ automatic thick film coater at a casting speed of 0.6 cm/s. After stacking and pressing, the films were placed in a model PTC LT₀₈₀₀₁ isostatic pressing machine (EASEN) and pressed at 75 ℃. Finally, the green samples were firstly heated at 600 ℃ for 8 h to remove the organics, and then sintered at 1 180-1 220 ℃ for 2 h.

The phase composition of ceramic was characterized by a model D/max 2550V X-ray diffractometer (XRD, Rigaku Co., Japan). The grain size of the sample was determined by a model TM4000 desktop scanning electron microscope (SEM, Hitachi Co., Japan). The Raman spectra were collected by a model Jobin Yvon HR800 Raman scattering spectrometer (Horiba Co., France) under 532 nm laser excitation. The hysteresis loop was determined by a model Premier Ⅱ and radiant ferroelectric analyzer (Precision Co., USA) at 10 Hz; The dielectric performance and frequency dependence were analyzed by a model Agilent E4980A LCR meter and heating equipment (Tongguo Technology Co., China). A specially designed RLC circuit was used to test the charging and discharging performance of the capacitor.

Results and discussion

From the analysis of phase composition, Sr and Ca ions at a position A, and Al and Nb ions at a position B completely enter the interior of the lattice, forming a solid solution. The improvement of grain size by B-site (Al_0.5Nb_0.5)⁴⁺ ion doping is beneficial to enhancing the breakdown field strength. The average grain size of the ceramic gradually increases from 1.36 μm to 1.09 μm as the Ca doping content increases. From the Raman spectroscopy analysis, the substitution of A-site ions increases an overall local structural disorder. Furthermore, the transformation of their internal phase structure can be investigated based on the dielectric temperature spectra of BNST-xC ceramics. The substitution of Ca causes T_s and T_m moving towards a high-temperature region. Also, the dispersion of the peak shape in the dielectric temperature spectrum further proves that the relaxation degree of the overall material system continuously increases with the increase of Ca ion doping content. To more accurately demonstrate the law of material relaxation degree, the Curie-Weiss law is used to calculate the relaxation coefficient of the dielectric temperature spectrum. The flipping of the internal domain structure at the electric field was tested by PFM, further showing the contribution of Ca ions to the enhancement of relaxation properties.

Conclusions

A series of BNST-xC ceramics were prepared by a solid-state reaction method. The relationship between the relaxation characteristics and energy storage characteristics of BNT based ceramics was analyzed via adjusting the ratio of Sr and Ca ions. The optimal energy storage performance (i.e., E_b of 630 kV/cm, and W_rec of 6.4 J/cm³) was achieved as x=0.15. The energy storage efficiency reached 85%. At E_b of 300 kV/cm, the ceramic exhibited a good stability at different temperatures and frequencies as well as a high power density and an operating current density. It was indicated that BNT based relaxor ferroelectrics could have a promising application potential.

Key words

bismuth sodium titanate ceramics / relaxation property / energy storage density / energy storage efficiency

引用本文

王思民, 葛广龙, 钱进, 林锦锋, 李国辉, 刘志甫, 翟继卫. Bi_0.5Na_0.5TiO₃基铁电陶瓷的弛豫特征与储能性能. 硅酸盐学报, 2024 , 52 (4) : 1173 -1182 . DOI: 10.14062/j.issn.0454-5648.20230736

Simin WANG, Guanglong GE, Jin QIAN, Jinfeng LIN, Guohui LI, Zhifu LIU, Jiwei ZHAI. Relaxation Characteristics and Energy Storage Properties of Bi_0.5Na_0.5TiO₃-Based Ferroelectric Ceramics[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (4) : 1173 -1182 . DOI: 10.14062/j.issn.0454-5648.20230736

基金

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国家重点研发计划(2021YFB3800604)

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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.0454-5648.20230736

接收时间：2023-09-21
首发时间：2026-10-22
出版时间：2024-04-20

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收稿日期：2023-09-21
修回日期：2023-11-06

基金

国家重点研发计划(2021YFB3800604)

作者信息

^1．同济大学材料科学与工程学院，功能材料研究所，上海 201804

^2．中国科学院上海硅酸盐研究所，无机功能材料与器件重点实验室，上海 200050

^3．中国科学院大学，材料科学与光电工程研究中心，北京 100049

通讯作者:

翟继卫（1963—），男，博士，教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230736

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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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