硅酸盐学报

KNN对BNBST陶瓷储能特性的影响

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李志鹏 ¹^,²^,³^,⁴ , 沈宗洋 ¹^,²^,³^,⁴ , 李妍 ¹^,²^,³^,⁴ , 王竹梅 ¹^,²^,³^,⁴ , 石旭海 ¹^,²^,³^,⁴ , 邓伟 ¹^,²^,³^,⁴ , 李月明 ¹^,²^,³^,⁴

硅酸盐学报 | 电介质储能材料专刊—研究论文 2024,52(4): 1217-1228

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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) : 1217 -1228

KNN对BNBST陶瓷储能特性的影响

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李志鹏¹^,²^,³^,⁴, 沈宗洋¹^,²^,³^,⁴, 李妍¹^,²^,³^,⁴, 王竹梅¹^,²^,³^,⁴, 石旭海¹^,²^,³^,⁴, 邓伟¹^,²^,³^,⁴, 李月明¹^,²^,³^,⁴

作者信息

^1．景德镇陶瓷大学材料科学与工程学院，江西景德镇 333403

^2．先进陶瓷材料研究所，江西景德镇 333403

^3．中国轻工业功能陶瓷材料重点实验室，江西景德镇 333403

^4．江西省能量存储与转换陶瓷材料工程实验室，江西景德镇 333403

通讯作者:

沈宗洋（1979—），男，博士，教授。

作者简介:

李志鹏（1994—），男，博士研究生。

Effect of KNN on Energy Storage Performance of BNBST Ceramics

Zhipeng LI¹^,²^,³^,⁴, Zongyang SHEN¹^,²^,³^,⁴, Yan LI¹^,²^,³^,⁴, Zhumei WANG¹^,²^,³^,⁴, Xuhai SHI¹^,²^,³^,⁴, Wei DENG¹^,²^,³^,⁴, Yueming LI¹^,²^,³^,⁴

Affiliations

^1.School of Materials Science and Engineering, Jingdezhen Ceramic University, Jingdezhen 333403, Jiangxi, China

^2.Institute of Advanced Ceramic Materials, Jingdezhen 333403, Jiangxi, China

^3.China Key Laboratory of Functional Ceramic Materials for Light Industry, Jingdezhen 333403, Jiangxi, China

^4.Jiangxi Energy Storage and Conversion Ceramic Materials Engineering Laboratory, Jingdezhen 333403, Jiangxi, China

Corresponding Author:

SHEN Zongyang (1979-), male, Ph.D., Professor. E-mail: shenzongyang@163.com

LI Zhipeng (1994-), male, Ph.D., Doctoral candidate. E-mail: 1534098087@qq.com

出版时间: 2024-04-20 doi: 10.14062/j.issn.0454-5648.20230750

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摘要

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具有优异储能特能及温度稳定性的电介质电容器是电子工业的理想选择。可用于脉冲功率系统的无铅弛豫铁电陶瓷电容器在低电场条件下表现出较低的有效储能密度（W_rec）。为了解决这一问题，采用传统固相法设计并制备了Ba_0.105Na_0.325Bi_0.325Sr_0.245TiO₃+x%K_0.5Na_0.5NbO₃（BNBST-x%KNN，摩尔分数，x=0、2、4、6、8、10、12）陶瓷，研究了不同KNN掺杂量对BNBST陶瓷的相结构、微观形貌、介电性能、储能特性和充放电特性的影响规律。结果表明：当x=6时，在较低电场（@140 kV/cm）下即可获得较大的有效储能密度（W_rec=1.8 J/cm³）和较高的储能效率（η=86%）。同时，BNBST-6%KNN陶瓷在-8~215 ℃的宽温度范围内获得了3 128±15%（@1 kHz）的高介电常数，并在80 kV/cm，20~180 ℃，10 000次电循环等条件下，其电储能均保持良好的温度、频率稳定性与抗疲劳特性。此外，BNBST-6%KNN陶瓷的功率密度P_D、放电密度W_d在20~140 ℃温度区间内均能维持良好的温度稳定性，说明其可作为低电场驱动高储能密度脉冲功率电容器制作的候选材料。

关键词

储能陶瓷 / 脉冲功率电容器 / 弛豫铁电体 / 钛酸铋钠 / 铌酸钾钠

Abstract

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Introduction

Dielectric materials have critical applications in many fields. Compared with electrochemical energy storage batteries, ceramic capacitors show outstanding competitive power performance in actual energy storage applications, such as diesel engine starters, camera flashlights, spacecraft, pulsed power weapons, and medical devices due to their ultra-fast charge/discharge capability and high-power density. However, with the development of electronic device integration and miniaturization, capacitors are required to have a high effective energy storage density (W_rec) under low electric field. The existing dielectric ceramic capacitors are difficult to meet the corresponding requirements, so it is urgent and significant to develop dielectric ceramic capacitors that can obtain high energy storage density under low voltage. In recent years, the co-design strategy has been used as a typical and effective method to enhance the energy storage performance of BNT, which is achieved by adding different kinds of ABO₃ perovskites and various doping ions. Co-design strategy improves energy storage properties by compositional design to induce the formation of polar nanoregions (PNRs) as a result of A/B site ion disordering or structural phase transitions. In this paper, KNN was added to BNBST ceramics to modify the internal crystal structure, and the effect of KNN on the phase structure, microstructure, dielectric properties, energy storage properties, ferroelectric stability and fast charge-discharge characteristics of BNBST ceramics were investigated.

Methods

As we know, high P_max, low P_r and high breakdown strengthen E_b are required for dielectric ceramics to achieve high W_rec. To obtain high energy storage density under a low electric field, we chose Ba_0.105Na_0.325Bi_0.325Sr_0.245TiO₃ (BNBST) with large P_max and high Curie temperature as the research object, the co-design strategy with the introduction of K_0.5Na_0.5NbO₃ was adopted to further destroy the ordered arrangement of A/B position ions, reduce their residual polarization intensity P_r, and optimize their electric polarization behavior.

Using solid-state method prepared Ba_0.105Na_0.325Bi_0.325Sr_0.245TiO₃+x%K_0.5Na_0.5NbO₃ (BNBST-x% KNN, mole fraction, x=0, 2, 4, 6, 8, 10, 12) ceramic samples. Bi₂O₃ (99.999%), K₂CO₃ (99%), BaCO₃ (99%), SrCO₃ (99%), Na₂CO₃ (99.8%), TiO₂ (99%), Nb₂O₅ (99.95%) were used as synthetic raw materials to prepare samples according to the following process: 1) Accurately weigh the ingredients according to the corresponding stoichiometric ratio, put them in the nylon ball mill tank for 24 h, dry, grind, and pass 80 mesh sieve; 2) Pre-burning after pressing into large sections, heating up to 850 ℃ with a heating rate of 5 ℃/min and holding for 3 h to exclude CO₂ and pre-synthesize the powder; 3) The large pieces are ground into powder, passed through an 80-mesh sieve, ball milling again for 24 h, drying, adding 5% concentration of PVA adhesive for granulation, pressing into a small disc with thickness of about 1 mm, diameter of about 13 mm (pressure (120±10) MPa); 4) The small disc was heated to 650 ℃ for 3 h to remove organic matter, and then heated to 1 240 ℃ for 2 h to sintering; 5) After polished and silvered, heating up 30 min at 650 ℃, and then various electrical properties are tested.

Results and discussion

All BNBST-x%KNN ceramics have a single perovskite pseudo-cubic phase structure, and no second phase is generated. The grain distribution of all ceramics is uniform and the density is good. When x=6, the optimized energy storage characteristics are obtained only at the low electric field of 140 kV/cm with W_rec=1.8 J/cm³ and η=86%. Whatmore, BNBST-6% KNN ceramics have TCC=±15% high dielectric constant (ε_r=3 128@125 ℃) and excellent temperature, frequency, cycle stability and fast charge-discharge characteristics in the temperature range of -8-215 ℃. The results show that BNBST-6%KNN ceramics can be used as a candidate material for pulsed power capacitors, and has obvious advantages in low electric field application.

Conclusions

The main innovation points of this paper are summarized as following. A collaborative design strategy with the introduction of K_0.5Na_0.5NbO₃ was used to further destroy the ordered arrangement of A/B ions and promote the formation of polar nanodomains (PNRs), under a certain electric field, PNRs can be transformed into long-range ordered ferroelectric domains, resulting in larger P_max. When the electric field is removed, the ferroelectric domains formed by PNRs will quickly break back to the initial state, resulting in smaller P_r. More importantly, "premature saturation" is delayed due to the appearance of PNRs, which can obtain hight larger P_max at low electric field, resulting in a high W_rec=1.8 J/cm³ at the low electric field of 140 kV/cm.

Key words

energy storage ceramics / pulse power capacitor / relaxor ferroelectric / bismuth sodium titanate / potassium sodium niobate

引用本文

李志鹏, 沈宗洋, 李妍, 王竹梅, 石旭海, 邓伟, 李月明. KNN对BNBST陶瓷储能特性的影响. 硅酸盐学报, 2024 , 52 (4) : 1217 -1228 . DOI: 10.14062/j.issn.0454-5648.20230750

Zhipeng LI, Zongyang SHEN, Yan LI, Zhumei WANG, Xuhai SHI, Wei DENG, Yueming LI. Effect of KNN on Energy Storage Performance of BNBST Ceramics[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (4) : 1217 -1228 . DOI: 10.14062/j.issn.0454-5648.20230750

基金

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国家自然科学基金(52267002)
江西省自然科学基金重点项目(20212ACB204010)
江西省教育厅科学技术研究重点项目(GJJ211301)

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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.0454-5648.20230750

接收时间：2023-09-28
首发时间：2026-10-22
出版时间：2024-04-20

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收稿日期：2023-09-28
修回日期：2023-10-24

基金

国家自然科学基金(52267002)

江西省自然科学基金重点项目(20212ACB204010)

江西省教育厅科学技术研究重点项目(GJJ211301)

作者信息

^1．景德镇陶瓷大学材料科学与工程学院，江西景德镇 333403

^2．先进陶瓷材料研究所，江西景德镇 333403

^3．中国轻工业功能陶瓷材料重点实验室，江西景德镇 333403

^4．江西省能量存储与转换陶瓷材料工程实验室，江西景德镇 333403

通讯作者:

沈宗洋（1979—），男，博士，教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230750

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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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