钙钛矿型(La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3高熵氧化物陶瓷的制备及性能研究

doi:10.15541/jim20200500

无机材料学报 ›› 2021, Vol. 36 ›› Issue (4): 379-385.DOI: 10.15541/jim20200500 CSTR: 32189.14.10.15541/jim20200500

钙钛矿型(La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃高熵氧化物陶瓷的制备及性能研究

张晓燕¹^,²^,³(), 刘馨玥¹^,², 闫金华¹^,², 谷耀行¹^,², 齐西伟³^,⁴()

1.东北大学材料科学与工程学院, 沈阳 110819
2.东北大学秦皇岛分校资源与材料学院, 秦皇岛 066004
3.河北省电介质与电解质功能材料重点实验室, 秦皇岛 066004
4.华北理工大学冶金与能源学院, 唐山 063210

收稿日期:2020-08-28 修回日期:2020-09-29 出版日期:2021-04-20 网络出版日期:2020-10-30
通讯作者: 齐西伟, 教授. E-mail: qixiwei@mail.neu.edu.cn
作者简介:张晓燕(1982-), 女, 副教授. E-mail: xyaaa2005@163.com
基金资助:
国家自然科学基金(51972048)

Preparation and Property of High Entropy (La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ Perovskite Ceramics

ZHANG Xiaoyan¹^,²^,³(), LIU Xinyue¹^,², YAN Jinhua¹^,², GU Yaohang¹^,², QI Xiwei³^,⁴()

1. School of Materials Science and Engineering, Northeastern University, Shenyang 110819, China
2. School of Resources and Materials, Northeastern University at Qinhuangdao Branch, Qinhuangdao 066004, China
3. Key Laboratory of Dielectric and Electrolyte Functional Material, Qinhuangdao 066004, China
4. College of Metallurgy and Energy, North China of Science and Technology, Tangshan 063210, China

Received:2020-08-28 Revised:2020-09-29 Published:2021-04-20 Online:2020-10-30
Contact: QI Xiwei, professor. E-mail: qixiwei@mail.neu.edu.cn
About author:ZHANG Xiaoyan(1982-), female, associate professor. E-mail: xyaaa2005@163.com
Supported by:
Natural Science Foundation of China(51972048)

摘要/Abstract

摘要：

高熵陶瓷是近年来在高熵合金基础上逐渐发展起来的一种新的陶瓷材料体系, 它的出现为开发具有优异性能的非金属材料提供了新的理念和路线。本研究采用固相烧结法制备A位等摩尔比的钙钛矿型高熵氧化物陶瓷(La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃, 并探索了烧结温度对高熵陶瓷的物相结构及电学性能的影响。结果表明, 陶瓷经现有温度烧结后均表现为立方钙钛矿结构, 并且展现出良好的绝缘性, 其漏电流密度在10^-8~10^-6 A/cm²数量级。尽管随烧结温度的升高, 陶瓷的晶粒尺寸不断增大, 但该显微结构与介电性能的关联并不显著。当烧结温度为1350 ℃时, 介电常数出现最大值, 在频率为100 Hz下, 介电常数约为230。同时, 该高熵陶瓷的介电温谱表明陶瓷存在弛豫行为, 其介电常数的弛豫峰随着频率的增加向高温方向移动。

关键词: 高熵陶瓷, 钙钛矿, 介电性能

Abstract:

High entropy ceramic is a kind of ceramic developed based on the high entropy alloy in recent years. The appearance of high entropy ceramics provides a new concept and route for developing non-metallic materials with excellent properties. In present work, a series of high-entropy ceramics with a molar ratio of A site—(La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ were successfully synthesized by solid state reaction. The effects of sintering temperature on phase, microstructure and electric properties were investigated. Results show that the high-entropy ceramics sintered at current temperatures are of cubic perovskite structure, and exhibit excellent insulation, with low leakage current density of J value around 10^-8-10^-6 A/cm². Although the grain size increases with the increase of sintering temperature, the correlation between microstructure and dielectric properties of (La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ ceramics is not significant. The dielectric constant reaches its maximum value at 1350 ℃, with the value of 230 at the frequency of 100 Hz. Meanwhile, this high-entropy ceramic has relaxation behavior, and the relaxation peak of the permittivity moves towards high temperature with the increase of frequency.

Key words: high-entropy ceramics, perovskite, dielectric property

中图分类号:

TQ174

张晓燕, 刘馨玥, 闫金华, 谷耀行, 齐西伟. 钙钛矿型(La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃高熵氧化物陶瓷的制备及性能研究[J]. 无机材料学报, 2021, 36(4): 379-385.

ZHANG Xiaoyan, LIU Xinyue, YAN Jinhua, GU Yaohang, QI Xiwei. Preparation and Property of High Entropy (La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ Perovskite Ceramics[J]. Journal of Inorganic Materials, 2021, 36(4): 379-385.

图/表 8

图1 在不同温度烧结(La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3高熵陶瓷的XRD图谱

Fig. 1 XRD patterns of high entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2) TiO3 ceramic sintered at different temperatures

图2 (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3高熵陶瓷的高分辨TEM照片

Fig. 2 HRTEM image of high entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2) TiO3 ceramic sintered at 1350 ℃

图3 不同温度烧结(La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3高熵陶瓷的SEM照片

Fig. 3 SEM images of high entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic sintered at different temperatures (a) 1250 ℃; (b) 1300 ℃; (c) 1350 ℃; (d)1400 ℃; (e) 1450 ℃; (f) 1500 ℃

图4 (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3高熵陶瓷的密度和相对密度随烧结温度的变化曲线

Fig. 4 Variation of density and relative density of high entropy (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic sintered at different temperatures

图5 (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3陶瓷Ti2p(a)和O1s(b)的XPS谱图

Fig. 5 (a) Ti2p and (b) O1s XPS spectra of (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic

图6 室温下(La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3陶瓷的(a)介电常数和(b)介电损耗随频率的变化关系

Fig. 6 Frequency dependences of dielectric constant εr (a) and dielectric loss tanδ (b) of (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic

图7 1350 ℃烧结(La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3陶瓷的介电常数与介电损耗随温度的变化关系

Fig. 7 Temperature dependence of dielectric constant and dielectric loss of (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramic sintered at 1350 ℃

图8 不同温度烧结(La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3陶瓷的漏电流曲线

Fig. 8 Leakage current density of (La0.2Li0.2Ba0.2Sr0.2Ca0.2)TiO3 ceramics sintered at different temperatures (a) J-E curves; (b) lnJ-lnE curves

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钙钛矿型(La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃高熵氧化物陶瓷的制备及性能研究

Preparation and Property of High Entropy (La_0.2Li_0.2Ba_0.2Sr_0.2Ca_0.2)TiO₃ Perovskite Ceramics

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