层状结构第二相增强BiFeO3-BaTiO3陶瓷电阻率研究

doi:10.15541/jim20230167

无机材料学报 ›› 2023, Vol. 38 ›› Issue (12): 1420-1426.DOI: 10.15541/jim20230167 CSTR: 32189.14.10.15541/jim20230167

所属专题：【信息功能】介电、铁电、压电材料（202409）；【信息功能】纪念殷之文先生诞辰105周年虚拟学术专辑

层状结构第二相增强BiFeO₃-BaTiO₃陶瓷电阻率研究

康文烁¹^,²(), 郭晓杰¹^,², 邹凯¹^,², 赵祥永³, 周志勇¹, 梁瑞虹¹()

1.中国科学院上海硅酸盐研究所, 中国科学院无机功能材料与器件重点实验室, 上海 200050
2.中国科学院大学, 北京 100049
3.上海师范大学光电子材料与器件重点实验室, 上海 200234

收稿日期:2023-04-06 修回日期:2023-05-10 出版日期:2023-09-12 网络出版日期:2023-09-12
通讯作者: 梁瑞虹, 研究员. E-mail: liangruihong@mail.sic.ac.cn
作者简介:康文烁(1994-), 男, 博士研究生. E-mail: kangwenshuo20@mails.ucas.ac.cn
基金资助:
国家自然科学基金(51972321);国家自然科学基金(U2241242);国家重点研发计划(2022YFF0709702);中国科学院先导计划(XDA2203003)

Enhanced Resistivity Induced by the Second Phase with Layered Structure in BiFeO₃-BaTiO₃ Ceramics

KANG Wenshuo¹^,²(), GUO Xiaojie¹^,², ZOU Kai¹^,², ZHAO Xiangyong³, ZHOU Zhiyong¹, LIANG Ruihong¹()

1. Key Laboratory of Inorganic Functional Materials and Devices, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
2. University of Chinese Academy of Sciences, Beijing 100049, China
3. Key Laboratory of Optoelectronic Material and Device, Shanghai Normal University, Shanghai 200234, China

Received:2023-04-06 Revised:2023-05-10 Published:2023-09-12 Online:2023-09-12
Contact: LIANG Ruihong, professor. E-mail: liangruihong@mail.sic.ac.cn
About author:KANG Wenshuo (1994-), male, PhD candidate. E-mail: kangwenshuo20@mails.ucas.ac.cn
Supported by:
National Natural Science Foundation of China(51972321);National Natural Science Foundation of China(U2241242);National Key Research and Development Program of China(2022YFF0709702);Pilot Technology for Chinese Academy of Sciences(XDA2203003)

摘要/Abstract

摘要：

BiFeO₃-BaTiO₃(BF-BT)陶瓷兼具高居里温度和优异的压电性能, 在高温压电传感器和驱动器等部件具有广泛的应用前景。BF-BT陶瓷在高温环境下电阻率较低, 易造成器件高温性能恶化甚至失效。因此, 改善BF-BT陶瓷电阻性能是应用推广必须解决的关键问题。作为一种铁酸盐, 其电阻率很难通过掺杂改性等常规方法进行改善。本研究在BF-BT陶瓷体系中发现一种电阻率异常升高的现象, 并证实这与样品中的第二相Bi₂₅FeO₄₀有关。显微结构分析表明, 该第二相具有一种特殊的层状周期性结构, 其中每三排原子构成一个周期, 而缺陷大多集中在其中一层原子当中。本研究采用传统固相法成功地制备出纯相的Bi₂₅FeO₄₀, 将其作为外添加剂加入到0.70BF-0.30BT组分中, 使基体组分在300 ℃的电阻率从1.03 MΩ·cm提高到4.33 MΩ·cm。此外, COMSOL仿真模拟的结果证实, 通过引入该第二相可以将0.67BF-0.33BT组分电阻率提高一个数量级。根据能量过滤效应, 这种特殊的结构具有高能垒, 可以阻碍载流子迁移, 从而提高BF-BT陶瓷电阻率。本工作为改善BF-BT陶瓷电阻率提供了一种切实可行的方法。

关键词: 电阻率, 载流子迁移, BiFeO₃-BaTiO₃陶瓷, 仿真模拟

Abstract:

BiFeO₃-BaTiO₃ (BF-BT) ceramics possess both high Curie temperature and excellent piezoelectric properties, and have a quite wide application prospects in high-temperature piezoelectric sensors and actuators. However, the resistivity of BF-BT ceramics is too low at high-temperature, which can lead to deterioration or even failure of the device's high-temperature performance. Therefore, improving the resistance performance of BF-BT ceramics is the key issue that must be addressed before its application. However, as a type of ferrite, it is difficult to improve resistivity through conventional methods, such as doping modification and optimizing sintering system. In this work, an abnormal increase in resistivity was discovered in BF-BT ceramics, which was confirmed to be related to the second phase Bi₂₅FeO₄₀. Microstructural analysis shows that the second phase has a special layered periodic structure, in which every three rows of atoms constitute a period, and most defects concentrate in one layer of atoms. The pure Bi₂₅FeO₄₀ was successfully synthesized using traditional solid phase method and introduced as an additive into the 0.70BF-0.30BT component, which can increase the resistivity at 300 ℃ from 1.03 MΩ·cm to 4.33 MΩ·cm. In addition, the results of COMSOL simulation confirm that introducing this second phase can increase the resistivity of the 0.67BF-0.33BT component by one order of magnitude. According to the energy filtering effect, this special structure with high energy barriers can prevent carrier migration and improve the resistivity of BF-BT ceramics. This work provides a practical and feasible method for improving the resistivity of BF-BT ceramics.

Key words: resistivity, carrier migration, BiFeO₃-BaTiO₃ ceramics, simulation confirm

中图分类号:

TQ174

康文烁, 郭晓杰, 邹凯, 赵祥永, 周志勇, 梁瑞虹. 层状结构第二相增强BiFeO₃-BaTiO₃陶瓷电阻率研究[J]. 无机材料学报, 2023, 38(12): 1420-1426.

KANG Wenshuo, GUO Xiaojie, ZOU Kai, ZHAO Xiangyong, ZHOU Zhiyong, LIANG Ruihong. Enhanced Resistivity Induced by the Second Phase with Layered Structure in BiFeO₃-BaTiO₃ Ceramics[J]. Journal of Inorganic Materials, 2023, 38(12): 1420-1426.

图/表 7

图1 (1−x)BF-xBT陶瓷烧结后的样品在2θ=15°~80°范围的XRD图谱(a)以及2θ=39°附近衍射峰的放大图(b)

Fig. 1 XRD patterns of sintered (1−x)BF-xBT samples in the range of 2θ=15°-80° (a) and the magnified image at 2θ=39° (b)

图2 (1−x)BF-xBT陶瓷样品自然断面的背散射形貌(a~d)和x=0.10组分抛光的表面形貌(e)以及面扫能谱(f, g)

Fig. 2 Backscattered electron images of the cross-section for (1−x)BF-xBT ceramics (a-d), polished surface image for x=0.10 composition (e), and EDS mapping of Bi (f) and Fe (g)

图3 (1−x)BF-xBT陶瓷的直流电阻率(a)、复阻抗数据(b)以及x=0.10组分两段圆弧的拟合结果(c)

Fig. 3 DC resistivity versus temperature of (1−x)BF-xBT ceramics (a), Nyquist plots at 300 ℃ (b), and grain boundary resistivity obtained from fitting Cole-Cole plots of x=0.10 composition (c)

图4 x=0.10组分在不同温度的模量频谱图(a)以及从中提取的电容值随温度的变化关系(b)

Fig. 4 Modulus plots versus temperature for x=0.10 composition (a), and capacitance values extracted from modulus peaks at different temperatures (b)

图5 第二相[111]取向的TEM图像(a)、选区电子衍射(b)、高分辨TEM图像(c)以及高角环形暗场像(d,e)，(e)中插图为绿色框中的原子柱强度

Fig. 5 TEM image (a), selected-area electron diffraction (b) and high-resolution TEM image (c) at [111] of second phase, and high-angle annular dark-field images in [111] zone axis (d, e) with illustration in (e) showing intensity plot of atoms in green box

图6 对含有第二相的BF-BT陶瓷电阻性能的仿真模拟(a)、第二相提高电阻率的作用机理(b)和Schottky能垒模型(c)

Fig. 6 Resistivity simulation of the BF-BT composite ceramic at 300 ℃ (a), schematic diagram describing carrier migration (b), and Schottky barrier model (c)

图7 0.70BF-0.30BT纯组分样品加入Bi25FeO40前(a)后(b)的背散射形貌、电阻率随温度的变化关系(c)以及文献报道的0.70BF-0.30BT在300 ℃的电阻率

Fig. 7 Backscatter morphologies of the polished 0.70BF-0.30BT pure component sample (a) and the sample modified with the second phase (b), resistivities of two samples versus temperature (c), and summary results of the resistivities of 0.70BF-0.30BT at 300 ℃ reported in the literatures (d)

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层状结构第二相增强BiFeO₃-BaTiO₃陶瓷电阻率研究

Enhanced Resistivity Induced by the Second Phase with Layered Structure in BiFeO₃-BaTiO₃ Ceramics

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