Ce 3+掺杂Na0.5Bi8.5Ti7O27铋层状陶瓷的结构与电性能研究

doi:10.15541/jim20180550

无机材料学报 ›› 2019, Vol. 34 ›› Issue (9): 997-1003.DOI: 10.15541/jim20180550

Ce ³⁺掺杂Na_0.5Bi_8.5Ti₇O₂₇铋层状陶瓷的结构与电性能研究

胡浩,江向平(),陈超,聂鑫,黄枭坤,苏春阳

景德镇陶瓷大学材料科学与工程学院, 江西省先进陶瓷材料重点实验室, 景德镇 333001

收稿日期:2018-11-26 修回日期:2019-01-16 出版日期:2019-09-20 网络出版日期:2019-05-29
作者简介:胡浩(1992-), 男, 硕士研究生. E-mail: 1980988765@qq.com
基金资助:
国家自然科学基金(51562014);国家自然科学基金(51602135);国家自然科学基金(51862016);国家自然科学基金(51762024);江西省自然科学基金(20171BAB216012);江西省教育厅科技项目(GJJ170789);江西省教育厅科技项目(GJJ170794);江西省教育厅科技项目(GJJ170804)

Influence of Ce ³⁺ Substitution on the Structure and Electrical Characteristics of Bismuth-layer Na_0.5Bi_8.5Ti₇O₂₇ Ceramics

HU Hao,JIANG Xiang-Ping(),CHEN Chao,NIE Xin,HUANG Xiao-Kun,SU Chun-Yang

Jiangxi Key Laboratory of Advanced Ceramic Materials, School of Material Science and Engineering, Jingdezhen Ceramic Institute, Jingdezhen 333001, China

Received:2018-11-26 Revised:2019-01-16 Published:2019-09-20 Online:2019-05-29
Supported by:
National Natural Science Foundation of China(51562014);National Natural Science Foundation of China(51602135);National Natural Science Foundation of China(51862016);National Natural Science Foundation of China(51762024);Natural Science Foundation of Jiangxi Province(20171BAB216012);Foundation of Jiangxi Provincial Education Department(GJJ170789);Foundation of Jiangxi Provincial Education Department(GJJ170794);Foundation of Jiangxi Provincial Education Department(GJJ170804)

摘要/Abstract

摘要：

采用固相法制备了Ce ³⁺掺杂的Na_0.5Bi_8.5-_xCe_xTi₇O₂₇(NBT-BIT-xCe, 0≤x≤0.1)共生铋层状无铅压电陶瓷, 研究了NBT-BIT-xCe陶瓷的结构和电学性能。研究结果表明所有陶瓷样品均为单一的铋层状结构, 随Ce ³⁺掺杂量的增加, 样品的畸变程度呈现上升趋势, 同时陶瓷晶粒的平均尺寸不断减小, 介温谱和差热分析结果表明样品的介电双峰均对应于陶瓷内部结构的铁电相变。Ce ³⁺掺杂可以显著减少陶瓷内部的氧空位浓度以及降低陶瓷的介电损耗, 提升陶瓷的压电常数(d₃₃), 当x=0.06时, 陶瓷的综合电性能最佳: 压电常数(d₃₃)达到27.5 pC/N, 居里温度(T_C)达到658.2 ℃, 介电损耗(tanδ)为0.39%。

关键词: 压电陶瓷, Na_0.5Bi_8.5Ti₇O₂₇, 氧空位, 激活能

Abstract:

The structure and electrical properties of Ce ³⁺-doped intergrowth bismuth layer-structured piezoelectric ceramics Na_0.5Bi_8.5-_xCe_xTi₇O₂₇(NBT-BIT-xCe, 0≤x≤0.1) prepared by conventional solid-state reaction process were systematically studied. In this study, all the ceramic samples were found to possess a single bismuth layer structure, and with the increase of x content, there is an increasing trend towards the lattice distortion of the sample, while the average grain size decreased. As demonstrated by dielectric spectrum and DSC method, two dielectric anomalies of the samples occur, which corresponds to ferroelectric phase transitions of the ceramics. And Ce ³⁺doping significantly reduces concentration of oxygen vacancy and dielectric loss in materials, improving piezoelectric constant (d₃₃) of ceramic samples. The resultant ceramics with x=0.06 reached the optimal performance, possessing a d₃₃ up to 27.5 pC/N with the Curie temperature of 658.2 ℃ and tanδ=0.39%.

Key words: piezoelectric ceramics, Na_0.5Bi_8.5Ti₇O₂₇, oxygen vacancy, activation energy

中图分类号:

TQ174

胡浩, 江向平, 陈超, 聂鑫, 黄枭坤, 苏春阳. Ce ³⁺掺杂Na_0.5Bi_8.5Ti₇O₂₇铋层状陶瓷的结构与电性能研究[J]. 无机材料学报, 2019, 34(9): 997-1003.

HU Hao, JIANG Xiang-Ping, CHEN Chao, NIE Xin, HUANG Xiao-Kun, SU Chun-Yang. Influence of Ce ³⁺ Substitution on the Structure and Electrical Characteristics of Bismuth-layer Na_0.5Bi_8.5Ti₇O₂₇ Ceramics[J]. Journal of Inorganic Materials, 2019, 34(9): 997-1003.

图/表 11

图1 NBT-BIT-xCe陶瓷样品的室温XRD图谱

Fig. 1 XRD patterns of NBT-BIT-xCe ceramics

图2 NBT-BIT-xCe陶瓷样品的Raman谱图

Fig. 2 Raman spectra of NBT-BIT-xCe ceramics

图3 NBT-BIT陶瓷XRD图谱Rietveld 精修结果

Fig. 3 Rietveld refinements for NBT-BIT ceramics

表1 NBT-BIT-xCe陶瓷样品的晶胞参数

Table 1 Lattice parameters of NBT-BIT-xCe ceramics

Compound	a/nm	b/nm	c/nm	V/nm³	Orthorhombicity
NBT-BIT	0.5421138	0.5449559	7.3766121	2.179259	0.005230
NBT-BIT-0.04Ce	0.5422069	0.5450802	7.3880188	2.183502	0.005290
NBT-BIT-0.06Ce	0.5420991	0.5451425	7.3788872	2.180618	0.005600
NBT-BIT-0.07Ce	0.5420621	0.5451272	7.3959427	2.185448	0.005640
NBT-BIT-0.08Ce	0.5425093	0.5456971	7.3701042	2.181888	0.005858
NBT-BIT-0.10Ce	0.5421451	0.5453683	7.3819908	2.182624	0.005930

图4 (a)陶瓷表面OH吸附示意图; (i)表面的M-OH, (ii)由破坏的M-O形成的M-OH, (iii)由表面氧空位形成的Vo-OH; (b)NBT-BIT陶瓷样品O1s窄扫高分辨XPS图谱

Fig. 4 (a) Diagram of OH adsorption on ceramic surface: (i) surface M-OH; (ii) M-OH formed from broken M-O; (iii) Vo-OH formed from surface oxygen vacancies; (b) high resolution O1s XPS spectra of NBT-BIT ceramics

表2 XPS曲线中OV和OL峰的参数

Table 2 Parameters of OV and OL peaks in XPS curves

Sample	O_V	O_L	O_V/O_L
NBT-BIT	76.10	23.90	3.18
NBT-BIT-0.06Ce	53.47	46.53	1.15

图5 NBT-BIT-xCe陶瓷样品的SEM照片和晶粒尺寸分布图

Fig. 5 SEM images and grain size distribution for NBT-BIT-xCe ceramic samples (a) x=0.00; (b) x=0.04; (c) x=0.06; (d) x=0.08; (e) x=0.10

图6 NBT-BIT陶瓷粉末的DSC曲线

Fig. 6 DSC spectra of NBT-BIT ceramic powder

图7 NBT-BIT-xCe陶瓷样品在100 kHz频率下介电常数和介电损耗随温度的变化曲线

Fig. 7 The curves of dielectric constant and dielectric loss varied with temperature for NBT-BIT-xCe ceramic samples at 100 kHz

图8 NBT-BIT-xCe陶瓷样品在不同温度下的复阻抗图

Fig. 8 Complex impedance plots of NBT-BIT-xCe ceramics at different temperatures (a) x=0.00; (b) x=0.04; (c) x=0.06; (d) x=0.07; (e) x=0.08; (f) x=0.10

图9 NBT-BIT-xCe陶瓷的压电常数和激活能随x的变化曲线

Fig. 9 The curves of piezoelectric constant and activation energy varied with x for NBT-BIT-xCe ceramic

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Ce ³⁺掺杂Na_0.5Bi_8.5Ti₇O₂₇铋层状陶瓷的结构与电性能研究

Influence of Ce ³⁺ Substitution on the Structure and Electrical Characteristics of Bismuth-layer Na_0.5Bi_8.5Ti₇O₂₇ Ceramics

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