0.94Na1/2Bi1/2TiO3-0.06BaTiO3:TiO2无铅复合陶瓷的结构及退极化温度研究

doi:10.15541/jim20180568

摘要/Abstract

摘要：

采用固相法将纳米TiO₂引入0.94Na_1/2Bi_1/2TiO₃-0.06BaTiO₃ (简称NBT-6BT)钙钛矿结构压电陶瓷晶界中, 成功制备出NBT-6BT: xTiO₂ (x=0, 0.05, 0.1, 0.2, 0.3) 0-3型复合结构陶瓷, 并系统地研究了掺杂TiO₂对陶瓷的结构及压电性能的影响。实验结果表明, 部分TiO₂进入晶格内部造成陶瓷单斜相Cc含量减少, 晶体对称性提高; 随着TiO₂的掺杂量的增加, 明显提高了NBT-6BT陶瓷的退极化温度。对NBT-6BT:0.1TiO₂样品, 在保持一定压电常数(69 pC/N)的前提下, 陶瓷的退极化温度相比纯NBT-6BT提升约88%, 此时介电损耗tanδ=0.044, 表明该材料是一种适用于更高温区间的新型无铅压电材料。

关键词: 压电陶瓷, NBT-6BT, 复合材料, 退极化

Abstract:

0.94Na_1/2Bi_1/2TiO₃-0.06BaTiO₃ (NBT-6BT) perovskite structure ceramics doped by nano-sized TiO₂, which stayed in the grain boundaries of NBT-6BT grains, were prepared by the solid-state method. NBT-6BT: xTiO₂ (x=0, 0.05, 0.1, 0.2, 0.3) 0-3 type composite structure ceramics were fabricated successfully and the effects of doped TiO₂ on structure and piezoelectric properties were investigated in detail. The results show that some TiO₂ enter into the lattice of NBT-6BT matrix, which result in a decrease of Cc phase content and an enhancement of crystal symmetry. The increasing amounts of TiO₂ significantly improve the depolarization temperature of NBT-6BT ceramics. After doping 0.1 mol of TiO₂, the depolarization temperature improves by 88%. The dielectric loss tanδ and piezoelectric coefficient d₃₃ are 0.044 and 99 pC/N, respectively, which indicates that this kind of ceramic is a new type of lead-free piezoelectric materials suitable for higher temperature range.

Key words: piezoceramic materials, NBT-6BT, composite structure, depolarization

中图分类号:

TQ174

苏春阳, 江向平, 陈超, 胡浩, 刘芳, 郑来奇. 0.94Na_1/2Bi_1/2TiO₃-0.06BaTiO₃:TiO₂无铅复合陶瓷的结构及退极化温度研究[J]. 无机材料学报, 2019, 34(10): 1085-1090.

SU Chun-Yang, JIANG Xiang-Ping, Chen Chao, Hu Hao, Liu fang, ZHENG Lai-Qi. Structural and Depolarization Temperature of 0.94Na_1/2Bi_1/2TiO₃-0.06BaTiO₃:TiO₂ Lead Free Composite Ceramics[J]. Journal of Inorganic Materials, 2019, 34(10): 1085-1090.

图/表 8

图1 室温下NBT-6BT: xTiO2复合陶瓷样品的XRD图谱

Fig. 1 Room temperature unpoled XRD patterns of NBT-6BT: xTiO2 composite ceramics (a) 2θ=10°-80°; (b) 2θ=36°-50°

图2 NBT-6BT: 0.1TiO2复合陶瓷样品的SEM照片(a)和EDS图谱(b~e)

Fig. 2 SEM (a) and EDS (b-e) images of NBT-6BT: xTiO2 composite ceramic

图3 室温下NBT-6BT: xTiO2复合陶瓷样品的拉曼光谱图

Fig. 3 Raman spectra of NBT-6BT: xTiO2 composite ceramics at room temperature

图4 NBT-6BT: xTiO2复合陶瓷样品的拉曼模频率随组分的变化

Fig. 4 Raman mode frequencies as a function of compositions for NBT-6BT: xTiO2 composite ceramics

图5 不同组分NBT-6BT: xTiO2复合陶瓷样品的精修结果

Fig. 5 Rietveld structural refinement plots of NBT-6BT: xTiO2 composite ceramics at room temperature (a) x=0.0; (b) x=0.2

表1 NBT-6BT: xTiO2陶瓷的相含量与晶胞参数

Table 1 Phase fraction and lattice parameters of structural refinement plots of NBT-6BT: xTiO2 samples originating from Rietveld structural refinement

Sample/mole	Phase fraction/wt%		Lattice parameters			V/nm³
Sample/mole	Phase fraction/wt%		a/nm	b/nm	c/nm	V/nm³
x=0.0	R3c	20.84	0.5564	0.5564	1.3674	0.366654
x=0.0	Cc	79.16	0.9559	0.5533	0.5530	0.238807
x=0.05	R3c	32.64	0.5542	0.5542	1.3648	0.363140
x=0.05	Cc	67.36	0.9524	0.5504	0.5537	0.237428
x=0.1	R3c	33.77	0.5517	0.5517	1.3616	0.358981
x=0.1	Cc	66.23	0.9508	0.5492	0.5533	0.236407
x=0.2	R3c	42.84	0.5531	0.5531	1.3636	0.361341
x=0.2	Cc	57.16	0.9517	0.5490	0.5531	0.236311
x=0.3	R3c	58.92	0.5503	0.5503	1.3443	0.352637
x=0.3	Cc	41.08	0.9589	0.5488	0.5556	0.237663

图6 (a~d)极化后x=0, 0.1, 0.2,0.3的NBT-6BT: xTiO2陶瓷样品的介电常数εr和介电损耗tanδ随温度的变化关系; (e)Td和tanδ随组分的变化关系

Fig. 6 Temperature dependence (a-d) of the dielectric constant εr and dielectric loss tanδ of poled NBT-6BT: xTiO2 composite ceramics with x=0, 0.1, 0.2 and 0.3, and Composition dependence (e) of Td and dielectric loss tanδ

图7 室温下NBT-6BT: xTiO2陶瓷样品压电常数随组分的变化(a)和NBT-6BT: xTiO2 复合陶瓷样品的压电常数随温度的变化(b)

Fig. 7 Piezoelectric coefficient (d33) of NBT-6BT: xTiO2 composite ceramics at room temperature (a) and temperature dependence of d33 of composite ceramics (b)

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0.94Na_1/2Bi_1/2TiO₃-0.06BaTiO₃:TiO₂无铅复合陶瓷的结构及退极化温度研究

Structural and Depolarization Temperature of 0.94Na_1/2Bi_1/2TiO₃-0.06BaTiO₃:TiO₂ Lead Free Composite Ceramics

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