晶粒尺寸对细晶钛酸钡陶瓷介电、压电和铁电性能的影响

doi:10.15541/jim20170289

无机材料学报 ›› 2018, Vol. 33 ›› Issue (7): 767-772.DOI: 10.15541/jim20170289 CSTR: 32189.14.10.15541/jim20170289

晶粒尺寸对细晶钛酸钡陶瓷介电、压电和铁电性能的影响

黄咏安, 路标, 邹艺轩, 李丹丹, 姚英邦, 陶涛, 梁波, 鲁圣国

广东工业大学材料与能源学院, 广东省智能材料和能量转化器件工程技术研究中心, 广东省功能软凝聚态物质重点实验室, 广州 510006

收稿日期:2017-06-08 修回日期:2017-11-08 出版日期:2018-07-10 网络出版日期:2018-06-19
作者简介:黄咏安(1991-), 男, 硕士研究生. E-mail: wangyongan_gdut@163.com
基金资助:
国家自然科学基金委-广东省联合基金(U1501246);国家自然科学基金(51372042);广东省自然科学基金重大基础研究培育项目(2015A030308004);The Guangdong Joint Funds from the National Science Foundation of China (U1501246);National Natural Science Foundation of China (51372042);Guangdong Natural Science Foundation (2015A030308004)

Grain Size Effect on Dielectric, Piezoelectric and Ferroelectric Property of BaTiO₃ Ceramics with Fine Grains

HUANG Yong-An, LU Biao, ZOU Yi-Xuan, LI Dan-Dan, YAO Ying-Bang, TAO Tao, LIANG Bo, LU Sheng-Guo

Guangdong Provincial Key Laboratory of Functional Soft Condensed Matter, Guangdong Provincial Research Center on Smart Materials and Energy Conversion Devices, School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China

Received:2017-06-08 Revised:2017-11-08 Published:2018-07-10 Online:2018-06-19
About author:HUANG Yong-An. E-mail: wangyongan_gdut@163.com

摘要/Abstract

摘要：

以采用水热法制备的BaTiO₃粉体作为原料, 利用普通烧结法和两步烧结法制备出晶粒尺寸为0.25~10.15 μm的BaTiO₃陶瓷, 研究了晶粒尺寸效应对BaTiO₃陶瓷的介电、压电以及铁电性能的影响。结果表明: BaTiO₃陶瓷的四方相含量随着陶瓷晶粒尺寸的增大而增加; 当晶粒尺寸在1 μm以上时, 室温相对介电常数(ε° )和压电系数(d₃₃)随着晶粒尺寸的减小而增大, 并在晶粒尺寸为1.12 μm时分别达到最大值5628和279 pC/N, 然后两者随着晶粒尺寸的进一步减小而迅速下降。BaTiO₃陶瓷的剩余极化强度P_r随晶粒尺寸的增大而提高, 而矫顽场E_c却呈现出相反的趋势。晶粒尺寸对介电性能和压电性能的影响是由于90°电畴尺寸和晶界数量的变化。晶粒的晶体场和晶粒表面钉扎作用的变化影响了电畴, 进而改变电滞回线。

关键词: 钛酸钡, 晶粒尺寸, 两步烧结, 介电, 压电, 铁电

Abstract:

A series of highly dense barium titanate (BaTiO₃) ceramics with average grain size ranging from 0.25 μm to 10.15 μm were prepared by either conventional sintering or a two-step sintering method, using ultrafine BaTiO₃powders prepared by hydrothermal approach. The impact of grain size on dielectric, piezoelectric and ferroelectric properties of BaTiO₃ ceramics was investigated. Results indicate that the tetragonal phase of BaTiO₃ ceramics increases with the increase of grain size. When the averaged grain size is above 1 μm, the relative dielectric constant (ε°) and piezoelectric coefficient (d₃₃) at room temperature increase firstly with the decrease of grain size, with the maximum values of 5628 and 279 pC/N, respectively, at the grain size of 1.12 μm, and then decrease rapidly with further decrease of the grain size. The remanent polarization P_rof BaTiO₃ceramics rises with the increase of grain size, but the coercive field E_c exhibits opposite tendency. The variation of dielectric and piezoelectric properties resulted from the change of grain size is regarded as the impact of 90° domain size and the number of the grain boundaries, while the change of hysteresis loops is due to the change of the crystal field in the grains and the “pinning” effect of the surface layer on the grains.

Key words: barium titanate, grain size, two-step sintering, dielectricity, piezoelectricity, ferroelectricity

中图分类号:

TQ174

黄咏安, 路标, 邹艺轩, 李丹丹, 姚英邦, 陶涛, 梁波, 鲁圣国. 晶粒尺寸对细晶钛酸钡陶瓷介电、压电和铁电性能的影响[J]. 无机材料学报, 2018, 33(7): 767-772.

HUANG Yong-An, LU Biao, ZOU Yi-Xuan, LI Dan-Dan, YAO Ying-Bang, TAO Tao, LIANG Bo, LU Sheng-Guo. Grain Size Effect on Dielectric, Piezoelectric and Ferroelectric Property of BaTiO₃ Ceramics with Fine Grains[J]. Journal of Inorganic Materials, 2018, 33(7): 767-772.

图/表 9

表1 不同烧结方法制备的BaTiO3陶瓷的相对密度及平均晶粒尺寸

Table 1 Relative density and average grain size of BaTiO3 ceramics prepared by different sintering methods

T₁/℃	t₁/h	T₂/℃	t₂/h	ρ_o/%	GS/μm
1250	0	800	15	95.1	0.25
1250	0	850	15	95.6	0.34
1250	0	950	15	96.2	0.48
1275	0	950	15	96.9	0.76
1300	0	950	15	97.5	1.12
1250	3.0	0	0	97.3	2.40
1275	2.5	0	0	97.8	4.61
1300	3.0	0	0	98.2	7.24
1325	3.0	0	0	98.3	10.15

图1 不同晶粒尺寸的BaTiO3陶瓷的SEM照片

Fig. 1 SEM images of BaTiO3 ceramics with different grain sizes(a) 0.25 μm; (b) 0.34 μm; (c) 0.48 μm; (d) 0.76 μm; (e) 1.12 μm; (f) 2.4 μm; (g) 4.61 μm; (h) 7.24 μm; (i) 10.15 μm

图2 (a)不同晶粒尺寸BaTiO3陶瓷的XRD图谱和(b)2θ=44.5°~46°的局部放大XRD图谱

Fig. 2 (a) XRD patterns of BaTiO3 ceramics with different grain sizes and (b) the magnification of (002)/(200) diffraction peaks

图3 BaTiO3陶瓷的c/a比与晶粒尺寸的关系

Fig. 3 c/a ratio as a function of grain size (GS) for BaTiO3 ceramics

图4 不同晶粒尺寸BaTiO3陶瓷的介电温谱

Fig. 4 Dielectric constant as a function of temperature for BaTiO3 ceramics with different grain sizes

图5 BaTiO3陶瓷的TO-T和TT-C随晶粒大小的变化关系

Fig. 5 TO-T and TT-C as a function of grain size for BaTiO3 ceramics

图6 BaTiO3陶瓷的压电常数d33随晶粒尺寸的变化关系

Fig. 6 Piezoelectric constant d33 as a function of grain size for BaTiO3 ceramics

图7 室温下不同晶粒尺寸BaTiO3陶瓷的电滞回线

Fig. 7 P-E hysteresis loops of BaTiO3 ceramics with different grain sizes at room temperature

图8 剩余极化强度Pr、矫顽场Ec与陶瓷晶粒尺寸的关系

Fig. 8 Remanent polarization Pr, coercive field Ec as a function of the grain size for BaTiO3 ceramics

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晶粒尺寸对细晶钛酸钡陶瓷介电、压电和铁电性能的影响

Grain Size Effect on Dielectric, Piezoelectric and Ferroelectric Property of BaTiO₃ Ceramics with Fine Grains

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晶粒尺寸对细晶钛酸钡陶瓷介电、压电和铁电性能的影响

Grain Size Effect on Dielectric, Piezoelectric and Ferroelectric Property of BaTiO3 Ceramics with Fine Grains

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Grain Size Effect on Dielectric, Piezoelectric and Ferroelectric Property of BaTiO₃ Ceramics with Fine Grains