NaCu3Ti3Sb0.5Ta0.5O12陶瓷的高介电性质及相关机制的研究

doi:10.15541/jim20160702

无机材料学报 ›› 2017, Vol. 32 ›› Issue (10): 1029-1035.DOI: 10.15541/jim20160702 CSTR: 32189.14.10.15541/jim20160702

NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂陶瓷的高介电性质及相关机制的研究

杨帅^{1, 2}, 徐攀攀³, 王明文^{1, 2}, 郝文涛^{1, 2}, 孙礼^{1, 2}, 曹恩思^{1, 2}, 张雍家^{1, 2}

(1. 太原理工大学新型传感器与智能控制教育部重点实验室, 太原 030024; 2. 太原理工大学物理与光电工程学院, 晋中 030600; 3. 太原理工大学材料科学与工程学院, 太原 030024)

收稿日期:2016-12-29 修回日期:2017-03-07 出版日期:2017-10-20 网络出版日期:2017-09-21
作者简介:杨帅(1993–), 男, 硕士研究生. E-mail: 635097631@qq.com
基金资助:
国家自然科学基金(51602214, 11404236, 11604234)

High Dielectric-permittivity Properties and Relevant Mechanism of NaCu₃Ti₃Sb_0.5Nb_0.5O₁₂ Ceramics

YANG Shuai^1,2, XU Pan-Pan³, WANG Ming-Wen^1,2, HAO Wen-Tao^1,2, SUN Li^1,2, CAO En-Si^1,2, ZHANG Yong-Jia^1,2

(1. Key Laboratory of Advanced Transducers and Intelligent Control Systems, Taiyuan University of Technology, Taiyuan 030024, China; 2. College of Physics and Optoelectronics, Taiyuan University of Technology, Jinzhong 030600, China; 3. College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China)

Received:2016-12-29 Revised:2017-03-07 Published:2017-10-20 Online:2017-09-21
About author:YANG Shuai. E-mail: 635097631@qq.com
Supported by:
National Natural Science Foundation of China(51602214, 11404236, 11604234)

摘要/Abstract

摘要：

在不同烧结温度下, 利用传统的固相反应工艺制备了一系列NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂陶瓷, 系统测试了它们的晶体结构、微观结构、介电性质和复阻抗谱。结果显示, 所有的NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂陶瓷的主相都呈现类钙钛矿结构, 介电性质随烧结温度变化很大。高于1020℃烧结的陶瓷的室温相对介电常数大于3000, 具有高介电性质。复阻抗谱显示, NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂陶瓷的电学分布不均匀, 由绝缘性的晶界和半导性的晶界组成。通过XRD和XPS测试发现, 在陶瓷中观察到了CuO第二相和Cu、Ti、Sb、Ta离子的变价。因此, 利用内阻挡层电容效应可以解释NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂陶瓷的高介电性质。

关键词: NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂, 高介电性质, CuO第二相, 元素变价, 内阻挡层电容效应

Abstract:

A series of NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂ ceramics were prepared by conventional solid-state reaction technique at different sintering temperatures. Their crystalline structures, microstructures, dielectric properties and complex impedance were systematically investigated. All the ceramics show the main phase of perovskite-related crystallographic structure, and their dielectric properties change significantly with sintering temperature. Those ceramics sintered above 1020°C perform high dielectric-permittivity properties with ε' over 3000. Impedance spectroscopy analysis reveals that NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂ ceramics are electrically heterogeneous and composed of semiconducting grains and insulating grain boundaries. Moreover, a small amount of CuO secondary phase and Cu²⁺/Cu⁺, Ti⁴⁺/Ti³⁺, Sb⁵⁺/Sb³⁺ and Ta⁵⁺/Ta³⁺ aliovalences are found to exist in NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂ ceramics through XRD and XPS analysis. Internal barrier layer capacitance effect suggests the origin of the high dielectric-permittivity properties in NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂ ceramics.

Key words: NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂, high dielectric-permittivity properties, CuO secondary phase, aliovalences, internal barrier layer capacitance effect

中图分类号:

TM283

杨帅, 徐攀攀, 王明文, 郝文涛, 孙礼, 曹恩思, 张雍家. NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂陶瓷的高介电性质及相关机制的研究[J]. 无机材料学报, 2017, 32(10): 1029-1035.

YANG Shuai, XU Pan-Pan, WANG Ming-Wen, HAO Wen-Tao, SUN Li, CAO En-Si, ZHANG Yong-Jia. High Dielectric-permittivity Properties and Relevant Mechanism of NaCu₃Ti₃Sb_0.5Nb_0.5O₁₂ Ceramics[J]. Journal of Inorganic Materials, 2017, 32(10): 1029-1035.

图/表 6

图1 NCTSTO陶瓷的XRD图谱

Fig. 1 XRD patterns of the various NCTSTO ceramics

图2 不同温度烧结的NCTSTO陶瓷的断面SEM照片

Fig. 2 Fractured cross-sectional SEM images of the NCTSTO ceramics sintered at different temperatures(a) 1020℃; (b) 1040℃; (c) 1060℃; (d) 1080℃; (e) 1100℃

图3 不同温度烧结的NCTSTO陶瓷的室温介电频谱

Fig. 3 Room temperature dielectric dispersion spectra of the NCTSTO ceramics sintered at different temperatures

图4 1060℃烧结的NCTSTO陶瓷在不同温度下的介电频谱和特定频率下的介电温谱

Fig. 4 (a) Dielectric dispersion change with temperature and (b) variation of ε' with temperature of the NCTSTO ceramic sintered at 1060℃

图5 1060℃烧结的NCTSTO陶瓷在(a)室温, (b)100℃, (c) 200℃和(d)300℃的复阻抗谱

Fig. 5 Complex impedance of NCTSTO ceramic sintered at 1060℃ and measured at (a) room temperature, (b) 100℃, (c) 200℃ and (d) 300℃

图6 1060℃烧结的NCTSTO陶瓷的(a)Cu-2p、(b)Ti-2p、(c)Sb-3d和(d)Ta-4f的XPS图谱

Fig. 6 (a) Cu-2p peaks, (b) Ti-2p peaks, (c) Sb-3d peaks and (d) Ta-4f peaks of XPS spectra of the NCTSTO ceramic sintered at 1060℃

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NaCu₃Ti₃Sb_0.5Ta_0.5O₁₂陶瓷的高介电性质及相关机制的研究

High Dielectric-permittivity Properties and Relevant Mechanism of NaCu₃Ti₃Sb_0.5Nb_0.5O₁₂ Ceramics

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