煅烧温度对Li0.33La0.56TiO3固态离子电容器性能的影响

doi:10.15541/jim20180049

无机材料学报 ›› 2018, Vol. 33 ›› Issue (10): 1077-1082.DOI: 10.15541/jim20180049

煅烧温度对Li_0.33La_0.56TiO₃固态离子电容器性能的影响

卢东亮^1,2, 代广周¹, 姚英邦¹, 陶涛¹, 梁波¹, 鲁圣国¹

1.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, 广东省软物质重点实验室, 广州 510006;
2.广东环境保护工程职业学院佛山 528216

收稿日期:2018-01-29 修回日期:2018-04-03 出版日期:2018-10-20 网络出版日期:2018-09-25
作者简介:卢东亮(1985-), 男, 博士研究生. E-mail: 327560923@qq.com
基金资助:
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);国家自然科学基金委-广东省联合基金(U1501246)

Influence of Calcining Temperature on the Property of Li_0.33La_0.56TiO₃Solid-state Ionic Capacitor

LU Dong-Liang^1,2, DAI Guang-Zhou¹, YAO Ying-Bang¹, TAO Tao¹, LIANG Bo¹, LU Sheng-Guo¹

1.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;
2. Guangdong Polytechnic of Environmental Protection Engineering, Foshan 528216, China

Received:2018-01-29 Revised:2018-04-03 Published:2018-10-20 Online:2018-09-25
About author:LU Dong-Liang. E-mail: 327560923@qq.com
Supported by:
Natural Science Foundation of China (51372042);The Guangdong Provincial Natural Science Foundation (2015A030308004);The NSFC-Guangdong Joint Fund (U1501246)

摘要/Abstract

摘要：

本文采用固相法在900、1000、1100和1200℃煅烧温度条件下合成了Li_0.33La_0.56TiO₃(LLTO)固态电解质材料, 并将其组装为LLTO固态离子电容器。采用X射线衍射(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、电化学阻抗谱(EIS)和循环伏安法(CV)等技术研究了煅烧温度对LLTO固态电解质和固态离子电容器的显微结构、形貌、离子电导率和储能性能的影响。实验表明, 较高的煅烧温度有利于获得性能优异的LLTO固态离子电容器。在室温下, 1200℃煅烧温度制备的固态离子电容器晶粒离子电导率高达 9.6×10^-4 S/cm, 且具有明显的双电层电容特性, 在4 V电压窗口下比电容为3.52 mF/g。此外, 固态离子电容器比电容随晶粒电导率的增大而增大, 同时受电极与固态电解质接触面积的影响。

关键词: 钛酸镧锂(LLTO), 固态电解质, 离子电导率, 固态离子电容器

Abstract:

Li_0.33La_0.56TiO₃ was synthesized under different calcination temperatures by using solid-state reaction method and assembled as LLTO solid-state ionic capacitors in this study. X-ray powder diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), and cyclic voltammetry (CV) were employed to investigate the influence of calcination temperature on the microstructure, morphology, ionic conductivity, and the energy storage property of the as-prepared products. Results indicate that Li_0.33La_0.56TiO₃ calcined at higher temperature exhibited better performance, and the product synthesized at 1200℃ occupied the highest grain ionic conductivity (9.6×10^-4S/cm) with obvious double-layer capacitor characteristics, while the specific capacitor is nearly 3.52 mF/g at a 4 V potential window. Besides, the specific capacitor of the solid-state capacitor increases with the increment of grain ionic conductivity and effected by the contact area between electrode and solid electrolyte.

Key words: lithium lanthanum titanate (LLTO), solid-state electrolyte, ionic conductivity, solid-state ionic capacitor

中图分类号:

TQ174
TM53

卢东亮, 代广周, 姚英邦, 陶涛, 梁波, 鲁圣国. 煅烧温度对Li_0.33La_0.56TiO₃固态离子电容器性能的影响[J]. 无机材料学报, 2018, 33(10): 1077-1082.

LU Dong-Liang, DAI Guang-Zhou, YAO Ying-Bang, TAO Tao, LIANG Bo, LU Sheng-Guo. Influence of Calcining Temperature on the Property of Li_0.33La_0.56TiO₃Solid-state Ionic Capacitor[J]. Journal of Inorganic Materials, 2018, 33(10): 1077-1082.

图/表 8

图1 不同煅烧温度合成的LLTO固态电解质的XRD图谱

Fig. 1 XRD patterns of LLTO synthesized at different calcination temperatures

图2 由不同煅烧温度制备的LLTO陶瓷样品的SEM照片

Fig. 2 SEM images of LLTO ceramics specimens prepared at different calcining temperatures(a) 900℃; (b) 1000℃; (c) 1100℃; (d) 1200℃

图3 900和1200℃煅烧合成的LLTO粉体主要元素的XPS图谱

Fig. 3 XPS spectra of main elements in the LLTO powders calcined at 900℃ and 1200℃ (a) Titanium; (b) Lanthanum; (c) Lithium

图4 不同煅烧温度制备的LLTO固态离子电容器的交流阻抗谱图, 插图为等效电路图

Fig. 4 Typical EIS of the LLTO solid-state ion capacitors with different calcination temperatures with inset showing equivalent circuit

图5 室温下晶粒电导率和晶界电导率随煅烧温度的变化

Fig. 5 Grain and grain boundary conductivities as a function of calcination temperature at room temperature

图6 固态离子电容器示意图

Fig. 6 Schematic diagram for a solid-state ionic capacitor

图7 不同煅烧温度制备的固态离子电容器在不同电压窗口下的循环伏安曲线

Fig. 7 The cyclic voltammograms for solid-state ion capacitors recorded under different potential windows(a)900℃; (b)1000℃; (c)1100℃; (d)1200℃

表1 不同煅烧温度制备的LLTO固态离子电容器在-2~2 V区间内的比电容

Table 1 Specific capacitance of the LLTO solid-state ionic capacitors with different calcination temperatures under a potential range of -2 V-2 V

Samples	Calcination temperature/℃	Specific capacitance/(mF∙g^-1)
1	900	0.79
2	1000	1.51
3	1100	3.29
3	1200	3.52

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煅烧温度对Li_0.33La_0.56TiO₃固态离子电容器性能的影响

Influence of Calcining Temperature on the Property of Li_0.33La_0.56TiO₃Solid-state Ionic Capacitor

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