用于高介电复合材料的全包裹Ag@TiO2填充颗粒的制备

doi:10.15541/jim20180370

摘要/Abstract

摘要：

高介电复合材料是近年来受到广泛关注的一种材料, 可用于嵌入式电容器及储能器件。本研究使用钛醇盐水解法在室温下制备全包裹Ag@TiO₂颗粒, 对该颗粒填充的复合材料进行漏电流、介电和储能性能表征, 并对其介电机理进行探讨。扫描电子显微镜和能谱结果显示Ag@TiO₂颗粒具有球形的全包裹核壳结构, 壳层厚度大约为400 nm。X射线衍射结果验证了Ag@TiO₂颗粒具有完整的物相。Ag@TiO₂填充的聚二甲基硅氧烷复合材料表现出小的漏电流(10 ^-8A/cm ²)、较大的介电系数(108)、低的介电损耗(0.2%)和较大的储能密度(8.58×10 ^-3J/cm ³)。有效场和Maxwell相结合的理论模型与实验数据对比验证, 推测界面极化作用提高了复合材料的等效介电系数。该颗粒填充的复合材料在嵌入式电容器方面具有潜在的应用价值。

关键词: Ag@TiO₂, 高介复合材料, 界面极化, 介电性能

Abstract:

High-k composites have been actively pursued in the past few years for potential applications in embedded capacitors and energy-storage devices. In this study, Ag@TiO₂ core@shell particles were synthesized by a hydrolysis from titanate alkoxides at room temperature. Composites filled with the particle fillers were characterized for I/V, dielectric and energy-storage characteristics. Mechanisms of influences of Ag@TiO₂ fillers on dielectric properties of composites were investigated. Scanning electron microscopy and energy dispersive spectra exhibit that the synthesized Ag@TiO₂ particles have spherical and fully-coated core@shell structures. X-ray diffraction pattern confirms the phase of Ag and TiO₂ in the particles. The polydimethylsiloxane composites filled with Ag@TiO₂ fillers exhibit a small leakage current of 10 ^-8A/cm ², a high dielectric permittivity of 108, and a very low dielectric loss of 0.2%, and a large energy storage density of 8.58×10 ^-3J/cm ³. Theoretical model containing effective medium theory (EMT) and Maxwell theory were used to compare with experimental results, and interfacial polarizations were proposed to enhance the permittivities of the composites. The composites filled with Ag@TiO₂ fillers show potential applications in the embedded capacitors.

Key words: Ag@TiO₂, high-k composite, interfacial polarization, dielectric properties

中图分类号:

TB333

简刚, 刘美瑞, 张晨, 邵辉. 用于高介电复合材料的全包裹Ag@TiO₂填充颗粒的制备[J]. 无机材料学报, 2019, 34(6): 641-645.

Gang JIAN, Mei-Rui LIU, Chen ZHANG, Hui SHAO. Preparation of Fully-coated Ag@TiO₂ Particle Fillers for High-k Composites[J]. Journal of Inorganic Materials, 2019, 34(6): 641-645.

图/表 8

图1 Ag@TiO2颗粒的SEM照片

Fig. 1 SEM images of Ag@TiO2 particles

图2 Ag@TiO2颗粒(550 ℃/2 h)的SEM照片(a)及其EDX面扫描图像(b~d)

Fig. 2 (a) SEM and (b-d) corresponding EDX mapping images of Ag@TiO2 core@shell particles (550 ℃/2 h)

图3 核壳Ag@TiO2颗粒(550 ℃/2 h)的XRD图谱

Fig. 3 XRD pattern of core@shell Ag@TiO2 particles (550 ℃/2 h)

图4 Ag@PVP/TiO2颗粒在氧气和氮气条件下的热失重曲线

Fig. 4 TGA curves of Ag@PVP/TiO2 particles in O2 and N2

图5 填充Ag和Ag@TiO2的复合材料的对比I/V曲线

Fig. 5 I/V curves of composites filled with Ag and Ag@TiO2 fillers

图6 不同颗粒填充复合材料介电常数和介电损耗的频率依赖性

Fig. 6 Frequency dependent dielectric permittivity and dielectric loss of composites filled with various particles

图7 复合材料介电参数(介电系数和损耗)与Ag@TiO2填充颗粒体积分数的关系(理论与实验对比)

Fig. 7 Experimental and theoretical relations between dielectric properties (permittivity and loss) of composites and volume fraction of Ag@TiO2 fillers

图8 不同颗粒填充的复合材料的(a)击穿强度和(b)储能密度的对比

Fig. 8 Comparison of (a) breakdown strength and (b) energy density of composites with different fillers

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用于高介电复合材料的全包裹Ag@TiO₂填充颗粒的制备

Preparation of Fully-coated Ag@TiO₂ Particle Fillers for High-k Composites

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