原位聚合法制备SiC@SiO2/BN/PI复合材料及其表征

doi:10.15541/jim20200360

摘要/Abstract

摘要：

聚酰亚胺复合材料以其优异的性能以及在航空航天、轨道交通、微电子等领域广泛的应用前景引起越来越多的关注。在750 ℃条件下对SiC晶须进行表面氧化处理, 形成SiC@SiO₂包覆结构晶须, 与BN颗粒构成复合填料, 分别采用硅烷偶联剂和钛酸酯偶联剂进行表面改性, 用原位聚合法制备了SiC@SiO₂/BN/PI(PI:聚酰亚胺)复合材料。采用傅里叶变换红外光谱仪(FT-IR)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和X射线衍射仪(XRD)等进行结构和性能表征。结果表明: 晶须与颗粒质量比为4 : 1时, 复合填料在PI基体内形成了有效的导热网络, 且当填料含量为45wt%时, SiC@SiO₂/BN/PI复合材料导热系数达到0.95 W/(m·K)。SiC@SiO₂/BN/PI复合材料的力学性能随着复合填料的种类和数量的变化呈现规律性变化。SiO₂氧化层阻断复合填料间自由电子的移动, SiC@SiO₂/BN/PI复合材料的电气绝缘性能下降幅度减小。

关键词: 聚酰亚胺, 复合填料, 导热性能, 电气绝缘性能

Abstract:

Polyimide composites have attracted more and more attention due to their excellent properties and wide application prospects in aerospace, rail transit, microelectronics and other fields. SiC@SiO₂ whisker was prepared by oxidation of SiC whisker at 750 ℃, which formed mixed fillers with BN particles. The SiC@SiO₂ whisker and BN were modified by a silane coupling agent and a titanate coupling agent, respectively. SiC@SiO₂/BN/PI composites were prepared by in-situ polymerization. The structure and property of the fillers and composites were characterized. Whiskers and particles formed an effective pathway in the polyimide matrix, which promoted continuous improvement of the thermal conductivity of SiC@SiO₂/BN/PI composites. When the total filler content was 45wt% and the mass ratio of whiskers to particles was 4 : 1, the thermal conductivity was increased to 0.95 W/(m·K). Mechanical properties of SiC@SiO₂/BN/PI composites changed regularly with the type and amount of mixed fillers. The SiO₂ layer blocks the communication of free electrons between the mixed fillers, and the decreasing range of electrical insulation performance of the SiC@SiO₂/BN/PI composites declined.

Key words: polyimide, mixed filler, thermal conductivity, electric insulation property

中图分类号:

TQ170
TB34

高纪明, 杨阳, 雷霆, 王进, 刘杰, 张丽敏. 原位聚合法制备SiC@SiO₂/BN/PI复合材料及其表征[J]. 无机材料学报, 2021, 36(1): 36-42.

GAO Jiming, YANG Yang, LEI Ting, WANG Jin, LIU Jie, ZHANG Limin. Synthesis and Characterization of SiC@SiO₂/BN/PI Composites by in-situ Polymerization[J]. Journal of Inorganic Materials, 2021, 36(1): 36-42.

图/表 8

图1 不同温度和时间氧化处理SiC晶须的XRD图谱

Fig. 1 XRD patterns of the SiC whiskers oxidized at different temperatures for different time

图2 SiC晶须的TEM照片

Fig. 2 TEM images of SiC whiskers oxidized at 750 ℃ for (a) 30, (b) 60 and (c) 90 min, and (d) 800 ℃ for 60 min

图3 表面改性的BN(a)和SiC@SiO2(b)的FT-IR光谱图

Fig. 3 FT-IR spectra of (a) BN and modified-BN; (b) SiC@SiO2 and modified-SiC@SiO2

图4 SiC@SiO2/BN/PI复合材料断口的SEM照片

Fig. 4 SEM images of fracture surfaces of SiC@SiO2/BN/PI composites with 20wt% mixed fillers m(BN):m(SiC@SiO2) (a) 5 : 0; (b) 4 : 1; (c) 3 : 2; (d) 2 : 3; (e) 1 : 4; (f) 0 : 5

图5 添加不同比例填料SiC@SiO2/BN/PI复合材料的导热系数

Fig. 5 Thermal conductivity of composites with different weight ratio of BN flakes to SiC@SiO2 whiskers at filler content of 20wt%

图6 添加不同含量填料的PI复合材料的导热系数

Fig. 6 Thermal conductivity of composites with different filler contents when the weight ratio of BN to SiC@SiO2 is 1 : 4.

图7 SiC@SiO2/BN/PI复合材料的力学性能

Fig. 7 Mechanical properties of SiC@SiO2/BN/PI composites (a) Different weight ratios of BN to SiC@SiO2 at filler content of 20wt%; (b) Different filler contents when the weight ratio of BN to SiC@SiO2 is 1 : 4.

图8 SiC@SiO2/BN/PI复合材料的表面电阻率和体积电阻率

Fig. 8 Surface resistivities and volume resistivities of the SiC@SiO2/BN/PI composites (a) Different weight ratios of BN to SiC@SiO2 at filler content of 20wt %; (b) Different filler contents when the weight ratio of BN to SiC@SiO2 is 1 : 4.

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原位聚合法制备SiC@SiO₂/BN/PI复合材料及其表征

Synthesis and Characterization of SiC@SiO₂/BN/PI Composites by in-situ Polymerization

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