取向碳化硅晶须硅橡胶复合材料导热性及绝缘性

于天骄; 宋伟; 冯景涛; 彭修峰; 宋文宏

doi:10.13801/j.cnki.fhclxb.20230404.002

取向碳化硅晶须硅橡胶复合材料导热性及绝缘性

doi: 10.13801/j.cnki.fhclxb.20230404.002

1.
哈尔滨理工大学　电气与电子工程学院，工程电介质及其应用教育部重点实验室，哈尔滨 150086
2.
上海拜高高分子材料有限公司，上海 201400

基金项目: 国家自然科学基金(51541702；51607048)

详细信息

通讯作者:
宋伟，博士，教授，博士生导师，研究方向为导热复合材料研发及绝缘材料改性研究　E-mail: sw7912@hrbust.edu.cn

中图分类号: TM211；TB333
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- 被引次数: 0
出版历程
- 收稿日期: 2023-02-27
- 修回日期: 2023-03-20
- 录用日期: 2023-03-27
- 网络出版日期: 2023-04-06
- 刊出日期: 2024-01-01

Research on thermal conductivity and insulation of oriented silicon carbide whisker silicone rubber composites

1.
Key Laboratory of Engineering Dielectric and Its Application, Ministry of Education, School of Electrical and Electronic Engineering, Harbin University of Science and Technology, Harbin 150086, China
2.
Shanghai Baigao Polymer Material CO., LTD., Shanghai 201400, China

Funds: National Natural Science Foundation of China (51541702; 51607048)

摘要

摘要: 随着电子产品的集成密度和功率密度不断增加，优化热界面材料变的尤为重要。本文以一维碳化硅晶须(SiC_w)为填料，硅橡胶为基体制备出导热硅橡胶复合材料，综合分析了复合材料的微观形貌、物相结构、导热性及绝缘性。首先通过共沉淀法制备出Fe₃O₄对SiC_w包覆的改性材料，其次将包覆Fe₃O₄的SiC_w在液体硅橡胶基体中分散均匀，最后将其置于恒稳磁场中完成晶须取向及基体固化。结果表明：SiC_w晶须表面包覆一层Fe₃O₄纳米颗粒且在硅橡胶基体中呈现取向排列，制备出SiC_w取向结构的硅橡胶复合材料。当取向SiC_w含量达到10wt%时，相比于纯硅橡胶导热系数可提升72%，比未取向10wt%SiC_w填充的高40%。相比于纯硅橡胶体积电阻率下降两个数量级，但仍然具有良好的绝缘性。通过COMSOL对SiC_w随机分散与取向排列的硅橡胶复合材料进行模拟仿真，仿真结果表明，含量10wt%的SiC_w可使硅橡胶导热系数提升60%，体积电阻率在10¹⁵ Ω∙cm以上，而10wt%取向SiC_w可使硅橡胶导热系数提升170%，体积电阻率在10¹⁴ Ω∙cm以上，与实验结果的趋势相一致。
- 硅橡胶 /
- 碳化硅晶须 /
- 取向 /
- 导热性 /
- 绝缘性
Abstract: With the increasing integration density and power density of electronic products. It is particularly important to optimize the research of thermal interface materials. In this paper, one-dimensional silicon carbide whisker (SiC_w) was used as filler and silicone rubber was used as matrix to prepare thermal conductive silicone rubber composites. The microstructure, phase structure, thermal conductivity and insulation of the composites were comprehensively analyzed. Firstly, the modified material of SiC_w coated by Fe₃O₄ was prepared by coprecipitation method. Secondly, SiC_w coated with Fe₃O₄ was evenly dispersed in the liquid silicone rubber matrix. Finally, it is placed in a constant magnetic field to complete whisker orientation and matrix curing. The results show that the surface of SiC_w whiskers is coated with Fe₃O₄ nanoparticles, and they are oriented in the silicone rubber matrix. Silicone rubber composites with SiC_w oriented structure were prepared. When the oriented SiC_w reaches 10wt%, the thermal conductivity can be increased by 72% compared with pure silicone rubber, and it is 40% higher than that filled with non-oriented 10wt%SiC_w. Compared with pure silicone rubber, the volume resistivity decreases by two orders of magnitude. But it still has good insulation. The silicone rubber composites with randomly dispersed and oriented SiC_w were simulated by COMSOL. The simulation results show that the thermal conductivity of silicone rubber can be improved by 60% with 10wt%SiC_w. The volume resistivity is above 10¹⁵ Ω∙cm. However, 10wt% oriented SiC_w can improve the thermal conductivity of silicone rubber by 170% and the volume resistivity is above 10¹⁴ Ω∙cm. It is consistent with the trend of experimental results.
- silicone rubber /
- silicon carbide whisker /
- orientation /
- thermal conductivity /
- insulation

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图 1 Fe₃O₄包覆碳化硅晶须(SiC_w)的制备流程

Figure 1. Preparation process of Fe₃O₄ coated SiC whisker (SiC_w)

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图 2 硅橡胶复合材料制备流程

Figure 2. Preparation process of silicone rubber composites

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图 3 XRD测试示意图

Figure 3. Schematic diagram of XRD test

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图 4 SiC_w及FE@SIC的SEM图像

Figure 4. SEM images of SiC_w and FE@SIC

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图 5 硅橡胶(SR)试样断面SEM图像

Figure 5. SEM images of silicone rubber (SR) section

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图 6 Fe₃O₄及FE@SIC的XRD图谱

Figure 6. XRD patterns of Fe₃O₄ and FE@SIC

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图 7 SR、SIC10、SICFE10*、FE@SIC10、FE@SIC10*的XRD图谱

Figure 7. XRD patterns of SR, SIC10, SICFE10*, FE@SIC10, FE@SIC10*

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图 8 SiC_w/SR导热系数对数值线性拟合图

Figure 8. Linear fitting diagram of SiC_w/SR thermal conductivity versus numerical value

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图 9 导热模型与SiC_w/SR的导热系数折线图

Figure 9. Thermal conductivity model and thermal conductivity line chart of SiC_w/SR

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图 10 SIC10、FE@SIC10*截面模拟图

Figure 10. Simulation diagram of SIC10, FE@SIC10* section

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图 11 FE@SIC10*与SIC10的几何仿真模型

Figure 11. Geometric simulation model diagram of FE@SIC10* and SIC10

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图 12 FE@SIC10*和SIC10几何模型在热场下的温度分布

Figure 12. Temperature distribution of geometric model of FE@SIC10* and SIC10 under thermal field

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表 1 仿真与实验数据对比表

Table 1. The comparison table of simulation results and experimental data

	Experimental data		Simulation results
Name of sample	SIC10	SIC10@FE10*	SIC10	SIC10@FE10*
Thermal conductivity/(W/(m·K))	0.167	0.235	0.221	0.374
Volume resistivity/Ω·cm	3.71×10¹⁵	8.11×10¹⁴	4×10¹⁵	1×10¹⁴

下载: 导出CSV

表 1 试样编号明细表

Table 1. Specimen details

Name of sample	Detailed description
FE@SIC	Fe₃O₄ coated SiC_w
SR	Pure silicone rubber sample
SiC_w/SR	SiC_w filled silicone rubber series samples
SIC10	10wt% SiC_w filled silicone rubber sample
FE@SIC10*	Magnetized sample of 10wt%FE@SIC silicone rubber
FE@SIC10	10wt%FE@SIC silicone rubber sample
SICFE10*	Magnetized sample of 10wt%SiC_w+Fe₃O₄ silicone rubber

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表 2 SiC_w/SR的导热系数

Table 2. Thermal conductivity of SiC_w/SR

SiC_w/SR/wt%	Thermal conductivity/(W·(m·K)⁻¹)
0	0.137
5	0.148
10	0.167
15	0.181
20	0.236

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表 3 FE@SIC10*导热系数对比表

Table 3. Comparison table of thermal conductivity of FE@SIC10*

Name of sample	Thermal conductivity/(W·(m·K)⁻¹)
SR	0.137
SIC10	0.167
SICFE10*	0.172
FE@SIC10	0.168
FE@SIC10*	0.235

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表 4 SiC_w/SR体积电阻率

Table 4. Volume resistivity of SiC_w/SR

SiC_w/SR/wt%	Volume resistivity/(Ω·cm)
0	4.00×10¹⁶
5	7.84×10¹⁵
10	3.70×10¹⁵
15	5.60×10¹⁴
20	3.90×10¹⁴

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表 5 FE@SIC10*体积电阻率对比

Table 5. Comparison of volume resistivity of FE@SIC10*

Name of sample	Volume resistivity/(Ω·cm)
SR	4.0×10¹⁶
SIC10	3.7×10¹⁵
FE@SIC10*	8.1×10¹⁴

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表 6 试样性能的仿真与实验数据对比

Table 6. Comparison of simulation results and experimental data of sample properties

Sample	Thermal conductivity/(W·(m·K)⁻¹)		Volume resistivity/(Ω·cm)
Sample	Experimental data	Simulation results	Experimental data	Simulation results
SIC10	0.167	0.221	3.70×10¹⁵	4.00×10¹⁵
SIC10@ FE10*	0.235	0.374	8.11×10¹⁴	1.00×10¹⁴

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