Thermal conductivity and electrical properties of three-dimensional porous aluminum nitride/epoxy composites
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摘要: 环氧树脂(EP)是一种典型的电子封装绝缘材料，但其导热系数(小于0.2 W/(m·K))较低，提高其导热性是解决电子器件散热问题的有效办法。本文通过构筑三维多孔的氮化铝骨架(3D-AlN)，制备得到3D-AlN/EP复合材料。SEM形貌和XRD物相表征结果证实3D-AlN骨架及3D-AlN/EP复合材料的成功制备。利用TGA精确测量3D-AlN骨架所占复合材料的质量分数，通过与含有不同含量随机分布的AlN/EP (Random AlN/EP)复合材料对比发现，3D-AlN/EP复合材料的导热系数要高于Random AlN/EP复合材料，45.48wt%3D-AlN/EP复合材料的室温(25℃)导热系数为1.00 W/(m·K)，是纯EP(0.18 W/(m·K))的5.6倍。利用理论模型(Fogyel、Agari)计算复合材料的界面热阻，发现3D-AlN/EP复合材料相比于Random AlN/EP具有更低的填料与填料间界面热阻，分别为2.704×105 K·W−1、4.019×105 K·W−1。电性能测试结果表明，45.48wt%3D-AlN/EP复合材料具良好的介电性能及绝缘性能(体积电阻率为4.16×1011 Ω·cm)。本研究从封装绝缘材料改性角度为电子器件散热问题提供了一种有效解决方案。Abstract: Epoxy resin (EP) is a typical insulating material for electronic packaging, but its thermal conductivity (less than 0.2 W/(m·K)) is low, and improving its thermal conductivity is an effective way to solve the heat dissipation problem of electronic devices. In this paper, 3D-AlN/EP composites were prepared by constructing a three-dimensional porous aluminum nitride skeleton (3D-AlN). The SEM morphology and XRD phase characterization results confirmed the successful preparation of 3D-AlN skeleton and 3D-AlN/EP composites. The mass fraction of the composite accounted for by the 3D-AlN skeleton was precisely measured using TGA, and by comparing with different contents of random distribution AlN/EP (Random AlN/EP) composites, it was found that the thermal conductivity of 3D-AlN/EP composites was higher than that of Random AlN/EP composites, the thermal conductivity of the 45.48wt%3D-AlN/EP composite at room temperature (25℃) was 1.00 W/(m·K), which was 5.6 times higher than that of pure EP (0.18 W/(m·K)). The interfacial thermal resistance of the composites was calculated using the theoretical model (Fogyel, Agari), and it was found that the 3D-AlN/EP composites had lower filler-to-filler interfacial thermal resistance compared to Random AlN/EP, with 2.704×105 K·W−1 and 4.019×105 K·W−1, respectively. The electrical properties showed that the 45.48wt%3D-AlN/EP composite had good dielectric and insulating properties (volume resistivity is 4.16×1011 Ω·cm). This study provides an effective solution to the heat dissipation problem of electronic devices from the perspective of package insulation material modification.
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图 1 三维多孔的氮化铝骨架(3D-AlN)骨架及3D-AlN/环氧树脂(EP)的制备示意图
Figure 1. Schematic diagram of the preparation of three-dimensional porous aluminum nitride skeleton (3D-AlN) framework and 3D-AlN/epoxy resin (EP) composites
APG—Alkyl polyglucoside
图 2 (a) 3D-AlN骨架的SEM图像；(b) 图2(a)的局部放大SEM图像；(c) 3D-AlN/EP复合材料的SEM图像；((d), (e)) 对于图2(c)的能谱及元素分布
Figure 2. (a) SEM image of 3D-AlN framework; (b) Partially enlarged SEM image according to Fig. 2(a); (c) SEM image of 3D-AlN/EP composite; ((d), (e)) Energy spectrum and element distribution according to Fig. 2(c), respectively
图 3 (a) 3D-AlN/EP复合材料的TGA曲线；(b) AlN和3D-AlN/EP复合材料的XRD图谱
Figure 3. (a) TGA curves of 3D-AlN/EP composites; (b) XRD patterns of AlN and 3D-AlN/EP composites
图 4 (a) 不同3D-AlN含量的随机分布AlN/EP及3D-AlN/EP复合材料的导热系数及Foygel非线性拟合；(b) Agari模型线性拟合；(c) 不同3D-AlN含量3D-AlN/EP复合材料导热系数随温度变化的曲线；(d) 不同3D-AlN含量3D-AlN/EP复合材料的DSC图谱
Figure 4. (a) Thermal conductivity and Foygel nonlinear fit of randomly distributed AlN/EP and 3D-AlN/EP composites with different contents of 3D-AlN; (b) Linear fit of Agari model; (c) Thermal conductivity curves of 3D-AlN/EP composites with different contents of 3D-AlN as a function of temperature; (d) DSC spectra of 3D-AlN/EP composites with different contents of 3D-AlN
Cf—Ability of the filler to form continuity; Cm—Effect of the filler on the structure of the matrix; λ—Thermal conductivity of composites
图 5 (a) 不同3D-AlN含量3D-AlN/EP复合材料的红外热成像照片；((b), (c)) 随机分布AlN/EP和3D-AlN/EP复合材料的固体传热仿真结果
Figure 5. (a) Infrared thermal images of 3D-AlN/EP composites with different contents of 3D-AlN; ((b), (c)) Solid heat transfer simulation results of random AlN/EP and 3D-AlN/EP composites
图 6 不同3D-AlN含量3D-AlN/EP复合材料的介电常数 (a) 和介电损耗随频率变化图谱 (b)
Figure 6. Permittivity (a) and loss tangent (b) of 3D-AlN/EP composites with different contents of 3D-AlN as a function of frequency
图 7 不同3D-AlN含量3D-AlN/EP复合材料的体积电阻率
Figure 7. Volume resistivity of 3D-AlN/EP composites with different contents of 3D-AlN
表 1 随机分布的AlN/EP和3D-AlN/EP复合材料的参数计算结果
Table 1. Calculation results of parameters for Random AlN/EP and 3D-AlN/EP composites
Composites K0 Vc/vol% β Rc/(105 K·W−1) Random AlN/EP 3.412 0.0994 0.83392 4.019 3D-AlN/EP 3.615 0.0597 0.56296 2.704 Notes: K0—Pre-exponential factor; Vc—Critical volume fraction of filler; β—Conductivity exponent that depends on the aspect of filler; Rc—Interface thermal resistance. 
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