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电子器件向着大功率、小型化方向发展对环氧树脂电子封装材料的高温电学性能提出了更高的要求. 本研究采用环氧基封端苯基三硅氧烷（ETS）作为功能单体，通过交联反应将Si-O键引入到双酚A环氧树脂中，系统地研究了ETS对环氧树脂复合材料的结构以及高温电学特性的影响及调控作用. 实验结果表明：随着ETS含量的增加，环氧树脂复合材料的交联度逐渐降低. 当ETS添加质量分数为2.5 %时，复合材料的玻璃化转变温度及热稳定性得到了提升，且呈现最优综合电学性能，在70℃下，该复合材料电导率大幅下降，空间电荷积聚程度得到明显改善，陷阱深度加深，介电损耗降低，击穿强度提升至74.2 kV/mm. 随着ETS含量的逐步增加，环氧复合材料的电学性能呈现先增强后减弱的非线性变化规律，这种浓度依赖性行为与纳米填料改性体系具有相似的特性演变特征.本文提出通过对硅氧烷交联后与环氧构成的微观交联网络拓扑结构演变来解释ETS对环氧树脂高温电学性能的影响. 本研究为开发硅氧烷改性高性能环氧树脂电子封装材料提供了重要的理论依据以及设计策略.The ongoing trend toward high-power and miniaturized electronic devices has imposed increasingly stringent requirements on the high-temperature electrical properties of epoxy encapsulating materials. In this study, epoxy-terminated phenyltrisiloxane (ETS) was employed as a functional monomer to incorporate Si-O bonds into bisphenol-A epoxy resin through crosslinking reactions, systematically investigating the influence and modulation effects of ETS on the structure and high-temperature electrical characteristics of epoxy composites. Gel content measurements indicate that as the concentration of ETS increases, the gel content of the epoxy resin composites decreases accordingly, suggesting that higher ETS content reduces the crosslinking density of the epoxy network. Experimental test results demonstrate that compared to pure epoxy resin, the composite with 2.5 wt% ETS exhibits superior performance: the glass transition temperature increases to 129℃ with enhanced thermal decomposition temperature, while showing optimal high-temperature (70℃) electrical properties - including significantly reduced conductivity, markedly suppressed space charge accumulation, deepened trap energy level (from 0.834 eV to 0.847 eV), decreased dielectric loss (0.005 at 50 Hz), and improved breakdown strength (74.2 kV/mm). Notably, the electrical properties of epoxy composites follow a non-monotonic concentration dependence with increasing ETS content, initially enhancing then deteriorating, exhibiting similar evolutionary characteristics to nanoparticle-modified systems. We propose a competitive mechanism between the epoxy network structure and intrinsic properties of ETS to explain this phenomenon: At low concentrations, the original C-C network dominates, where the intrinsic properties of ETS are constrained by the host matrix, leading to improved thermal stability. Simultaneously, the bandgap difference between ETS and DGEBA establishes charge barriers that enhance insulation performance. However, at higher concentrations, the reduced crosslinking density and increased free volume caused by reactivity and structural mismatch between ETS and DGEBA ultimately lead to performance degradation. This study provides crucial theoretical insights and design strategies for developing high-performance siloxane-modified epoxy encapsulants.
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Keywords:
- Epoxy resin /
- Siloxane /
- Crosslinked network /
- High-temperature insulation
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