超低损耗热固性聚合物复合材料及其介电性能稳定性研究

超低介电损耗的热固性芯片封装载板和印刷电路板基板材料，是高算力芯片、5G通信、汽车雷达等新型高频高速系统中的基础材料。近年来，尽管不断有新型低损耗材料问世，但在投入实际应用前这些材料还需要经过广泛的验证，包括可靠性的验证和工业化工艺条件的适配等。随着系统工作频率的提升和工况的复杂化，对基板材料介电常数（D_k）与介电损耗因子（D_f）的要求也越来越严苛，在受热情况下基板材料介电性能的劣化问题已成为影响基板材料和高频高速系统可靠性的新因素。然而，当前对其背后的化学反应机理和介电性能变化规律的研究还不够深入，未形成标准的测试方法，也缺乏相应的解决方案。

材料老化过程中结构的变化与微波介电性能之间的联系是探究介电性能劣化机理的基础。本文以当前广泛应用的超低损耗热固性聚苯醚/碳氢树脂体系为研究对象进行了加速老化实验，确认了材料的介电性能劣化源于材料的热氧老化。通过研究材料热氧老化过程中交联结构与化学结构的变化，发现在材料老化初期，氧化反应主要发生在固化反应不完全的碳氢树脂链段，而且材料的D_f与材料老化产物的积累量之间接近线性的关系。此外，我们还分析了样品尺寸、吸湿等因素对介电性能劣化的影响。

基于上述老化机理，我们进一步研究了材料的固化反应动力学。结果表明聚苯醚/碳氢低损耗树脂体系的交联固化过程为减速反应，与常规的环氧树脂等材料不同。固化反应的转化率受到引发剂含量的影响，并呈现出出多步骤的特点，活化能随反应物迁移能力的下降、不同活性官能团的聚合反应的切换、以及玻璃化对反应物扩散的限制而逐步增大。由于在环氧体系中常用的等转化率分析方法并不完全适用于本文体系，我们设计了一种可有效拟合反应速率曲线的半经验性的方案。通过分析不同引发剂含量样品的性能，我们提出固化过程中引发剂的分解副产物影响了材料的Df ，并初步探讨了兼顾材料固化程度和超低D_f的方案。

在介电性能劣化问题的解决方案方面，我们首先尝试了受阻酚类主抗氧剂、芳香胺类主抗氧剂、辅助抗氧剂、金属螯合剂在自由基交联的超低损耗树脂体系中的应用，发现所有的抗氧剂都提高了材料的初始D_k，大部分同时提高了材料的初始D_f。然而，由于抗氧剂与材料固化反应的拮抗作用，包括两种反应性抗氧剂在内的大部分抗氧剂并未提高材料的抗热氧老化能力。仅有两种金属螯合剂通过减少树脂内铜离子的催化作用而提供了氧化诱导期，从而提高了材料长期抗老化能力。

除了抗氧剂外，为了同时达成材料的低损耗和高抗老化能力，我们还探究了多乙烯基含硅交联剂在自由基交联的热固性聚苯醚体系中的应用。实验结果表明，这类交联剂与聚苯醚有良好的相容性以及合适的反应温度。相比使用已广泛商用的交联剂，使用含硅交联剂固化产物可以达到更低的D_f，代号为PPO-SiX1的样品在10 GHz下的D_f达到了0.00159。还展现出更强的抗热氧老化能力，碳氢树脂交联的样品在150℃下老化7天后D_f增大了0.0043，而三种含硅交联剂交联样品的增长均少于0.0015。

为建立介电性能劣化问题的评价方法，我们采用商业级的低损耗基板材料以及实验室内制备的基板材料进行了多温度的长期老化实验。结果表明碳氢树脂类样品老化速度最快、介电性能劣化最为显著；环氧树脂类和马来酰亚胺类样品虽然老化迅速，但介电性能变化较小；而聚苯醚类样品尤其是含硅的聚苯醚样品的介电性能劣化速度最慢。结合质量、交联结构和化学结构的变化，我们讨论了各类样品在不同温度下介电性能的不同变化规律，通过Arrhenius方法计算了材料在70℃工况下的预期寿命，并指出材料在不同温度下的反应机理差异可能导致了寿命预测时的误差。

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