四元共聚型聚酰亚胺的合成及应用

Synthesis and Applications of Quaternary Copolymer Polyimide

在聚酰亚胺(PI)中引入旋转能垒较低的醚键或酮键可以增加分子链的柔性,从而有效地提高PI的黏附力。本文将含柔性醚键的4,4′-二氨基二苯醚(ODA)、含柔性酮键的3,3′,4,4′-二苯甲酮四甲酸二酐(BTDA)、具有非共面扭曲结构的联苯四甲酸二酐(BPDA)和1,4-二氨基苯(PPDA)原位缩聚,通过两步法制备了一种四元共聚型PI膜。结果表明,该共聚型PI膜的玻璃化转变温度为237.1℃,10%热分解温度为538.1℃,拉伸强度为139.64 MPa,断裂伸长率为22.29%,弹性模量为3.12 GPa,将0.5%(相对于单体总质量的百分比)的滑石粉填料在单体聚合之前加入N,N-二甲基乙酰胺(DMAc)溶液内,酰亚胺化后制备的PI膜对铜箔的剥离强度由0.62 N/mm提高到了0.94 N/mm。

The introduction of ether or ketone bonds with lower rotational barrier into polyimide(PI)could increase the flexibility of the molecular chain and effectively improve the stick force of PI.In this paper,with a two-step method,one kind of tetrameric copolymerized PI film was prepared by the in-situ polycondensation of 4,4′-diaminodiphenyl ether(ODA)containing flexible ether bonds,3,3′,4,4′-benzophenone tetracarboxylic acid dianhydride(BTDA)containing flexible ketone bonds,biphenyl tetracarboxylic acid dianhydride(BPDA)with a non-coplanar twisted structure,and 1,4-diaminobenzene(PPDA).The results show that the copolymerized PI film has a glass transition temperature of 237.1℃,a 10%thermal decomposition temperature of 538.1℃,a tensile strength of 139.64 MPa,an elongation at break of 22.29%,and a modulus of elasticity of 3.12 GPa.The peel strength of the PI film after imidization for the copper foil is increased from 0.62 N/mm to 0.94 N/mm,which was prepared by adding the talc filler with a mass fraction of 0.5%to N,N-dimethylacetamide(DMAc)solution prior to the monomer polymerization.