Abstract

High‐performance copolyimide (co‐PI) fibers were prepared via the wet spinning process of co‐polyamide acid precursors based on 3,3′,4,4′‐biphenyldianhydride (BPDA) and a mixture of three diamines namely p‐phenylene diamine (p‐PDA), 2‐(4‐aminophenyl)‐5‐aminobenzimidazole (BIA), and 4,4′‐oxidianiline (ODA), followed by drawing and imidization at high temperatures. Effects of the ODA and BIA contents on the molecular packing, morphology, hydrogen‐bonding interactions, mechanical and thermal properties of the prepared fibers were investigated. The mechanical properties of the co‐PI fibers were improved with the addition of ODA and BIA, and they reached the optimum tensile strength of 2.7 GPa and modulus of 94.3 GPa. Wide‐angle X‐ray diffraction results (WAXD) showed that the co‐PI fibers exhibited highly oriented structure along the fiber direction with low degree of lateral packing orders in the transverse direction. Two‐dimensional small‐angle X‐ray scattering (2D‐SAXS) revealed that the incorporation of ODA resulted in the reduction in radius, length, misorientation, and internal surface roughness of the microvoids in the fibers. Fourier transform infrared (FTIR) results indicated that hydrogen‐bonding formed between the BIA and cyclic imide units effectively strengthened the intermolecular interactions. The co‐PI fibers exhibited excellent thermal and thermal‐oxidative stability, with a 5%‐weight‐loss temperature of 578°C under N2 and 572°C in air. POLYM. ENG. SCI., 55:2615–2625, 2015. © 2015 Society of Plastics Engineers

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