HIGH-MODULUS POLYIMIDE POLYIMIDE MOLECULAR COMPOSITE FILMS THAT UTILIZE ACETYLENE UNIT AS A CROSS-LINK SITE

Polyimide/polyimide molecular composite (MC) films comprised of a rigi d polyimide derived from biphenyltetracarboxylic dianhydride (BPDA) an d p-phenylenediamine (PDA) and a flexible polyimide derived from BPDA and bis (3,3'-diaminodiphenyl) acetylene (intA) and/or oxydianiline (O DA) were prepared by blending the polyamic acid solutions in 7 : 3 wei ght ratio, and then imidizing the blend films. Acetylene content in th e flexible polyimide backbone was controlled by the ratio of intA and ODA. Cold-drawing of the blend polyamic acid films, followed by imidiz ation, gives high modulus polyimide/polyimide MC films. The modulus of the MC films increased almost linearly with the draw ratio, reaching 25.5 GPa for the 40% drawn film. Acetylene groups in the flexible poly imide can be thermally cured to crosslink. The onset of exotherm appea red at 340-degrees-C on DSC, reaching maximum at 398-degrees-C. After the thermal crosslinking, the MC films maintained the high modulus, th ough elongation became small. Taking advantage of the crosslinkable ac etylene units, two MC films were laminated and processed at 400-degree s-C for 20 min under 100 kg/cm2 to give a good-quality laminate film. The interface of the two films was strongly bonded through the crossli nking of acetylene groups. Laminate films maintained the high modulus afforded by the cold-drawing. (C) 1994 John Wiley & Sons, Inc.