Synthesis and Properties of Semicrystalline Copolyimides Based on 4,4′-Diaminodiphenylether and 1,3-Bis(4-aminophenoxy) Benzene

Copolyimides were prepared from 4,4′-diaminodiphenylether (4,4′-ODA), 1,3-bis(4-aminophenoxy) benzene (TPER), and pyromellitic dianhydride (PMDA) through a three-step imidization process with different monomer compositions. The copolymerization disrupted the molecular regularity and decreased the intermolecular interaction of the polyimide chains. The X-ray diffraction (XRD) results indicated the prepared copolyimides showed the same semicrystalline character, but had various crystallinity and crystal forms. The copolymerization also changed the crystal morphologies of the polyimides. With increasing TPER ratio, the copolyimides started to form spherulites and hedrites, which then tended to grow more perfectly as the TPER ratio was further increased. The solubility of the copolyimides and their dependence on the crystallnity and the chain flexibility was investigated. These copolyimides exhibited excellent thermal and thermo-oxidative stability.