Semi-Alicyclic Thermoplastic Polyimide Matrixes Based on Hydrogenated Pyromellitic Dianhydride and Asymmetrical 3,4′-Oxydianiline with Good Thermal Stability and Improved Optical Transparency

Thermoplastic polyimide (PI) matrixes, including PI-a (cc-34ODA) and PI-b (ct-34ODA) were prepared via the hot-pressing procedures of the resins derived from the 3,4′-oxydianiline (34ODA) and two alicyclic dianhydrides of 1S,2R,4S,5R-hydrogenated pyromellitic dianhydride (ccHPMDA) and 1R,2S,4S,5R-hydrogenated pyromellitic dianhydride (ctHPMDA), respectively. The resins exhibited thermoplastic features with good formability at higher temperatures. The afforded semi-alicyclic PI sheets exhibited enhanced properties in comparison to commercially available, wholly aromatic thermoplastic PIs, such as PI-ref1, which are derived from 3,3′,4,4′-oxydiphthalic anhydride (ODPA) and 4,4′-oxydianiline (44ODA), as well as PI-ref2, which is based on pyromellitic dianhydride (PMDA) and 4,4′-bis(3-aminophenoxy)biphenyl (mBAPB). In addition, the developed PI sheets exhibited high heat deflection temperatures (HDT) of 267.4 °C for PI-a and 268.6 °C for PI-b. There values were significantly higher when compared with those of PI-ref1 (Ratem® YS20, HDT: 239.0 °C), PI-ref2 (Aurum® PL450C, HDT: 238.0 °C), PI-ref3 (Ultem® 1000, HDT: 206.0 °C), PI-ref4 (Therplim® TO65, HDT: 180.0 °C), and PI-ref5 based on phthalic anhydride-terminated fluorinated PIs (HDT: 215.0 °C). In terms of mechanical properties, the current PI sheets showed superior flexural properties among the polymers with the flexural strength of 189.0 ± 11.7 MPa (PI-a) and 200.5 ± 4.2 MPa (PI-b), respectively. In addition, the PI sheets exhibited comparable compression properties, inferior impact strength, and tensile properties compared with the referenced PI counterparts. Basically, the PI-b sheet showed better comprehensive properties than those of the stereoisomeric PI-a analog.