Effects of pre-imidization on rheological behaviors of polyamic acid solution and thermal mechanical properties of polyimide film: an experiment and molecular dynamics simulation
2021
A series of polyamic acid (PAA) solutions and corresponding polyimide (PI) films with different chemical structures were prepared through a partial pre-imidization process, and the rheological behavior of PAA solutions and thermal mechanical properties of PI films were investigated in detail. The FT-IR spectra indicate that the pre-imidization degree (pre-ID) of PI could be accurately controlled by adjusting the amount of dehydration reagents. The PI films with a certain pre-ID exhibit better mechanical properties and lower coefficient of thermal expansion. The viscosity curves of PAA solution with varying shear rate show that the PAA solutions with high pre-ID have low shear sensitivity, which exhibits a lower viscosity at the low shear rate, but retains almost the same viscosity at high shear rate. Chain conformation variations with pre-IDs and solvent content were investigated by molecular dynamic (MD) simulation. The MD results indicate that a sudden increase in cohesive energy density leads to gel at a certain pre-ID and the mobility of molecular chain decreases greatly with solvent volatilization. It is supposed that the molecular chain orientation induced by the pre-imidization will be preserved in the subsequent thermal imidization process. Therefore, the PI films with a certain pre-IDs exhibit more excellent thermal mechanical properties, especially for the PI with rigid-rod segments.
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