Abstract: Natural composites have inspired the fabrication of various biomimetic composites that have achieved enhancement on certain mechanical performance. Herein, a facial approach enabled by recent advances in polyimine chemistry has been developed to fabricate bio-inspired hard-soft-integrated copolymers from two polyimines (i.e. PI-H and PI-S) with hardness differential. Subsequent evaluations of multiple mechanical properties on the bio-inspired copolymers with PI-S contents of full-range variability (0 wt%–100 wt%) have revealed extremal transitions for friction coefficients, impact strengths and tensile moduli. More interestingly, the minimum points of friction coefficients show a deformation-resisting response toward the change of applied loads, but not for the altered sliding speeds, suggesting a more significant role of load in determining the optimal anti-friction composition of the hard-soft integrated copolymers. These trends have been further corroborated by scanning electron microscopy of the worn specimens. Together these results have demonstrated that full-range extremal transitions exist on multiple mechanical properties for hard-soft-integrated copolymers, providing valuable insights to the design and fabrication of composite polymers for many applications. The polyimine-based approach outlined here also affords a convenient method to tune the ratio of two components in the copolymers within the full range of 0 wt%–100 wt%, enabling quick integration with high content variability.

Key words: bio-inspiration, polyimine, extremal transition, content variability, mechanical properties