Confinement of Oligopeptides by Terminally Functionalized Polyisoprene to Improve Their Mechanical Strength, Creep Resistance, and Antifatigue Properties

A small amount of terminal polar phase endows natural rubber (NR) with excellent comprehensive properties superior to those of synthetic isoprene rubber. In this work, the comprehensive properties of synthetic rubber were remarkably improved by introducing a stable terminal nanoconfinement structure by combining terminal hydroxyl groups and pentapeptide molecules noncovalently into the same phases. The results show that the stable terminal phases hardly affect the free chain motion but enhance the entanglement. Under cyclic loading, the terminal polar phases undergo hierarchically structural changes such as reversible dissociation of the weak bonds, phase deformation, and crystalline reorganization, all of which dissipate the stress and are beneficial for high strength and extensibility. At the same time, synthetic rubbers demonstrate much superior fatigue resistance and lower hysteresis relative to NR and maintain comparable dimensional stability. This strategy suggests that the comprehensive properties of elastomers can be regulated and upgraded by facile terminal noncovalent interactions.