Biomimetic design of elastomers with improved mechanical properties by integrating hydrogen bonds with covalent crosslinking bonds

Abstract

It is an important issue for rubber to realize reinforcement and expand application gallery in material science and engineering. In the present work, we initiated a bioinspired design to introduce sacrificial hydrogen bonds by post-modifying sulfur crosslinked carboxyl nitrile rubber with pendent urazole through triazolinedione “click” chemistry. The post-modification of the crosslinked rubber can not only avoid adverse effect of the grafted urazoles on rubber vulcanization, but also enable to evaluate the effect of sacrificial hydrogen bonds on the rubber based on a consistent covalent network. Under external stress, the hydrogen bonds between the urazoles can function as sacrificial bonds that would rupture prior to covalent bonds, during which enormous energy is dissipated and meanwhile facilitates the rubber chain orientation. In light of the unique energy dissipating mechanism, the modulus, ultimate stress, and toughness of the hydrogen bonds and sulfur bonds dual-crosslinked rubber material are improved simultaneously without sacrificing the stretchability, and these properties can be easily manipulated by varying the grafting ratio of urazoles.