Ultraductile, notch and stab resistant supramolecular hydrogels via host–guest interactions

Various supramolecular materials, especially hydrogels, based on host–guest interactions have been widely studied due to their attractive properties and potential applications. However, many of their practical uses are still severely limited by their poor mechanical performance. In this report, we present a novel kind of supramolecular hydrogel showing extremely ductile, notch and stab resistant properties as well as excellent self-healing behavior. These supramolecular hydrogels are prepared by simple free-radical copolymerization of acrylamide and adamantane monomers which were preloaded on low molecular weight poly(AOI-β-cyclodextrin) (pAOI-β-CD). We attribute the hydrogel's exceptional mechanical performance to the synergy effect of the supramolecular imprint and movable multi-valent supramolecular crosslinker characters of pAOI-β-CD in forming reversible crosslinking before and after polymerization, respectively. The findings of this work provide the basis for the molecular design of supramolecular soft materials with distinguished mechanical performance, and will expand the scope of host–guest supramolecular hydrogel applications.