Supramolecular materials are widely recognized among the most promising candidates for future generations of sustainable plastics because of their dynamic functions. However, the weak noncovalent crosslinks that endow dynamic properties usually trade off materials’ mechanical robustness. Here, learning from ice, we present the discovery of a simple and robust supramolecular crosslinking strategy based on acylhydrazine units, which can hierarchically crosslink the solvent-free network of poly(disulfides) by forming unique reticular hydrogen bonds, enabling the conversion of soft into stiff dynamic material. The resulting supramolecular materials exhibit increase in stiffness exceeding two to three orders of magnitude compared to those based on the hydrogen-bonding network of analogous carboxylic acids, simultaneously preserving the repairability, malleability, and recyclability of the materials. The materials also show high adhesion strength on various surfaces while allowing multiple surface attachment cycles without fatigue, illustrating a viable approach how robustness and dynamics can be merged in future material design.

Ice-inspired reticular hydrogen bonds enable robust, tough and dynamic supramolecular materials

ACS Spring 2022

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