Engineering hydrophobically associated hydrogels with rapid self‐recovery and tunable mechanical properties using metal‐ligand interactions

Abstract In this contribution, hydrophobic association and metal‐ligand coordination have been employed in a dual physical crosslinking strategy to access hydrogels based on micellar copolymerization of acrylamide and a hydrophobic acrylic monomer (containing terpyridine (terpy) for metal‐ligand interaction). The mechanical properties of these hydrogels are strongly influenced by the thermodynamic stability and kinetic lability of the metal‐terpy crosslinks present in these materials. While the hydrogel tensile strength and stability on water exposure are enhanced by choosing stronger Fe 2+ ‐terpy crosslinks, the weaker and more kinetically labile Zn 2+ ‐terpy coordination bonds enable significantly higher energy dissipation under tensile loading and self‐healing in the resultant hydrogels.