Dual Physical Crosslinking Strategy to Construct Moldable Hydrogels with Ultrahigh Strength and Toughness

Abstract A dual physical crosslinking (DPC) strategy is used to construct moldable hydrogels with ultrahigh strength and toughness. First, polyelectrolyte complex (PEC) hydrogels are prepared through the in situ polymerization of acrylic acid monomers in the concentrated chitosan (Ch) solutions. Subsequently, Ag + ions are introduced into the PEC hydrogels to form coordination bonds between NH 2 and COOH groups. High‐density electrostatic interaction and coordination bonds endow the DPC hydrogels with high strength and toughness. The mechanical properties of the DPC hydrogels strongly depend on the weight ratio of Ch to poly(acrylic acid) and the loading concentration of Ag + ions. When the loading concentration of Ag + ions is in the range of 1.0–1.5 mol L −1 , DPC 0.10–0.25 hydrogels display the maximum tensile strength (24.0 MPa) and toughness (84.7 MJ m −3 ) with a strain of more than 600%. Specially, the DPC hydrogels display an excellent moldable behavior due to the reversible properties of the electrostatic interaction and coordination bonds. The DPC strategy can also be applied in various other systems and opens a new avenue to fabricate hydrogels with outstanding mechanical properties and antibacterial activities.