Chitosan derivative-based double network hydrogels with high strength, high fracture toughness and tunable mechanics

Physically cross-linked double-network (DN) hydrogels are capturing more and more attention due to their good mechanical properties and self-recovery ability. However, they usually suffer from complicated preparation process and fussy performance regulation, which severely limit their applications in many fields. Herein, we fabricated a physically cross-linked poly(vinyl alcohol)-(2-hydroxypropyltrimethyl ammonium chloride chitosan) (PVA-HACC) DN hydrogels without organic solvents or toxic cross-linking agents via a simple two-step method of freezing/thawing and immersion processing. The effects of immersion time and concentration of Na₃Cit solution on the structures and mechanical properties of the hydrogels were investigated. The obtained hydrogels exhibited excellent mechanical properties including high elastic modulus (1.44 MPa), high strength (a maximal tensile fracture stresses of 4.14 MPa and a maximal compressive stresses of over 70 MPa at 98% strain), and superior fracture toughness (17.09 MJ/m³). In addition, good self-recovered property and anti-fatigue performance were realized for the hydrogels owing to the reversible HACC ionic networks. The preparation of PVA-HACC DN hydrogels offers a new guidance for the design and synthesis of environmentally friendly DN hydrogels with outstanding mechanical properties and broad application prospects.