Highly Mechanical and Fatigue-Resistant Double Network Hydrogels by Dual Physically Hydrophobic Association and Ionic Crosslinking

Double network (DN) hydrogels with high strength and toughness are considered as promising soft materials. Herein, a dual physically cross-linked hydrophobic association polyacrylamide (HPAAm)/alginate-Ca 2+ DN hydrogel is reported, consisting of a HPAAm network and a Ca 2+ cross-linked alginate network. The HPAAm/alginate-Ca 2+ DN hydrogel exhibits excellent mechanical properties with the fracture stress of 1.16 MPa (3.0 and 1.7 times higher than that of HPAAm hydrogel and HPAAm/alginate hydrogel, respectively), fracture strain of 2604%, elastic modulus of 71.79 kPa, and toughness of 14.20 MJ m −3 . HPAAm/alginate-Ca 2+ DN hydrogels also demonstrate self-recovery, notch-insensitivity, and fatigue resistance properties without any external stimuli at room temperature through reversible physical bonds consisting of hydrophobic association and ionic crosslinking. As a result, the dual physical crosslinking would offer an avenue to design DN hydrogels with desirable properties for broadening current applications of soft materials.