Double-Network Tough Hydrogels: A Brief Review on Achievements and Challenges

This brief review attempts to summarize research advances in the mechanical toughness and structures of double-network (DN) hydrogels. The focus is to provide a critical and concise discussion on the toughening mechanisms, damage recoverability, stress relaxation, and biomedical applications of tough DN hydrogel systems. Both conventional DN hydrogel with two covalently cross-linked networks and novel DN systems consisting of physical and reversible cross-links are discussed and compared. Covalently cross-linked hydrogels are tough but damage-irreversible. Physically cross-linked hydrogels are damage-recoverable but exhibit mechanical instability, as reflected by stress relaxation tests. This remains one significant challenge to be addressed by future research studies to realize the load-sustaining applications proposed for tough hydrogels. With their special structure and superior mechanical properties, DN hydrogels have great potential for biomedical applications, and many DN systems are now fabricated with 3D printing techniques.