Fast Recovery Double-Network Hydrogels Based on Particulate Macro-RAFT Agents

Synthetic hydrogels struggle to match the high strength, toughness, and recoverability of biological tissues under periodic mechanical loading. Although the hydrophobic polymer chain of polystyrene (PS) may initially collapse into a nanosphere upon contact with water, it has the ability to be elongated when it is subjected to an external force. To address this challenge, we employ the reversible addition–fragmentation chain transfer (RAFT) method to design a carboxyl-substituted polystyrene (CPS) which can form a covalently cross-linked network with four-armed amino-terminated polyethylene glycol (4-armed-PEG-NH2), and a ductile polyacrylamide network is introduced in order to prepare a double-network (DN) hydrogel. Our results demonstrate that the DN hydrogel exhibits exceptional mechanical properties (0.62 kJ m–2 fracture energy, 2510.89 kJ m–3 toughness, 0.43 MPa strength, and 820% elongation) when a sufficient external force is applied to fracture it. Moreover, when the DN hydrogel is subjected to a 200% strain, it displays superior recoverability (94.5%). This holds a significant potential in enhancing the mechanical performance of synthetic hydrogels and can have wide-ranging applications in fields such as tissue engineering for hydrophobic polymers.