Tunable cross‐linked copolymer networks for improvement of physical performance

Abstract The ability to tune the physical properties of polymeric materials through the different compositions in copolymer networks is suitable for the strategy of materials accompanied by combined high mechanical strength and stretchability simultaneously. Here, we developed a practical and straightforward strategy of a copolymer network structure via controlling the compositions of the acrylic‐based urethane copolymers of diurethane acrylate (DUA) and diurethane cyclic acrylate (DUCA) with hydrogen‐bonds through photo‐polymerization. The copolymer networks led to the development of a physically cross‐linked structure between the amide groups of DUA and/or DUCA and the hydroxyl groups of pentaerythritol ethoxylate (PEEL) by hydrogen‐bonds. Based on the rheological analysis, the composition of the copolymer networks had a significant effect on the control of physical properties and development of cross‐linked structure and thus led to the tunable comprehensive properties including high elastic modulus, high chain mobility and high recovery performance with a higher proportion of DUCA in the copolymer networks. Consequently, the tunable copolymer networks based on the developed physically cross‐linked structure can improve the elastic properties, recovery performance, and healing ability simultaneously, providing significant progress in the fields of coating and adhesive.