One-step synthesis of self-healable hydrogels by the spontaneous phase separation of linear multi-block copolymers during the emulsion copolymerization

Abstract Self-healable polyacrylamide-based hydrogels were prepared at room temperature via a one-step emulsion copolymerization of acrylamide (AM), dodecyl 2-methacrylate (DM), and 5-acetylaminopentyl acrylate (AAPA) using sodium dodecyl sulfonate (SDS) as the emulsifier and ammonium persulfate (APS) as the initiator. The produced linear multi-block copolymer chains are composed of randomly-linked hydrophilic polyacrylamide segments (PAM) and hydrophobic segments constituted by DM and AAPA units (P(DM- co -AAPA)). The P(DM- co -AAPA) segments will self-aggregate into hydrophobic microdomains during the polymerization process driven by the hydrophobic interactions, and finally separate from water phase, acting as the crosslinks and leading to the formation of strong hydrogels with a storage modulus as high as 400 Pa. These hydrophobic microdomains will be dissolved in water when the temperature increases to 70 °C, resulting in a temperature-responsive reversible sol-gel transition of the prepared hydrogels. Furthermore, the prepared hydrogels have excellent self-healing ability. The broken hydrogels can be automatically healed into a body with a same strength within 2-min’s contact. This work provides a new simple way to prepare reversible physical crosslinked hydrogel with high strength and self-healing efficiency.