Muscle-like Ultratough Hybrid Hydrogel Constructed by Heterogeneous Inorganic Polymerization on an Organic Network

Inspired by inorganic oligomers and their polymerization, we herein develop a heterogeneous inorganic polymerization tactic that can be used to prepare a muscle-like hybrid hydrogel by inducing the polymerization of calcium phosphate oligomers (CPO) onto a polyvinyl alcohol (PVA) molecular chain network. In this heterogeneous process, the CPO units bond with PVA molecules via assistance from sodium alginate (SA), and then gradually polymerize along the organic chains to form ultrafine hydroxyapatite nanolines with a diameter of ∼1 nm. Because of the well integration of organic and inorganic phases from the heterogeneous polymerization, the hierarchical structured hydrogel can exhibit ultratough mechanical properties of ∼17.84 MPa in strength and ∼8.97 kJ m^–2 in fracture energy, which exceed natural muscles and almost synthetic hydrogels. Moreover, the damaged hydrogel can be repaired readily by adding the precursors of CPO, PVA, and SA, which can induce in situ re-polymerization. The hydrogel also exhibits muscle-like rotational motion under aqueous conditions, which can be developed into a water-driven biomimetic motor. This study indicates that inorganic polymerization can achieve a novel organic–inorganic integration rather than conventional organic–inorganic composition, and it provides a novel tactic for design and manufacture of advanced materials.