with an ionic cross-linking alginate-Ca 2+ network, which exhibit highly stretchable property of beyond 20 times their initial length and remarkable fracture energy of nearly 9 kJ m −2 . [15] Chen et al. engineered hybrid Agar/PAM hydrogels, which exhibited high stiffness of 313 kPa and high toughness of 1089 J m −2 . [16] They also fabricated fully physical cross-linking DN hydrogels combing Agar with hydrophobic associated PAM, which showed rapid selfrecovery and self-healing properties at room temperature. [17] Besides, integrating the covalent bonds and physical bonds into a single network has attracted more and more attention. Hu et al. prepared PAM/ carbon nanodot hybrid hydrogels using carbon nanodot as physical cross-linker. The fabricated hydrogel, even in the swelling equilibrium state, keeps extraordinary mechanical and recoverable properties. [18] Xie and co-workers synthesized poly(acrylic acid) hybrid hydrogels by introducing ionic cross-linking interaction between Fe(III) and carboxyl groups into the chemical cross-linking network, and the resulting hydrogels achieve tensile stress of ≈1.07 MPa and toughness of ≈11.7 MJ m −3 . [19] In these network structures, the covalent cross-linking preserved the initial state of the network and the recoverable physical cross-linking could well disperse the stress concentration during deformation process, resulting in excellent mechanical property of these hydrogels. However, these hydrogels presented apparently poor elasticity and large residual strain after cyclic tensile test. Therefore, fabricating hydrogels simultaneously owing high toughness and elasticity remains a challenge.Molecular self-assembly behavior plays an important role in biological systems. [20] For example, cell membranes share a common structure of phospholipid bilayers, formed by the self-assembly of amphiphilic molecules. Besides, amphiphilic molecules can also form a variety of self-assembled morphologies, such as micelles, hexagonal, and cubic phases, which have been attracting significant attention for the purpose of fabricating tough hydrogels. Interesting examples are presented by the hydrogels crosslinked by micelles. [21,22] In such hydrogels, crack energy can be efficiently dissipated by flexible dislocation of polymeric micelles along with the chain slippage, leading to highly stretchable and excellent resilience of hydrogels. [21] As a result, it was envisioned that the combination of covalent bonds and physical interactions from self-assembled micelles is a viable method to prepare hybrid hydrogel with extraordinary mechanical performance.
HydrogelsIn this work, a hybrid cross-linked polyacrylamide (PAM)/cationic micelle hydrogel is fabricated by introducing the cationic micelles into the chemically cross-linked PAM network. The cationic micelles act as the physical cross-linking points through the strong electrostatic interaction with anionic initiator potassium persulfate. Thereafter, in situ free radical polymerization is initiated thermally from the cationic micelle surfac...