Despite existing in biological systems, developing synthetic polyampholyte (PA) hydrogels constructed by both ionic and metal–ligand bonds remains challenging. Herein, a simple secondary equilibrium approach is proposed to fabricate strong and tough PA hydrogels via the synergy of ionic and metal–ligand bonds. The original PA gels (constructed by ionic bonds) are first dialyzed in multivalent metal‐ion solutions to reach a swelling equilibrium and then moved to deionized water to dialyze excess free ions to achieve a new equilibrium. Through this approach, the original PA gel network can be optimized and eventually constructed by ionic and metal–ligand bonds, enabling a synergistic reinforcement. By selecting different original PA gel systems and diverse multivalent metal‐ions, the proposed approach is proved to be generalizable to fabricate strong and tough PA gels. Additionally, the hydrogels have stable ion‐conductivity even at the water‐equilibrium state, making them promising as strain sensors. The viscoelastic and elastic contributions to the mechanical properties of the hydrogels by a viscoelastic model are also discussed to further understand the strengthening and toughening mechanisms. The proposed strategy is simple but effective for achieving strong and tough PA‐based hydrogels. This study also provides new insights for PA hydrogels in electrolyte environments.
Hydrogels with high mechanical strength, good crack resistance, and good adhesion are highly desirable in various areas, such as soft electronics and wound dressing. Yet, these properties are usually mutually exclusive, so achieving such hydrogels is difficult. Herein, we fabricate a series of strong, tough, and adhesive composite hydrogels from polyampholyte (PA) gel reinforced by nonwoven cellulose-based fiber fabric (CF) via a simple composite strategy. In this strategy, CF could form a good interface with the relatively tough PA gel matrix, providing high load-bearing capability and good crack resistance for the composite gels. The relatively soft, sticky PA gel matrix could also provide a large effective contact area to achieve good adhesion. The effect of CF content on the mechanical and adhesion properties of composite gels is systematically studied. The optimized composite gel possesses 35.2 MPa of Young’s modulus, 4.3 MPa of tensile strength, 8.1 kJ m−2 of tearing energy, 943 kPa of self-adhesive strength, and 1.4 kJ m−2 of self-adhesive energy, which is 22.1, 2.3, 1.8, 6.0, and 4.2 times those of the gel matrix, respectively. The samples could also form good adhesion to diverse substrates. This work opens a simple route for fabricating strong, tough, and adhesive hydrogels.
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