New insights into pure zwitterionic hydrogels with high strength and high toughness

Zwitterionic hydrogels are electrically neutral materials with both cationic and anionic groups that impart excellent anti-fouling properties and ion channel orientations. However, pure zwitterionic hydrogels generally exhibit low strength and toughness. In this study, it has been discovered that polymerizable zwitterionic monomers in aqueous solution exhibit a unique liquid-liquid phase separation phenomenon at a high monomer concentration of ≥50 wt%, resulting in pure and commercial zwitterionic hydrogels with high compressive strength (6.5 MPa) and high toughness (2.12 kJ m^-2). This phase separation and the corresponding aggregations might be caused by strong dipole-dipole interactions among residual zwitterionic monomers under the lack of free-water condition. The synergistic effect of liquid-liquid phase separation and polymer entanglement enhances the mechanical strength, toughness, self-recovery, and anti-freezing properties of pure polyzwitterionic hydrogels. Moreover, the high fracture energy of highly elongated yet tough polyzwitterionic hydrogels facilitates the development of high crack propagation resistance, which supports an expanded role in tissue engineering, soft flexible devices, and electronics applications with improved durability. A wide range of applications for the proposed polyzwitterionic hydrogels is demonstrated by the development and testing of a strain sensor and a triboelectric nanogenerator device. Our findings provide novel insights into the network structure of pure polyzwitterionic hydrogels.