Novel Zwitterionic Hydrogels with High and Tunable Toughness for Anti-Fouling Application

Zwitterionic hydrogels have emerged as eco-friendly anti-fouling materials owing to their superior hydration-mediated resistance to biofouling. Nevertheless, their practical utility remains constrained by intrinsically poor mechanical robustness. Herein, this study proposes a novel strategy to develop novel tough zwitterionic hydrogels by freezing the gels' polymer network. As a proof of concept, a zwitterionic hydrogel was synthesized via copolymerization of hydrophobic monomer phenyl methacrylate (PMA) and hydrophilic cationic monomer N-(3-dimethylaminopropyl) methacrylamide (DMAPMA), followed by post-oxidation to yield a zwitterionic structure. At service temperature, the rigid and hydrophobic PMA segments remain frozen, while the hydrophilic zwitterionic units maintain substantial water content by osmotic pressure. Synergistically, the zwitterionic hydrogel achieves robust toughness and adhesiveness, with high rigidity (66 MPa), strength (4.78 MPa), and toughness (2.53 MJ/m³). Moreover, the hydrogel exhibits a distinct temperature-dependent behavior by manifesting softer and more stretchable behavior after heating, since the thawing of the gel network at high temperatures increases segmental mobility. Therefore, it achieved satisfactory adhesiveness to substrates (80 kPa). Additionally, the hydrogel demonstrated remarkable anti-fouling performance, effectively suppressing biofilm formation and larval attachment. In summary, this work opens up promising prospects for the development of zwitterionic hydrogels with high application potential.