Synergy of Hofmeister effect and ligand crosslinking enabled the facile fabrication of super-strong, pre-stretching-enhanced gelatin-based hydrogels

Hydrogels are becoming increasingly popular in biomedical and soft machine manufacturing, but their practical application is limited by poor mechanical properties. In recent years, Hofmeister effect-enhanced gelatin hydrogels have become popular. However, the synergy of the Hofmeister effect using other toughening methods is still less investigated. We have fabricated an ultra-high strength gelatin-based hydrogel by introducing ligand cross-linking and hydrogen bonds. Unlike conventional double-network hydrogels, the dense physical cross-linking involving sacrificial bonds gives the hydrogel excellent fatigue resistance and self-recovery properties. The enhancement of mechanical properties by the Hofmeister effect is attributed to the disruption of the hydration shell of the gelatin molecular chains, which leads to stronger interactions between the molecular chains. The mechanical properties of the hydrogels are adjustable over a wide range by varying the concentration of the soaked (NH₄)₂SO₄ solution. The fixation of the gelatin molecular chain orientation by the Hofmeister effect and the reorganization of the coordination bonds allow the hydrogels to be self-reinforced by pre-stretching. At the same time, the modulus contraction of hydrogels in high-concentration salt solutions, and relaxation and swelling in dilute solutions exhibit ionic stimulation responses and shape recovery capability, and hybrid hydrogels have great potential as bio-actuators.