Hofmeister Effect‐Assisted One Step Fabrication of Ductile and Strong Gelatin Hydrogels

Hydrogels with high strength and ductility are normally prepared from synthetic polymers, and most protein‐based hydrogels are soft and brittle. Here, a strong, ductile gelatin hydrogel is prepared by simply soaking a virgin gelatin gel in an ammonium sulfate solution. The polymer chains in the covalent, crosslink‐free network can freely move to homogeneously distribute stress, and more importantly, the highly kosmotropic ammonium sulfate ions greatly enhance the hydrophobic interactions and chain bundling within the gelatin gels. As a result, the treated hydrogels have an extraordinary ultimate strength (compressive and tensile strains of over 99% and 500%, respectively, and stresses of 12 and 3 MPa) superior to that of common protein gels. The physical crosslinks introduced by the Hofmeister effect can rapidly absorb energy and sustain large deformations via decrosslinking and dissociation, which result in energy dissipation and antifatigue properties. The effects of the gelatin and (NH4)2SO4 concentrations on the hydrogel mechanics are evaluated, and the possible strengthening mechanism is discussed. The effect of various ions in the Hofmeister series on the gelatin hydrogel is also investigated. Kosmotropic ions enhance the mechanical properties, whereas chaotropic ions soften and dissolve the gel. A gelatin‐based, strong, ductile hydrogel is prepared by soaking a virgin gelatin hydrogel in ammonium sulfate solutions. Chain bundling, hydrophobic interactions, and microphase separation regions induced by the Hofmeister effect endow the hydrogels with superior mechanical properties.