Enhancing the Properties of Self-Healing Gelatin Alginate Hydrogels by Hofmeister Mediated Electrostatic Effect

The cross-linker-free hydrogels have gained attention due to their lack of need for chemically modified polymers, resulting in better biocompatibility. The hydrogel properties can be enhanced by altering physical forces such as electrostatics and H-bonds. Tuning the physical interactions between polymers, salts, and plasticisers can unlock new horizons in material properties. This article examines four different salts and mixtures to determine their impact on gelatin-alginate biomaterial design. Drug release, swelling, and rheological properties are represented using a 3-D plot, and optimum samples are identified. It is concluded that kosmotropes yield better release and swelling results than chaotropes. The physical interactions of these salts with polymers are explained using DLS and FTIR/ATR studies, and these findings are corroborated with release, swelling, and rheological analyses. Another aspect of the biomaterial, self-healing property, is also considered. A 3-D plot is prepared using release kinetics, gel strength, and recovery percentage (three important factors for self-healing hydrogels). Chaotropes are identified as better candidates for self-healing behaviour. However, when considering gel strength, release, and self-healing, kosmotropes are favourable. Hence, different salts can be selected based on the desired application for hydrogels. It is also concluded that electrostatic forces hinder the formation of H-bonds between polymer chains. Kosmotropes are unable to screen the positive charges on gelatin due to lower mobility and repulsions from amide bonds, which leads to more interactions between gelatin and alginate. Chaotropes having higher mobility are able to screen the positive charges on gelatin, leading to fewer interactions between gelatin and alginate. These interactions, in turn, impact the drug release, swelling, degradation, rheology and self-healing properties.image