Engineering heterogeneous hierarchical hydrogels based on Artemisia sphaerocephala Krasch polysaccharide/whey protein isolate fibrils aqueous two-phase emulsion

Emulsion-templating techniques have been used to develop structurally anisotropic hydrogels. This paper proposes a method to couple biopolymer assembly behavior with a phase-separated aqueous two-phase system (ATPS) to construct a hierarchical structure on protein-polysaccharide hydrogels. Based on the phase separation of Artemisia sphaerocephala Krasch polysaccharide (ASKP) and whey protein isolate (WPI) fibrils, a bi-continuous hydrogel was fabricated through spontaneous iron-facilitated molecular chelation. The impact of WPI fibrils under ultrasonic treatment for varying duration on gel structurization and physicochemical properties was also exploited. Shorter length of WPI fibrils facilitated stepwise cross-linking gelation during the oxidation of ferrous ions to ferric ions. Specifically, ultrasonic treatment for 6 min and 8 min promoted the accumulation of shorter fibrils, resulting in the formation of a more intensive clockwise-oriented hierarchical network. Compared to the hydrogels with longer linear aggregates without the ultrasonic treatment, the incorporation of the shorter aggregates resulting from ultrasonic treatment for 6 min and 8 min significantly increased the gel's water holding capacity and mechanical properties. Additionally, the fibrils that underwent ultrasonic treatment for 6 min resulted in a more stable three-dimensional network with optimal elastic performance. This study presents a new w-w emulsion-templated strategy for structural regulation and stabilization of multiform hydrogels.