In Situ Stimulation of Self-Assembly Tunes the Elastic Properties of Interpenetrated Biosurfactant–Biopolymer Hydrogels

Hydrogels are widespread soft materials, which can be used in a wide range of applications. The control over the viscoelastic properties of the gel is of paramount importance. Ongoing environmental issues have raised the consumer’s concern toward the use of more sustainable materials, including hydrogels. However, are greener materials compatible with high functionality? In a safe-by-design approach, this work demonstrates that functional hydrogels with in situ responsivity of their elastic properties by external stimuli can be developed from entirely “sustainable” components, a biobased amphiphile and biopolymers (gelatin, chitosan, and alginate). The bioamphiphile is a stimuli-responsive glycolipid obtained by microbial fermentation, which can self-assemble into fibers, but also micelles or vesicles, in water under high dilution and by a rapid variation of the stimuli. The elastic properties of the bioamphiphile-/biopolymer-interpenetrated hydrogels can be modulated by selectively triggering the phase transition of the glycolipid and/or the biopolymer inside the gel by mean of temperature or pH.