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Controlling the viscoelastic properties of hydrogels is a challenge for manyapplications. Low molecular weight gelators (LMWG) like bile salts andglycolipids, and biopolymers like chitosan and alginate, are good candidatesfor developing fully biobased hybrid hydrogels that combine the advantages ofboth components. Biopolymers lead to enhanced mechanics while LMWG addfunctionality. In this work, hybrid hydrogels are composed of biopolymers(gelatin, chitosan, alginate) and microbial glycolipid bioamphiphiles, known asbiosurfactants. Besides their biocompatibility and natural origin,bioamphiphiles can present chameleonic behavior, as pH and ions control theirphase diagram in water around neutrality under strongly diluted conditions (< 5wt%). The glycolipid used in this work behaves like a surfactant (micellarphase) at high pH or like a phospholipid (vesicle phase) at low pH. Moreover,at neutral-to-alkaline pH in the presence of calcium, it behaves like a gelator(fiber phase). The impact of each of these phases on the elastic properties ofbiopolymers is explored by means of oscillatory rheology, while the hybridstructure is studied by small angle X-ray scattering. The micellar andvesicular phase reduce the elastic properties of the hydrogels, while the fiberphase has the opposite effect, it enhances the hydrogel's strength by formingan interpenetrated biopolymer-LMWG network.

Interpenetrated biosurfactant-biopolymer orthogonal hydrogels: the biosurfactant's phase controls the hydrogel's mechanics