Biological Hydrogels Formed by Swollen Multilamellar Liposomes

The self-assembly of lecithin-bile salt mixtures in solutions has long been an important research topic, not only because they are both biosurfactants closely relevant to physiological functions but also for the potential biomedical applications. In this paper, we report an unusual biological hydrogel formed by mixing bile salts and lecithin at low bile salt/lecithin molar ratios (B0) in water. The gel can be prepared at a total lipid concentration as low as ∼15 wt %, and the solidlike property of the solutions was confirmed by dynamic rheological measurements. We used cryo-TEM and SAXS/SANS techniques to probe the self-assembled structure and clearly evidence that the gel is made up of jammed swollen multilamellar vesicles (liposomes), instead of typical fibrous networks found in conventional gels. A mechanism-based on the strong repulsion between bilayers due to the incorporation of negatively charged bile salts is proposed to explain the swelling of the liposomes. In addition to gel, a series of phases, including viscoelastic, gel-like, and low-viscosity fluids, can be created by increasing B0. Such a variety of phase behaviors are caused by the transformation of bilayers into cylindrical and spheroidal micelles upon the change of the effective molecular geometry with B0.