A self-supporting biomimetic chemical hydrogel that can be reversibly swollen in water is described. An aqueous dispersion of a diacrylate end-derivatized PEO-PPO-PEO macromer, a saturated phospholipid, and a zwitterionic co-surfactant self-assembles into a multilamellar-structured physical gel at room temperature as determined by SAXS. The addition of a water soluble PEGDA co-monomer and photoinitiator within the water layers does not alter the self-assembled structure. ATR/FT-IR spectroscopy reveals that photoirradiation initiates the crosslinking between the acrylate end groups on the macromer with the PEGDA, forming a polymeric network within the aqueous domains. The primitive cytoskeleton mimic serves to stabilize the amphiphile bilayer, converting the physical gel into an elastic self-supporting chemical gel. Storage under ambient conditions causes dehydration of the hydrogel to 5 wt % water which can be reversed by swelling in water. The fully water swollen gel (85 wt % water) remains self-supporting but converts to a non-lamellar structure. As water is lost the chemical gel regains its lamellar structure. Incubation of the hydrogel in nonpolar organic solvents that do not dissolve the uncrosslinked lipid component (hexane) allow for swelling without loss of structural integrity. Chloroform, which readily solubilizes the lipid, causes irreversible loss of the lamellar structure.
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