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Ice-templating, also referred to as freeze-casting, is a process exploitingunidirectional crystallization of ice to structure macroporous materials fromcolloidal solutions. Commonly applied to inorganic and polymeric materials, weemploy it here to cast soft self-assembled matter into spongy solid foams. Useof ice-templating to cast soft matter is generally confined to polymers. In thecase of polymeric hydrogels, cross-linking ensures a good stability towards theharsh conditions (fast cooling at temperatures as low as-80{\textdegree}C)employed during ice-templating. However, freeze-casting of soft systems heldtogether by weak interactions, like in physical gels, has not been explored,because the nonequilibrium conditions could easily disrupt the nano andmacroscale organization of self-assembled matter, resulting in a cruel loss ofmechanical properties. Whether this is a general assumption or a more specificrelationship exists between the structure of the physical gel and theproperties of the macroporous solid after ice-templating is the questionaddressed in this work. We compare two self-assembled lipid hydrogels, ofanalogous chemical composition and comparable elastic properties under ambientconditions, but different structure: isotropic entangled self-assembled fibersagainst heterogeneous lipid lamellar phase. Our results show that bothmaterials possess the same phase (fibrillar and lamellar) before 2 and afterfreeze-casting but the mechanical properties are absolutely at the opposite:the fibrillar hydrogel provides a brittle, highly anisotropic, macroporousfibrous solid while the lamellar hydrogel provides soft, spongy, solid foamwith isotropic Young moduli of several kPa, in the same order of magnitude assome soft living tissues.

Soft lamellar solid foams from ice-templating of self-assembled lipid hydrogels: organization drives the mechanical properties