A Simple Way to Synthesize a Protective “Skin” around Any Hydrogel

In nature, various structures such as fruits and vegetables have a water-rich core that is covered by a hydrophobic layer, i.e., their skin. The skin creates a barrier that prevents chemicals in the external environment from entering the core; at the same time, the skin also ensures that the water in the core is preserved and not lost by evaporation. Currently, for many applications involving hydrogels, especially in areas such as soft robotics or bioelectronic interfaces, it would be advantageous if the gel could be encased in a skin-like material. However, forming such a skin around a gel has proved challenging because the skin would need to be a hydrophobic material with a distinct chemistry from the hydrophilic gel core. Here, we present a simple solution to this problem, which allows any hydrogel of arbitrary composition and geometry to be encased by a thin, transparent “skin.” Our synthesis technique involves an inside-out polymerization, where one component of the polymerization (the initiator) is present only in the gel core, while other components (the monomers) are present only in the external medium. Accordingly, a thin polymeric layer (∼10–100 μm in thickness) grows outward from the core, and the entire process can be completed in a few minutes. We show that the presence of the skin prevents the gel from swelling in water and also from drying in air. Likewise, hydrophilic solutes in the gel core are completely prevented by the skin from leaking out into the external solution, while harsh chemicals (e.g., acids, bases, and chelators) or harmful microbes are prevented from entering the gels. The properties of the skin are all tunable, including its thickness and its mechanical properties. When the monomer used is urethane diacrylate, the resulting polyurethane skin is elastomeric, transparent, and peelable from the core gel. Conversely, when polyethylene glycol dimethacrylate is used as the monomer, the skin is hard and brittle (glass-like). The ability to grow a skin readily around any given hydrogel is likely to prove useful in numerous applications, such as in maintaining the electrical functionality of gel-based wires or circuit elements.