Reversible hydrogels with switchable diffusive permeability

Abstract

Hydrogels are polymer networks swollen in water that are characterized by soft mechanics and high permeability. This makes them good candidates for separation and membrane technologies. The diffusion is controlled by the mesh size of the network, and this can be made tunable through the introduction of thermoresponsive polymers. However, this is still a developing field. To contribute to this development, a dual dynamic network is formed composed of four-arm polyethylene glycol precursors in which each arm is functionalized with both a terpyridine moiety capable of forming reversible metal–ligand complexes along with branches of poly(N-isopropylacrylamide) (pNIPAAm), which can be switched between expanded and collapsed states and therewith offers a path for switching the microscopic gel-network mesh size, along with the macroscopic gel elasticity. The dually sensitive hydrogel has the capability of doubling its elastic modulus when going above the lower critical solution temperature (LCST) of pNIPAAm. In addition, the diffusive permeability of the hydrogel is switched upon change of temperature, whereby diffusants are trapped above the LCST of pNIPAAm. Moreover, it is possible to disassemble and reform the gel upon change of pH. With that, the hydrogel has potential application as a switchable and reversible membrane.