Regulating Electrostatic Interactions toward Thermoresponsive Hydrogels with Low Critical Solution Temperature

Abstract Low critical solution temperature (LCST) of commonly used thermoresponsive polymers in water is basically dominated by hydrophobic interactions. Herein, a novel thermoresponsive system based on electrostatic interactions is reported. By simply loading aluminum chloride (AlCl 3 ) into non‐responsive poly(2‐hydroxyethyl acrylate) (PHEA) hydrogels, PHEA‐Al gels turn to have reversible thermoresponsive behavior between transparent and opaque without any volume change. Further investigations by changing metal ion‐polymer compositions unravel the necessity of specific electrostatic interactions, namely, cation‐dipole bonding interactions between hydroxy groups and trivalent metal ions. The thermoresponsive hydrogel demonstrates high transparency (≈95%), excellent luminous modulation capability (>98%), and cyclic reliability, suggesting great potential as an energy‐saving material. Although LCST control by salt addition is widely known, salt‐induced expression of thermoresponsiveness has barely been discussed before. This design provides a new approach of easy fabrication, low cost, and scalability to develop stimuli‐responsive materials.