Synthesis and characterization of hydrogels containing <scp>redox‐responsive</scp> 2,2,6,6<scp><b>‐</b>tetramethylpiperidinyloxy</scp> methacrylate and <scp>thermoresponsive <i>N</i>‐isopropylacrylamide</scp>

Abstract Smart hydrogels containing 2,2,6,6‐tetramethylpiperidinoxy methacrylate (TEMPO) and N ‐isopropylacrylamide (NIPAM) that undergo reversible redox behavior are prepared and investigated. Several polymer networks are first prepared by free‐radical copolymerization of varying amounts of TEMPO, NIPAM, and a crosslinker (diethylene glycol diacrylate) and subsequently swelled with water to lead to hydrogels. In order to investigate the effects of the redox activity of TEMPO units and of the lower critical solution temperature of NIPAM on the hydrogel properties, a study of the swelling ratio of the polymer networks in distilled water at different temperatures is performed for the two forms of TEMPO, the reduced (TEMPO) and oxidized (TEMPO + ) one. Moreover, the rheological properties are also measured for both hydrogel forms. Finally, the encapsulation abilities of the oxidized hydrogels are demonstrated via electrostatic interactions between positively charged TEMPO + units and negatively charged guest molecules, supporting future application of our system in the biomedical and environmental fields.