Electrochemical-mediated gelation of catechol-bearing hydrogels based on multimodal crosslinking

Catechol-bearing polymers form hydrogel networks through cooperative oxidative crosslinking and coordination chemistry. Here we describe the kinetics of cation-dependent electrochemical-mediated gelation of precursor solutions composed of catechol functionalized four-arm poly(ethylene glycol) combined with select metal cations. The gelation kinetics, mechanical properties, crosslink composition, and self-healing capacity is a strong function of the valency and redox potential of metal ions in the precursor solution. Catechol-bearing hydrogels exhibit highly compliant mechanical properties with storage moduli ranging from