Design of <scp>PEG</scp> ‐Based Hydrogels as Soft Ionic Conductors

Conductive hydrogels have gained interest in biomedical applications and soft electronics. To tackle the challenge of ionic hydrogels falling short of desired mechanical properties in previous studies, our investigation aimed to understand the pivotal structural factors that impact the conductivity and mechanical behavior of polyethylene glycol (PEG)-based hydrogels with ionic conductivity. Polyether urethane diacrylamide (PEUDAm), a functionalized long-chain macromer based on PEG, was used to synthesize hydrogels with ionic conductivity conferred by incorporating ions into the liquid phase of the hydrogel. The impact of salt concentration, water content, temperature, and gel formation on both mechanical properties and conductivity was characterized to establish parameters for tuning hydrogel properties. To further expand the range of conductivity available in these ionic hydrogels, 2-acrylamido-2-methyl-1-propanesulfonic acid (AMPS) was incorporated as a single copolymer network or double network configuration. As expected, conductivity in these ionic gels was primarily driven by ion diffusivity and charge density, which were dependent on hydrogel network formation and swelling. Copolymer network structure had minimal effect on the conductivity, which was primarily driven by counter-ion equilibrium; however, the mechanical properties and equilibrium swelling were strongly dependent on network structure. The structure-property relationships elucidated here enable the rationale design of this new double network hydrogel to achieve target properties for a broad range of biomedical applications.