Correlating Ionic Conductivity and Microstructure in Polyelectrolyte Hydrogels for Bioelectronic Devices

Hydrogels have become the material of choice in bioelectronic devices because their high-water content leads to efficient ion transport and a conformal interface with biological tissue. While the morphology of hydrogels has been thoroughly studied, systematical studies on their ionic conductivity are less common. Here, an easy-to-implement strategy is presented to characterize the ionic conductivity of a series of polyelectrolyte hydrogels with different amounts of monomer and crosslinker and correlate their ionic conductivity with microstructure. Higher monomer increases the ionic conductivity of the polyelectrolyte hydrogel due to the increased charge carrier density, but also leads to excessive swelling that may cause device failure upon integration with bioelectronic devices. Increasing the amount of crosslinker can reduce the swelling ratio by increasing the crosslinking density and reducing the mesh size of the hydrogel, which cuts down the ionic conductivity. Further investigation on the porosity and tortuosity of the swollen hydrogels correlates the microstructure with the ionic conductivity. These results are generalizable for various polyelectrolyte hydrogel systems with other ions as the charge carrier and provide facile guidance to design polyelectrolyte hydrogel with desired ionic conductivity and microstructure for applications in bioelectronic devices.