Abstract
In various bioelectronic applications, conductive polymers come into contact with biological tissues, where water is the major component. In this study, we investigated the interface between the conductive polymer poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) and water, focusing on how the morphology of the PEDOT:PSS is altered by water permeation. We constructed well-equilibrated PEDOT:PSS-water systems in both PEDOT- and PSS-rich phases. Our findings show that water permeates into the polymer through a complex network of water channels, which exhibit a similar pore size distribution in both PEDOT- and PSS-rich phases, leading to similar water intake in these phases. Compared to the dry state of the polymer, water permeation leads to the formation of smaller, less ordered, and distantly located lamella crystallites, potentially resulting in reduced conductivity. Therefore, we argue that these structural changes from the dry state of the polymer to the wet state may be the origin of the significant conductivity reduction observed experimentally in PEDOT:PSS in water or PEDOT:PSS hydrogels.