Fabrication of Uniform Anionic Polymeric Nanoplatelets as Building Blocks for Constructing Conductive Hydrogels with Enhancing Conductive and Mechanical Properties

Abstract

AbstractConductive hydrogels play a crucial role in advancing technologies like implantable bioelectronics and wearable electronic devices, owing to their favorable conductivity and appropriate mechanical properties. Here, a novel bottom‐up approach is reported for crafting conductive nanocomposite hydrogels to achieve enhancing conductive and mechanical properties. In this approach, new poly(ɛ‐caprolactone)‐based block copolymers with sulfonic groups are first synthesized and self‐assembled into uniform polyanionic nanoplatelets. Subsequently, these negatively charged nanoplatelets, with sulfonic groups on the surface, are employed as nanoadditives for the polymerization of 3,4‐ethylenedioxythiophene (EDOT), resulting in poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)/nanoplatelet complex with 3.8 times enhanced electrical conductivity compared with their counterparts prepared using block copolymers (BCPs). Blending the (PEDOT:PSS)/nanoplatelet complex with calcium alginate, nanocomposite hydrogels are successfully prepared. In comparison with hydrogels with (PEDOT:PSS)/BCP complexes prepared by a top‐down method, the nanocomposite hydrogels are found to show twice as strong mechanical strength and 1.6 times higher conductivity. This work provides valuable insights into the bottom‐up construction of conductive hydrogels for bioelectronics using well‐controlled polymeric nanoplatelets.