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

Conductive 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, we report a novel bottom-up approach 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 were first synthesized and self-assembled into uniform polyanionic nanoplatelets. Subsequently, these negatively charged nanoplatelets, with sulfonic groups on the surface, were employed as nano-additives 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 were successfully prepared. In comparison with hydrogels with (PEDOT:PSS)/BCP complexes prepared by a top-down method, the nanocomposite hydrogels were 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. This article is protected by copyright. All rights reserved.