Supramolecular Self-Assembly of Polyaniline Embedded Enzyme-Mimicking GMP-Condensate Hydrogel for Electrochromic Energy Storage Applications

Abstract

Conductive polymer hydrogels combine the electrical conductivity of organic polymers with the high water content, porosity, and tissue-mimicking properties of hydrogels, making them ideal for bioelectronic interfaces. However, traditional polymer matrices often lack biocompatibility, self-healing ability, dynamic reconfigurability, and tunable mechanical properties. To address these challenges, herein we report a dimeric guanosine monophosphate (GMP)-based supramolecular hydrogel that self-assembles into a fibrillar network with intrinsic peroxidase-mimetic activity in a metal-free, microconfined environment. This unique catalytic property enables the in situ oxidative polymerization of aniline into polyaniline nanofibers, forming a hybrid conductive hydrogel with excellent mechanical strength, self-healing capability, stimuli-responsive sol–gel transitions, and high ionic conductivity. The resulting hydrogel was used to fabricate electrochromic energy-storing electrodes and “all-solid-state” supercapacitors with high capacitance (343 mF cm–2) and energy density (93.36 Wh cm–2). This work highlights the potential of small biomolecules as artificial enzyme mimics and structural matrices for transforming biomolecular self-assemblies into functionally conductive hydrogels. The integration of biomolecules for enzyme-mimetic catalysis for generating the conducting polymer hydrogels might provide a versatile platform for advancing bioelectronic technologies. © 2025 Elsevier B.V., All rights reserved.