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

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.