Unlocking Rapid Ion-Electron Kinetics via Amorphous 2,6-Diaminopyridine Covalent Organic Frameworks and Monoclinic WO3 Heterointerfaces for High-Performance Energy Storage

Abstract Covalent organic frameworks (COFs) possess diverse porous architectures and tailored structural features, making them platforms for advanced energy-storage systems. Here, we report, for the first time, a synergistic composite of SR-COF and monoclinic tungsten trioxide, exhibiting enhanced pseudocapacitive charge storage. The SR-COF is synthesized via condensation of 2,6-diaminopyridine and 1,3,5-benzenetricarbaldehyde through imine linkages, forming an irregular, highly aggregated porous morphology comprising interconnected spherical voids like a network with a rough and textured surface, providing an efficient framework for energy storage. Synergistic integration with WO3 effectively mitigates the intrinsic limitations of pristine COFs, thereby enhancing charge-storage capability. Electrochemical evaluation of the solid-state symmetric device, employing graphite flakes as a current collector and PVA-H2SO4 gel as an electrolyte, has demonstrated a high energy density of 94.44 Wh kg–1 at a power density of 1133 W kg–1 at 1 A g–1. The device retains 83.2% of its capacitance with a Coulombic efficiency of 102.9% after 10,000 cycles at 30 A g–1, underscoring its excellent durability and potential for next-generation high-performance supercapacitor applications. The assembled supercapacitor device is charged to approximately 1.0 V using a commercially available external power source for 5 min and then successfully used to illuminate a light-emitting diode (LED), confirming its potential for real-world energy storage applications.