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Rational Design of Pyrene-Based Metal-Free Covalent Organic Frameworks for Supercapacitor Application
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DOI：10.1039/D6NJ01264G.png)
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Abstract
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Rationally designed covalent organic frameworks (COFs) have garnered attention as advanced electrode materials for energy storage due to their ordered π-conjugated network; porous framework; and excellent stability. Judicious selection of redox-active organic moieties for COFs may impart intrinsic redox properties; efficient charge transfer; and high electrical conductivity; enabling high-performance supercapacitors. Considering this; a series of pyrene-based donor-acceptor COFs was prepared using porphyrin; pyrene; and diarylamine as π-conjugated monomers. While pyrene serves as the primary electron-donor unit in each COF; porphyrin and diarylamine moieties act as redox-active electron-acceptor sites; forming a donor-acceptor architecture within the COFs to enhance redox capability and ion transport; thereby enhancing the framework's electrochemical activity. Each COF exhibits long-range ordered structure with high porosity and has been further investigated for supercapacitor application. Among them; the porphyrin-incorporated COF exhibited high capacitive behavior; delivering a maximum specific capacitance of 178 F g−1 at a current density of 3.5 A g−1 with >90% retention of capacitance after 9000 cycles in a three-electrode setup. Additionally; the asymmetric device for the porphyrin-based COF showed a specific capacitance of 47 F g−1 at 0.75 A g−1; with an energy density of 14.7 Wh kg−1 and a power density of 583 W kg−1. The high performance of the porphyrin-based COF is rationalized by a crystalline porous network; redox-active sites; and a donor-acceptor architecture; which enable efficient ion diffusion and rapid electron transport during charge-discharge processes.
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