ABSTRACT Two‐dimensional (2D) metal–organic frameworks (MOFs) integrating redox‐active linkers enable dense charge sites and open ion pathways for microscale energy storage. We report a quinoidal dicarboxylate ligand, AQM‐H 2 L, derived from p ‐azaquinodimethane, forming crystalline frameworks with Cu 2+ and Zn 2+ nodes. The Cu‐based MOF (AQM‐AQM‐H 2 L‐Cu) exhibits layered sheets (>14 Å spacing) constructed from dinuclear Cu‐carboxylate units and conjugated AQM linkers, which narrow the bandgap and introduce Cu 2+ /Cu + pseudocapacitance. Exfoliated nanosheets (∼5 nm) retain crystallinity and excellent processability. Integrated into graphene films, they deliver areal and volumetric capacitances of 29.6 mF cm −2 and 18.1 F cm −3 , achieving 2.6 mWh cm −3 energy density at 160 mW cm −3 . As ionic fillers (1 wt%) in PEO solid polymer electrolytes, the nanosheets markedly enhance LiFePO 4 cell performance, affording 169.8 mAh g −1 at 0.2 C and 93% retention after 400 cycles. This work establishes quinoidal linkers as a compact and robust design motif for ionically active 2D frameworks toward high‐performance miniature and solid‐state energy devices.
Chen et al. (Wed,) studied this question.
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