Ultrafast-charging and durable organic cathodes enabled by two-dimensional supramolecular engineering

Abstract Strong demands for ultrafast-charging yet durable batteries drive research into high-performance organic electrodes beyond conventional layered metal oxides. Small-molecule organic electrode materials suffer from sluggish ion diffusion and high dissolution in electrolytes, thereby limiting their practical usage. Here we report a sulfur-heterocyclic extension strategy of redox-active triptycene tribenzoquinone molecules, enabling self-assembly into two-dimensional porous nanosheets with architectural robustness. This molecular engineering achieves rapid and stable lithium storage through three-dimensional cross-flow ion transport dominated by pseudocapacitance. At a current density of 18 A/g, a high-power-densed (~42 kW/kg) organic cathode reaches ~76% state-of-charge in 44 seconds while showing ~79% capacity retention over 5,000 cycles at high rates. Its superior rate capability and cycling stability maintain even at low temperatures. We finally demonstrate its practical applicability with a lithium-metal pouch cell with high active material mass loading, highlighting the potential of fast-charging and stable cycling organic batteries.