Novel Lamellar Tetrapotassium Pyromellitic Organic for Robust High‐Capacity Potassium Storage

Redox‐active organics are investigation hotspots for metal ion storage due to their structural diversity and redox reversibility. However, they are plagued by limited storage capacity, sluggish ion diffusion kinetics, and weak structural stability, especially for K+ ion storage. Herein, we firstly reported the lamellar tetrapotassium pyromellitic (K4PM) with four active sites and large interlayer distance for K+ ion storage based on a design strategy, where organics are constructed with the small molecular mass, multiple active sites, fast ion diffusion channels, and rigid conjugated π bonds. The K4PM electrode delivers a high capacity up to 292 mAh g−1 at 50 mA g−1, among the best reported organics for K+ ion storage. Especially, it achieves an excellent rate capacity and long‐term cycling stability with a capacity retention of ≈83 % after 1000 cycles. Incorporating in situ and ex‐situ techniques, the K+ ion storage mechanism is revealed, where conjugated carboxyls are reversibly rearranged into enolates to stably store K+ ions. This work sheds light on the rational design and optimization of organic electrodes for efficient metal ion storage. The lamellar tetrapotassium pyromellitic (K4PM) for a K‐organic battery delivers a high capacity and excellent cycling robustness due to its four K+ ion storage sites and large layer distance with reversible rearrangement of conjugated carboxyls into enolates.