Mitigating Dissolution and Kinetics Limitations in Aqueous Zinc‐Organic Batteries via a Conjugated Scaffold Integrated With Stable Nitroxyl Radicals

Aqueous zinc‐ion batteries employing organic cathodes hold promise for grid‐scale energy storage, yet they are frequently hindered by active material dissolution and slow reaction kinetics. Herein, we report a bipolar organic cathode, HATN‐T, designed by integrating stable nitroxyl radicals into a conjugated hexaazatrinaphthylene (HATN) scaffold. This claw‐shaped molecular design features multiple redox‐active centers (C═O, C═N, and N–O•) to facilitate reversible multi‐ion (Zn ²⁺ , H ⁺ , and ClO ₄ ⁻ ) storage. As a cathode, HATN‐T delivers a high specific capacity (316 mAh g ⁻¹ at 0.1 A g ⁻¹ ), exceptional rate performance (260 mAh g ⁻¹ at 10 A g ⁻¹ ), and robust cycling stability (79% retention after 5000 cycles). Mechanistic studies reveal that the charge storage is dominated by capacitance, originating from the synergistic redox activity of the integrated functional groups. Notably, the reversible formation of a zinc hydroxychloride byproduct acts as a chemical buffer, confirming a proton‐coupled mechanism that underpins the electrode’s exceptional reversibility. This work establishes a generalizable design strategy for merging stable radicals with conjugated scaffolds to create high‐performance organic electrodes for sustainable energy storage.