Electroactive Chelating Groups Enable High‐Performance Aqueous Zinc‐Organic Batteries

Abstract P‐type organic electrode materials, characterized by fast kinetics and high redox potential, hold great promise for aqueous zinc‐ion batteries (ZIBs), but suffer from low capacity and limited cycling stability in practical applications. Herein, we demonstrate that the introduction of electroactive chelating groups can significantly improve both the capacity and cycling stability of p‐type triphenylamine derivative‐based electrodes. The electroactive chelating groups promote a higher proportion of electroactive sites within the cathode material. The combined in/ex situ spectroscopic analysis and theoretical investigations show that electroactive chelating groups facilitate the formation of stable zinc‐supramolecular network, which effectively mitigates the dissolution of electrode materials and the decomposition of the aqueous electrolyte during cycling. The as‐synthesized poly(1,4‐naphthoquinone‐1,3,5‐tri(4‐aminophenyl)benzene) exhibits a high reversible capacity of 311 mAh g −1 at 50 mA g −1 and superior rate performance (199 mAh g −1 at 10 A g −1 ) in aqueous electrolyte. Moreover, it demonstrates excellent stability, retaining 83% to 96% of its capacity over 5000 cycles in various aqueous electrolytes, representing a new record for p‐type and bipolar‐type organic electrode materials. This work provides valuable insights into the design of organic electrode materials for high‐performance ZIBs.