Dual‐Active‐Center Covalent Organic Frameworks Engineered for H/Zn Cointercalation and Mn Mediation in Aqueous Zinc‐Ion Batteries

With the development of clean energy systems, more efforts have been put into aqueous zinc‐ion batteries (AZIBs), originating from its high safety and low cost. However, cathode materials still face challenges such as low capacity, poor cycling stability, and a lack of active sites at high potentials. This study proposes a covalent organic framework material (TABQ‐TFP‐COF) containing dual active sites, which has been successfully applied for AZIBs. It exhibits excellent structural stability, low solubility, and rapid ion transport capabilities. With an electrolyte system containing Mn 2+ additives, TABQ‐TFP‐COF cathode demonstrates a high specific capacity of 264 mAh g −1 (at 0.1 A g −1 ) and a capacity retention rate close to 100% in 1500 cycles (at 1 A g −1 ), along with outstanding rate performance. Through systematic characterization methods, including in situ FTIR, ex situ XRD, and XPS, combined with theoretical calculations, the reversible co‐intercalation mechanism of H + /Zn 2+ at CO/CN sites is revealed. Additionally, pouch cells assembled based on this material maintain stable voltage output under various mechanical deformation conditions. This study offers design strategies for high‐performance AZIBs and provides mechanistic insights into multi‐ion energy storage.