Rechargeable aqueous zinc-ion batteries (AZIBs) using polymer cathode materials generally exhibit excellent cycling stability due to the stable structure of polymer. However, their further development is curbed by relatively low capacity. Herein, we report a graphene/aza-fused π-conjugated microporous polymer composite (G-Aza-CMP) cathode with ultrahigh theoretical capacity (602 mAh g⁻¹) for AZIBs. The introduction of graphene makes the Aza-CMP expose more active sites to coordinate with H⁺/Zn²⁺, even boosts the storage of H⁺ to obtain faster kinetics, and endows the G-Aza-CMP//Zn battery with a redox pseudocapacitance mechanism. Thus, AZIBs using the G-Aza-CMP as cathode exhibit an extraordinary specific capacity of 456 mAh g⁻¹ at 0.05 A g⁻¹, and an outstanding cycling stability with 91.2% capacity retention after 9700 cycles at 10 A g⁻¹. This study provides a new insight into the charge storage mechanism and design of high-capacity polymer cathode materials for AZIBs.

由于聚合物的稳定结构，使用聚合物正极材料的可充电水系锌离子电池（AZIBs）通常表现出优异的循环稳定性。然而，它们的进一步发展受到相对较低的产能的限制。在此，我们报道了一种石墨烯/氮杂融合的 π-共轭微孔聚合物复合材料 (G-Aza-CMP) 正极，具有超高理论容量 (602 mAh g ^-1 ) 用于 AZIBs。石墨烯的引入使Aza-CMP暴露出更多的活性位点与H ⁺ /Zn ²⁺配位，甚至促进了H ⁺的储存以获得更快的动力学，并赋予了G-Aza-CMP//Zn电池的氧化还原能力赝电容机制。因此，使用 G-Aza-CMP 作为阴极的 AZIBs 表现出 456 mAh g 的非凡比容量^-1在 0.05 A g ^{-1下，以及在 10 A g -1}下 9700 次循环后具有出色的循环稳定性和 91.2% 的容量保持率。该研究为AZIBs高容量聚合物正极材料的电荷存储机制和设计提供了新的见解。