Polymeric Diaminophenazine with Spiral Architecture as Cathode Materials for Ultra‐Stable Aqueous Zinc‐Organic Batteries

Abstract Pyrazine‐based organic electrode materials hold great promise for applications in aqueous zinc‐ion batteries (AZIBs), while developing cost‐effective organic molecules that exhibit both high electrochemical activity and long cycle life remains challenging. Herein, we report an organic polymer (p‐DAP) featuring alternating rigid‐flexible spiral structures for AZIBs. Synthesized from cost‐effective o‐phenylenediamine via thermal polymerization, p‐DAP integrates saturated alicyclic rings and pyrazine moieties to stabilize interlayer spacing and facilitate ion transport. The polymer achieves nearly 95% redox‐active sites utilization at 0.2 A g −1 , delivering 145.2 mAh g −1 at 10 A g −1 with a capacity retention of 78.9% over 136 900 cycles. Notably, it maintains a capacity retention of 97.7% after 3550 cycles at –40 °C. Experimental and theoretical studies reveal a proton‐dominated charge storage mechanism. This work offers a promising strategy for designing durable organic electrodes for high‐performance AZIBs.