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

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.