Zn(TFSI)2-Mediated Ring-Opening Polymerization for Electrolyte Engineering Toward Stable Aqueous Zinc Metal Batteries

• A novel Zn(TFSI)2-mediated ring-opening polymerization strategy creates a pDOL-based electrolyte that significantly enhances the stability and reversibility of aqueous zinc metal batteries. • The pDOL electrolyte exhibits excellent antioxidant stability, non-flammability, a widened electrochemical window (2.6 V), and a low freezing point (−34.9 °C), enabling superior low-temperature performance. • The electrolyte effectively inhibits Zn dendrite growth and corrosion, leading to an ultra-long lifespan of 8200 h at 1 mAh cm−2 and 2500 h at 60% depth of discharge. • A Zn//VO2 pouch cell with lean electrolyte achieves 92% capacity retention after 600 cycles, demonstrating practical viability for high-energy-density energy storage.