Regulation of Dipolar‐Dipolar and Ion‐Dipolar Interactions Simultaneously in Strong Solvating Electrolytes for All‐Temperature Zinc‐Ion Batteries

Abstract Aqueous zinc‐ion batteries (AZIBs) attract attention due to their safety and high specific capacity. However, their practical applications are constrained by Zn anode corrosion, dendritic growth, and poor temperature adaptability induced by a strong hydrogen‐bond network in aqueous electrolytes. Herein, a universal strategy to design strong solvating electrolytes is proposed, in which the hydrogen‐bond network and solvation structures are reconstructed by regulating the dipolar‐dipolar and ion‐dipolar interactions simultaneously. Consequently, the hydrogen‐bond network in free water is largely weakened, and the water content in the Zn²⁺ solvated sheath is reduced, while the hydrogen‐bond network between solvents is strengthened, which effectively broadens the operating temperature range and suppresses Zn dendrites and corrosion. As a result, Zn anodes exhibit excellent platting/stripping efficiency with an average Coulombic Efficiency up to 99.89% after 2000 cycles at 0.5 mA cm⁻², impressive cycling stability (5000 h, 0.5 mA cm⁻²/0.5 mA h cm⁻²), and a wide operating temperature range of 140 °C (−50–90 °C). Moreover, the Zn//V₂O₃ full cells also display enhanced temperature‐resistance, implying that the designed strong solvation electrolyte has practical application potential in extreme environments. This study suggests a promising strategy to design ideal electrolytes for high‐performance AZIBs with safety, ultralong cycling life, and satisfying temperature‐resistance.