Thermal‐Induced Loose Solute Configuration Activates Organic Electrolyte for Zinc Metal Battery

ABSTRACT Zinc metal batteries face issues of low coulombic efficiency and persistent side reactions due to the active H 2 O in aqueous electrolytes. Organic electrolytes that can reduce side reactions and coulombic efficiency loss still suffer from sluggish Zn 2+ transfer and difficult desolvation. We propose a thermal‐induced loose solute configuration to activate rapid Zn 2+ transfer in “Zn(OTf) 2 + ACN” pure organic electrolyte. Zn metal batteries with the pure organic electrolyte realize stable and long‐term cycling for over 5500 h at 5 mA cm −2 and 10 mAh cm −2 . Moreover, a practical parameter of cumulative capacity reaches 7.5 Ah cm −2 at DOD > 90%. As an application demonstration, the pouch cells assembled with our organic electrolyte can be photo‐charged by illumination and drive LEDs or other portable electronics in daily life. The organic electrolyte activated by thermal‐induced loose solute configuration demonstrates long‐cycle lifespan and application potential, offering a new choice for electrolytes in Zn metal batteries.