Zwitterionic ionic liquids (ZIL) contain covalently bound cationic and anionic moieties with potential electrochemical applications. In this study, we construct a self-adaptive electric double layer (EDL) on the interfaces of...

Aqueous zinc ion batteries (ZIBs) have been extensively investigated as a next‐generation energy storage system due to their high safety and low cost. However, the critical issues of irregular dendrite growth and intricate side reactions severely restrict the further industrialization of ZIBs. Here, a strategy to fabricate a semi‐immobilized ionic liquid interface layer is proposed to protect the Zn anode over a wide temperature range from −35 to 60 °C. The immobilized SiO2@cation can form high conjugate racks that can regulate the Zn2+ concentration gradient and self‐polarizing electric field to guarantee uniform nucleation and planar deposition; the free anions of the ILs can weaken the hydrogen bonds of the water to promote rapid Zn2+ desolvation and accelerate ion‐transport kinetics simultaneously. Because of these unique advantages, the cycling performance of the symmetric Zn batteries is greatly enhanced, evidenced by a cycling life of 1800 h at 20 mA cm−2, and a cycle lifespan of 2000 h under a wide temperature window from −35 to 60 °C. The efficiency of this semi‐immobilizing strategy is well demonstrated in various full cells including pouch cells, showing high performance at large current (20 A g−1) and wide temperatures with extra‐long cycles up to 80 000 cycles.

Rechargeable aqueous zinc‐ion batteries are of great potential as one of the next‐generation energy‐storage devices due to their low cost and high safety. However, the development of long‐term stable electrodes and electrolytes still suffers from great challenges. Herein, a self‐separation strategy is developed for an interface layer design to optimize both electrodes and electrolytes simultaneously. Specifically, the coating with an organometallics (sodium tricyanomethanide) evolves into an electrically responsive shield layer composed of nitrogen, carbon‐enriched polymer network, and sodium ions, which not only modulates the zinc‐ion migration pathways to inhibit interface side reactions but also adsorbs onto Zn perturbations to induce planar zinc deposition. Additionally, the separated ions from the coating can diffuse to the electrolyte to affect the Zn2+ solvation structure and maintain the cathode structural stability by forming a stable cathode–electrolyte interface and sodium ions’ equilibrium, confirmed by in situ spectroscopy and electrochemical analysis. Due to these unique advantages, the symmetric zinc batteries exhibit an extralong cycling lifespan of 3000 h and rate performance at 20 mA cm−2 at wide temperatures. The efficiency of the self‐separation strategy is further demonstrated in practical full batteries with an ultralong lifespan over 10 000 cycles from −35 to 60 °C.

Aqueous Zinc (Zn) metal batteries have received widespread attention due to their high safety and environmental friendliness. However, the uncontrollable growth of dendrites, hydrogen evolution reaction, and corrosion severely limit...

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