Realizing a Wide‐Temperature Aluminum‐Foil‐Anode‐Based Lithium‐Ion Battery

Abstract Aluminum (Al) foil is regarded as a promising anode for lithium‐ion batteries (LIBs) owing to its high theoretical capacity, low lithiation/delithiation potential, and natural abundance. However, Al‐foil‐based LIBs are currently confined to operate at room temperature, owing to the deterioration of solid electrolyte interphase (SEI) at high/low temperatures, which ultimately renders Al anode unable to endure significant volumetric changes during alloying/de‐alloying under extreme temperatures. Herein, wide temperature (WT) cyclability of Al‐based LIBs are realized for the first time by designing an Al‐phobic SEI. A thin, robust Al‐phobic LiF‐rich SEI layer with high mechanical strength (1.08 GPa) is in situ constructed in all‐fluorinated electrolyte featured with anion‐dominated solvation structure. This Al‐phobic interphase, which bonds weakly with the Al anode, is capable of accommodating volume expansion, mitigating the electrode pulverization, and reducing dead Li x Al. Consequently, the Li||Al half‐cells exhibit a high Coulombic efficiency of 99.6% at 25 °C and maintain operational stability over the temperature range of −20–60 °C. The Al||LiNi 0.8 Mn 0.1 Co 0.1 O 2 full cells deliver considerable capacities of 165.4 mAh g −1 at −20 °C and 223.2 mAh g −1 at 60 °C (based on cathode). This work represents a critical step of Al‐based LIBs for WT applications.