Abstract

Rechargeable lithium-oxygen (Li-O2) batteries (LOBs) with extremely high theoretical energy density have been regarded as a promising next-generation energy storage technology. However, the limited cycle life, undesirable corrosion, and safety hazards are seriously limiting the practical application of the lithium metal anode in LOBs. Here, we demonstrate a rational design of the Li-Al alloy (LiAlx) anode that successfully achieves ultralong cycling life of LOBs with stable Li cycling. Through in situ high-current pretreatment technology, Al atoms accumulates, and a stable Al2O3-containing solid electrolyte interphase protective film formed on the LiAlx anode surface to suppress side reactions and O2 crossover. The cycling life of LOB with the protected LiAlx anode increases to 667 cycles under a fixed capacity of 1000 mA h g-1, as compared to 17 cycles without pretreatment. We believe that this in situ high-current pretreatment strategy presents a new vision to protect the lithium-containing alloy anodes, such as Li-Al, Li-Mg, Li-Sn, and Li-In alloys for stable and safe lithium metal batteries (Li-O2 and Li-S batteries).

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