Constructing an Interlaced Catalytic Surface via Fluorine‐Doped Bimetallic Oxides for Oxygen Electrode Processes in Li–O₂ Batteries

Abstract Lithium–oxygen (Li–O₂) batteries, renowned for their high theoretical energy density, have garnered significant interest as prime candidates for future electric device development. However, their actual capacity is often unsatisfactory due to the passivation of active sites by solid‐phase discharge products. Optimizing the growth and storage of these products is a crucial step in advancing Li–O₂ batteries. Here, a fluorine‐doped bimetallic cobalt‐nickel oxide (CoNiO_2–xF_x/CC) with an interlaced catalytic surface (ICS) and a corncob‐like structure is proposed as an oxygen electrode. Unlike conventional oxide electrodes with a “single adsorption catalytic mechanism,” the ICS of CoNiO_2−xF_x/CC offers a “competitive adsorption catalytic mechanism,” where oxygen sites facilitate oxygen conversion while fluorine sites contribute to the growth of Li₂O₂. This results in a change in Li₂O₂ morphology from a surface film to toroidal particles, effectively preventing the burial of active sites. Additionally, the unique open architecture aids in the capture and release of oxygen and the formation of well‐contacted Li₂O₂/electrode interfaces, which benefits the complete decomposition of Li₂O₂ products. Consequently, the Li–O₂ battery with a CoNiO_2−xF_x/CC cathode demonstrates a high specific capacity of up to 30923 mAh g⁻¹ and a lifespan exceeding 580 cycles, surpassing most reported metal oxide‐based cathodes.