Constructing Li-O-Vacancy Configuration Coupling with a Layered/Spinel Mixed Structure in Li-Deficient Li-Rich Layered Oxides to Realize Stable Oxygen Redox

Owing to the synergistic effect of cationic and anionic charge compensation, Li-rich layered oxide cathodes stand as the most promising candidates for next-generation high-energy-density Li-ion batteries. However, the unstable oxygen redox process triggers irreversible oxygen release and structural degradation of the layered framework, which further destabilizes the Li-O-Li configuration and leads to severe performance decay. In this work, a layered/spinel heterostructure coupled with a stabilized Li-O-vacancy configuration is successfully constructed in a Li-rich layered oxide cathode. This design enables outstanding structural and electrochemical stability, delivering an initial discharge capacity of 232 mAh g−1 with a Coulombic efficiency of 90.5%. Moreover, the cathode retains 86.5% of its capacity after 100 cycles. The proposed structural design strategy offers a new pathway toward high-performance Li-rich layered oxide cathodes.