G.R. Wang, Z.H. Bi, A.P. Zhang, P. Das, H. Lin, Z.-S. Wu*

Engineering, 2023, Accepted.

Lithium-ion batteries (LIBs) with double-high characteristics of high energy density and high power density are urgently demanded for facilitating the development of advanced portable electronics. However, the Li+ storage performance of the most commercialized lithium cobalt oxide (LCO, LiCoO2) cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for double-high target. Herein, we systematically summarized and discussed the high-voltage and fast-charging LCO from key fundamental challenges, latest advancement in modification strategies to future perspectives in depth. The comprehensive and elaborated discussions on key fundamental challenges are firstly presented from the view point of structural degradation, interfacial instability, inhomogeneity reaction, and sluggish interfacial kinetics. The deep insights into the promising modification strategies and underlined mechanism are further instructively overviewed, which are categorized into elements doping (Li-sites, Co/O-sites, and multiple-sites doping) for improved Li+ diffusivity and bulk-structure stability, surface coating (dielectrics, ionic/electronic conductors, and their combination) for surface stability and conductivity, nanosizing, their combination, and other strategies (optimization of electrolyte, binder, tortuosity of electrodes, charging protocols, prelithiation methods). Finally, the forward-looking perspectives and promising directions are sketched out and elucidated insightfully, providing constructive suggestions and instructions on designing and realizing high-voltage and fast-charging LCO for next-generation double-high LIBs.