ABSTRACT High‐nickel layered oxides are considered key cathode materials for high‐energy‐density lithium‐ion batteries due to their high specific capacity. However, the spin state localization of Ni 3+ (t 2g 6 e g 1 ) leads to severe Jahn–Teller distortion and structural degradation, limiting their cycling stability. This study proposes a high‐entropy transition metal (TM) regulation strategy, which introduces multicomponent vacant orbital TM ions (Mn, Ti, Nb, Ta, W, and Mo) to construct a Ni─OO─TM electronic resonance network, promoting the delocalization of Ni 3+ e g electrons, thereby suppressing spin disorder and enhancing structural stability. On the basis of this, a high‐entropy high‐nickel cathode material (HE‐LNF, LiNi 0.8 Fe 0.14 Mn 0.01 Ti 0.01 Nb 0.01 Ta 0.01 W 0.01 Mo 0.01 O 2 ) was designed. Combining first‐principles calculations with experimental characterization, the weakening effect of electronic resonance on magnetic frustration was revealed: This effect increases the phase transition temperature to 294.23°C by reducing the amplitude of lattice vibrations, while electronic delocalization reduces local nuclear repulsion, maintaining excellent structural stability with minimal lattice strain evolution after cycling. Electrochemical testing shows that HE‐LNF maintains a capacity retention rate of 91% after 100 cycles at a 0.33‐C rate, significantly outperforming traditional high‐nickel materials. This study provides new insights into the design of high‐stability high‐nickel cathodes based on electronic structure regulation.
Li et al. (Thu,) studied this question.