Unlocking the Potential of Li‐Rich Mn‐Based Oxides for High‐Rate Rechargeable Lithium‐Ion Batteries

Lithium‐rich Mn‐based oxides have gained significant attention worldwide as potential cathode materials for the next generation of high‐energy density lithium‐ion batteries. Nonetheless, the inferior rate capability and voltage decay issues present formidable challenges. Here, a Li‐rich material equipped with quasi‐three‐dimensional (quasi‐3D) Li‐ion diffusion channels is initially synthesized by introducing twin structures with high Li‐ion diffusion coefficients into the crystal and constructing a “bridge” between different Li‐ion diffusion tunnels. The as‐prepared material exhibits monodispersed micron‐sized primary particles (MP), delivering a specific capacity of 303 mAh g−1 at 0.1 C and an impressive capacity of 253 mAh g−1 at 1 C. More importantly, the twin structure also serves as a “breakwater” to inhibit the migration of Mn ions and improve the overall structural stability, leading to cycling stability with 85% capacity retention at 1 C after 200 cycles. The proposed strategy of constructing quasi‐3D channels in the layered Li‐rich cathodes will open up new avenues for the research and development of other layered oxide cathodes, with potential applications in industry. Li‐rich Mn‐based layered oxides, featuring quasi‐three‐dimensional (quasi‐3D) Li‐ion diffusion channels attained through the introduction of twin structures into the crystal framework, exhibit notably elevated Li‐ion diffusion coefficients, leading to impressive rate performance. Additionally, the twin structure serves as a protective barrier, impeding the migration of Mn ions and enhancing the overall structural stability.