Kinetically controlled synthesis of low-strain disordered micro–nano high voltage spinel cathodes with exposed {111} facets

Abstract

High-voltage LiNi_0.5Mn_1.5O₄ (LNMO) is one of the most promising cathode candidates for rechargeable lithium-ion batteries (LIBs) but suffers from deteriorated cycling stability due to severe interfacial side reactions and manganese dissolution. Herein, a micro–nano porous spherical LNMO cathode was designed for high-performance LIBs. The disordered structure and the preferred exposure of the {111} facets can be controlled by the release of lattice oxygen in the high-temperature calcination process. The unique configuration of this material could enhance the structural stability and play a crucial role in inhibiting manganese dissolution, promoting the rapid transport of Li⁺, and reducing the volume strain during the charge/discharge process. The designed cathode exhibits a remarkable discharge capacity of 136.7 mA h g⁻¹ at 0.5C, corresponding to an energy density of up to 636.4 W h kg⁻¹, unprecedented cycling stability (capacity retention of 90.6% after 500 cycles) and superior rate capability (78.9% of initial capacity at 10C). The structurally controllable preparation strategy demonstrated in this work provides new insights into the structural design of cathode materials for LIBs.