Highly‐Dispersed Submicrometer Single‐Crystal Nickel‐Rich Layered Cathode: Spray Synthesis and Accelerated Lithium‐Ion Transport

For conventional polycrystalline Ni-rich cathode material consisting of numerous primary particles in disordered orientation, the crystal anisotropy in charge/discharge process results in the poor rate capability and rapid capacity degradation. In this work, highly-dispersed submicron single-crystal LiNi_0.8 Co_0.15 Al_0.05 O₂ (SC-NCA) cathode is efficiently prepared by spray pyrolysis (SP) technique followed by a simple solid-state lithiation reaction. Porous Ni_0.8 Co_0.15 Al_0.05 O_x precursor prepared via SP exhibits high chemical activity for lithiation reaction, enabling the fabrication of single-crystal cathode at a relatively low temperature. In this way, the contradiction between high crystallinity and cation disordering is well balanced. The resulted optimized SC-NCA shows polyhedral single-crystal morphology with moderate grain size (≈1 μm), which are beneficial to shortening the Li⁺ diffusion path and improving the structural stability. As cathode for lithium ion batteries, SC-NCA delivers a high discharge capacity of 202 and 140 mAh g^-1 at 0.1 and 10 C, respectively, and maintains superior capacity retention of 161 mAh g^-1 after 200 cycles at 1C. No micro-crack is observed in the cycled SC-NCA particles, indicating such single-crystal morphology can greatly relieve the anisotropic micro-strain. This effective, continuous and adaptable strategy for preparing single-crystal Ni-rich cathode without any additive may accelerate their practical application.