High-Performance Layered Ni-Rich Cathode Materials Enabled by Stress-Resistant Nanosheets

Layered O3-type transition metal oxides are promising cathode candidates for high-energy-density Li-ion batteries. However, the structural instability at the highly delithiated state and low kinetics at the fully lithiated state are arduous challenges to overcome. Here, a facile approach is developed to make secondary particles of Ni-rich materials with nanosheet primary grains. Because the alignment of the primary grains reduces internal stress buildup within the particle during charge-discharge and provides straightforward paths for Li transport, the as-synthesized Ni-rich materials do not undergo cracking upon cycling with higher overall Li⁺ ion diffusion rates. Specifically, a LiNi_0.75Co_0.14Mn_0.11O₂ cathode with nanosheet grains delivers a high reversible capacity of 206 mAh g^-1 and shows ultrahigh cycling stability, e.g., 98% capacity retention over 500 cycles in a full cell with a graphite anode. © 2023 American Chemical Society.