Direct Synthesis of Single‐Crystalline LiNi 0.8 Co 0.1 Mn 0.1 O 2 Cathodes From Lithium‐Containing Precursors via Spray Pyrolysis

Single‐crystalline cathode materials have attracted considerable attention for addressing the cycling instability of Ni‐rich layered cathode materials caused by anisotropic lattice strain during repeated cycling. However, conventional synthesis methods for single‐crystalline cathodes generally require high temperatures and prolonged calcination times. Alternative approaches, such as multistep lithiation, molten‐salt, and hydrothermal methods, still suffer from limitations such as complex processes, mandatory washing, and challenges in large‐scale production. Therefore, in this study, a direct synthesis strategy for single‐crystalline LiNi 0.8 Co 0.1 Mn 0.1 O 2 (SC‐NCM) cathode materials was proposed using Li‐containing precursors prepared by spray pyrolysis. Because lithium was homogeneously incorporated within the precursor particles, SC‐NCM was successfully synthesized through direct calcination without additional Li‐mixing or washing processes. As a result, single‐crystalline NCM was successfully crystallized at 900 °C for 3 h with 700 °C for 6 h healing sequence and exhibited superior cycling performance compared with polycrystalline NCM (PC‐NCM), delivering a capacity retention of 81% after 1000 cycles at 0.5 C. Therefore, this work provides an effective approach to simultaneously address both the intrinsic limitations of Ni‐rich layered cathode materials and the challenges associated with conventional synthesis processes.