Facile Synthesis of Modified Single-Crystal NCM811 Cathode Materials and the Electrochemical Performance for Lithium-Ion Batteries

To address the capacity decay of NCM811 caused by microcracks and cation disorder during cycling, La, Al, and F tri-doped micron-sized single-crystal NCM811 material with a LiNbO3 coating was synthesized via a facile co-solvent method. Using a mixed glucose–urea thermal solution as the reaction medium, metal salts were incorporated, followed by step-wise sintering, ball-milling, heat treatment, and wet-chemical coating. This approach enables atomic-level precursor mixing and ensures homogeneous element distribution. La3+ enlarges the lithium layer spacing to enhance ion diffusion and Al3+ suppresses Ni3+ reduction to Ni2+, mitigating cation mixing and improving conductivity, while F− stabilizes the crystal structure via its strong electronegativity. The LiNbO3 coating protects the interface from electrolyte attack, and the single-crystal morphology effectively suppresses microcracking. Compared to unmodified single-crystal NCM811 prepared identically, the modified material exhibits reduced cation disorder, improved crystallinity, and superior thermal stability. Electrochemical tests in half-cells with 1 M LiPF6/(EC/EMC/DMC) electrolyte (2.8–4.3 V) show an initial discharge capacity of 208.32 mAh/g at 0.1 C and 194.05 mAh/g at 1 C. After 200 cycles at 1 C, the capacity retention remains at 92.21%, exceeding the market average. Rate performance is also notably enhanced, with the 5 C discharge capacity increasing from 141.12 mAh/g (unmodified) to 166.81 mAh/g, demonstrating improved kinetics and structural stability.