Elucidating the Structure-Performance Relationship in Single-Particle NCM Cathodes via Controlled Precursor Synthesis

Abstract

While high-energy-density Ni-rich layered oxides, LiNi1-x-yCoxMnyO2 (Ni > 0.8), are of significant attention as nextgeneration cathode materials, their practical application is limited by intergranular cracking and mechanical degradation arising from anisotropic lattice strain. The single-particle cathode strategy has emerged as a promising solution, effectively suppressing intergranular cracking by eliminating boundaries between primary particles. However, the fundamental relationships between single-particle size, internal microstructure, and electrochemical performance remain poorly understood. Here, we present a molten-salt synthesis strategy to produce LiNi0.92Co0.03Mn0.05O2 single-particle cathodes with tunable particle and crystallite sizes via precursor morphology control. Systematic analysis reveals clear correlations between precursor shape, final particle microstructure, and rate capability. This work aims to establish the causal link between precursor morphology, final particle microstructure, and electrochemical performance, thereby providing a core design principle for developing high-stability and -power single-particle cathode materials.