Abstract
Ni-rich layered LiNi1-x-y Cox Mny O2 systems are the most promising cathode materials for high energy density Li-ion batteries (LIBs). However, Ni-rich cathode materials inevitably suffer from rapid capacity fading and poor rate capability owing to structural instability and unstable surface side reactions. Zr doping has proven to be an effective method to enhance the cycle and rate performances by stabilizing the structure and increasing the Li+ diffusion rate. Herein, effects of Zr-doping on the structural stability and Li+ diffusion kinetics are thoroughly investigated in LiNi0.6 Co0.2 Mn0.2 O2 (LNCM) cathode material using atomic-resolution scanning transmission electron microscopy imaging, XRD Rietveld refinement, and density functional theory calculations. Zr doping mitigates the degree of cation mixing, decreases the structural transformation, and facilitates Li+ diffusion resulting in improved cyclic performance and rate capability. Based on the obtained results, an atomistic model is proposed to explain the effects of Zr doping on the structural stability and Li+ diffusion kinetics in LNCM cathode materials.
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