Influence of Ni/Mn distributions on the structure and electrochemical properties of Ni-rich cathode materials

To reveal the influence of element distribution on the structure and electrochemical performances of Ni-rich layered cathode materials, LiNiCoMnO (NCM) with four types of Ni/Mn distributions (homogeneous, core-shell, multi-shell and concentration-gradient structures) is designed and synthesized with a combination of co-precipitation and high-temperature solid-state method. Ni/Mn distributions of the as-prepared NCM cathode materials are investigated with focused ion beam (FIB) and energy disperse X-ray spectrum (EDS) line scanning on the cross-section of single particles, which illustrate that NCM materials with the desired Ni/Mn distributions are successfully prepared. For the three spherical heterogeneous NCM materials, the center is the Ni-rich component while the surface is the Mn-rich component. Ni/Mn distributions between the center and surface components are in different forms. Studies imply that the heterogeneous samples exhibit smaller cation disordering, lower charge transfer resistance, higher Li diffusion coefficient and higher structural stability than the homogeneous one. Therefore, the heterogeneous samples, especially the multi-shell and concentration-gradient ones, display improved cycling and thermal stability compared to the homogeneous one. These results manifest that multi-shell and concentration-gradient structures are effective strategies to modify the layered NCM cathode materials for Li-ion batteries.