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Novel Composition of Co-Free LiNi0.875-xMn0.125AlxO₂ Cathode Materials.

Ni-rich LiNi1-xMnxO₂ cathode materials have attracted widespread interest as promising alternative cathode materials owing to their higher capacity, lower cost, and lower toxicity compared to those of LiCoO₂. Therefore, we designed herein a LiNi0.875Mn0.125O₂ positive electrode material. However, as the Ni content increases, the materials suffer from an extensive phase transition during the de-lithiation process owing to the low-bond strength of Ni (391.6 kJ mol-1) and Mn (402 kJ mol-1). In this study, Al-doped LiNi0.875-xMn0.125AlxO₂ (x= 0, 0.05, 0.1) was synthesized using the coprecipitation method. Al had a higher bond strength (512 kJ mol-1) between oxygen and metal ions compared to that of Ni and Mn ions. Additionally, Al is usually stabilized in the form of Al3+. Therefore, the increased bond strength decreased the electrostatic repulsion with oxygen during the de-lithiation process and prevented cation mixing by stabilizing the Ni ion's valence, thereby resulting in increased structural stability. X-ray diffraction (XRD) was used to characterize their structures and calculate the cation mixing value. The electrochemical properties showed that LiNi0.775Mn0.125Al0.1O₂ exhibited the high capacity retention of 97.1% after 30 cycles at 1 C at 55 °C.