High-voltage electrochemical performance of LiNi0.5Co0.2Mn0.3O2 cathode materials via Al concentration gradient modification

Abstract Al2O3-modified LiNi0.5Co0.2Mn0.3O2 cathode material is successfully synthesized via a facile carboxymethyl cellulose (CMC)-assisted wet method followed by a high-temperature calcination process. Al concentration gradient doping and accompanying formation of Al-coating are simultaneously accomplished in the modified samples. XRD and EDS analysis demonstrate that Al element is successfully doped into the crystal lattice with concentration gradient distribution inside the particles, reducing the Li/Ni cation mixing and stabilizing the layered structure. The compact distribution of Al on the surface forms a protective layer between the electrodes and the electrolyte, prohibiting the harmful side reactions and phase transition on the interphase. Compared with the pristine, the modified material with 2000 ppm Al2O3 (Al-2000) shows the best high-voltage performance with the capacity retention increased by ~13.3% from 138.3 to 163.0 mAh g−1 at 1 C in 3.0–4.6 V after 100 cycles. Even under the high current rate of 8 C (1240 mAh g−1) after 200 cycles, the Al-2000 still exhibits a capacity retention of 88.6%, greater than 80.3% for the pristine. Furthermore, results from the cyclic voltammetry (CV) and the electrochemical impedance spectroscopy (EIS) measurements confirm the roles of the Al2O3 modification in decreasing polarization and electrochemical resistances, contributing to the kinetic process of electrodes.