Spray-drying synthesis of fluorine-doped LiNi0.5Mn1.5O4 as high-voltage cathodes for lithium-ion batteries

Abstract

In this current work, the pristine LiNi0.5Mn1.5O4 (LNMO) and fluorine-doped LiNi0.5Mn1.5O4–xFx (x = 0.1; 0.2; 0.3) cathode materials were successfully synthesized through a facile spray-drying method. The performed morphological and structural characterizations revealed that the fluorine doping led to a partial conversion of Mn4+ to Mn3+ ions in LNMO structure and an increase of their average particle sizes. These characteristics made the LiNi0.5Mn1.5O3.9F0.1 cathode exhibited the best rate capability at high C-rates and cycling performance among all investigated LNMO-based electrodes. Its improved electrochemical properties resulted from excellent crystallinity, high Li+ diffusion coefficient, and low charge-transfer resistance. Moreover, the LiNi0.5Mn1.5O3.9F0.1 electrode was found to possess the excellent resistant against Mn dissolution at elevated temperature. According to its great thermal stability, an impressive capacity retention of 81.5% after 100-cycle at 0.2 C at elevated temperature was achieved. In terms of the facile synthesis approach, superior electrochemical performances, and great thermal stability, the LiNi0.5Mn1.5O3.9F0.1 electrode synthesized by the scalable spray-drying method can be regarded as a promising high-voltage cathode material for high-performance Li-ion batteries.