Enhanced Electrochemical Performance of the LiNi_0.5Mn_1.5O₄ Cathode Material by the Construction of Uniform Lithium...

In order to alleviate the rapid capacity decay caused by the instability of the crystal structure and electrode/electrolyte interface, a series of Li₂SiO₃-coated LiNi_0.5Mn_1.5O₄ materials have been prepared via the lithium acetate-assisted sol-gel method followed by a short-term calcination process. During the sol-gel process, TEOS is hydrolyzed, condensed, and polymerized with the assistance of lithium acetate to form a Li⁺-embedded [Si-O-Si] network structure to ensure the uniformity of the coating. By changing the amount of TEOS and lithium acetate, the coating thickness can be precisely controlled, whose effects on the structural and electrochemical properties of LiNi_0.5Mn_1.5O₄ materials are intensively investigated. The results show that the material with an appropriate thickness of Li₂SiO₃ coating exhibits a larger primary particle size and reduced secondary particle agglomeration. The uniform Li₂SiO₃ coating with appropriate thickness can not only improve Li⁺ ion diffusion kinetics but also suppress side reactions and CEI growth at the electrode/electrolyte interface. Besides, the interaction of Li₂SiO₃ with HF can alleviate electrode corrosion and the dissolution of transition metal ions. All the abovementioned factors together promote the significant improvement of the electrochemical performance of Li₂SiO₃-coated LiNi_0.5Mn_1.5O₄ materials.