High-voltage LiNi0.5Mn1.5O4 cathodes for Li-ion batteries obtained by sol–gel combustion method: effects of fuel-type and silver doping

Abstract

High-voltage LiNi_0.5Mn_1.5O₄ (LNMO) cathode materials are highly desirable for the fabrication of next-generation lithium-ion batteries (LIBs). In this study, citric acid, glycine, and sucrose fuels were used to optimize the structural and electrochemical properties of LNMO materials obtained by sol–gel combustion synthesis (SCS). The experimental results showed that the type of fuel used in the SCS process influenced the enthalpy of combustion, crystallite size, morphology, cationic disorder and electrochemical properties of the LNMO materials. XRD results indicated that all the LNMO materials have a phase-pure spinel structure with the Fd3m space group. The glycine fuel composition produced LNMO material (LNMO-G) with the least crystallite size, less cationic disorder and the highest crystallinity compared with those having the citric acid fuel (LNMO-C) and sucrose fuel (LNMO-S) compositions. As a result, the LNMO-G cell delivered the highest first discharge capacity of 115.83 mA h g⁻¹ and retained 80.06% of its initial capacity after 200 cycles at a current density of 1C. Moreover, the LNMO-G cell had the best rate capability compared with the LNMO-C and LNMO-S cells, with a discharge capacity of 60 mA h g⁻¹ at a rate of 2C between 3.50 and 5.30 V. Furthermore, Ag doping (LNMAO) improved the rate capability and Li-ion kinetics of the LNMO-G cathode material. The LNMAO cathode achieved a reversible discharge capacity of 100 mA h g⁻¹ at a rate of 2C between 3.50 and 5.30 V. These findings show that LNMO cathode materials can be optimized for ultra-high-voltage (>5.0 V) performance in LIBs for advanced applications.