Carbon-coated Ni0.5Mg0.5Fe1.7Mn0.3O4 nanoparticles as a novel anode material for high energy density lithium-ion batteries

Phys Chem Chem Phys. 2024 Feb 28;26(9):7492-7503. doi: 10.1039/d4cp00182f.

Abstract

Lithium-ion batteries (LIBs) have gained considerable attention from the scientific community due to their outstanding properties, such as high energy density, low self-discharge, and environmental sustainability. Among the prominent candidates for anode materials in next-generation LIBs are the spinel ferrites, represented by the MFe2O4 series, which offer exceptional theoretical capacities, excellent reversibility, cost-effectiveness, and eco-friendliness. In the scope of this study, Ni0.5Mg0.5Fe1.7Mn0.3O4 nanoparticles were synthesized using a sol-gel synthesis method and subsequently coated with a carbon layer to further enhance their electrochemical performance. TEM images confirmed the presence of the carbon coating layer on the Ni0.5Mg0.5Fe1.7Mn0.3O4/C composite. The analysis of the measured X-ray diffraction (XRD) and Raman spectroscopy results confirmed the formation of nanocrystalline Ni0.5Mg0.5Fe1.7Mn0.3O4 before coating and amorphous carbon in the Ni0.5Mg0.5Fe1.7Mn0.3O4/C after the coating. The Ni0.5Mg0.5Fe1.7Mn0.3O4 anode material exhibited a much higher specific capacity than the traditional graphite material, with initial discharge/charge capacities of 1275 and 874 mA h g-1, respectively, at a 100 mA g-1 current density and a first coulombic efficiency of 68.54%. The long-term cycling test showed a slight capacity fading, retaining approximately 85% of its initial capacity after 75 cycles. Notably, the carbon-coating layer greatly enhanced the stability and slightly increased the capacity of the as-prepared Ni0.5Mg0.5Fe1.7Mn0.3O4. The first discharge/charge capacities of Ni0.5Mg0.5Fe1.7Mn0.3O4/C at 100 mA g-1 current density reached 1032 and 723 mA h g-1, respectively, and a first coulombic efficiency of 70.06%, with an increase of discharge/charge capacities to 826.6 and 806.2 mA h g-1, respectively, after 75 cycles (with a capacity retention of 89.7%), and a high-rate capability of 372 mA h g-1 at 2C. Additionally, a full cell was designed using a Ni0.5Mg0.5Fe1.7Mn0.3O4/C anode and an NMC811 cathode. The output voltage was about 2.8 V, with a high initial specific capacity of 755 mA h g-1 at 0.125C, a high rate-capability of 448 mA h g-1 at 2C, and a high-capacity retention of 91% after 30 cycles at 2C. The carbon coating layer on Ni0.5Mg0.5Fe1.7Mn0.3O4 nanoparticles played a crucial role in the excellent electrochemical performance, providing conducting, buffering, and protective effects.