Surface and Interface Issues in Spinel LiNi_0.5Mn_1.5O₄: Insights into a Potential Cathode Material for High Energy Density Lithium Ion Batteries

Abstract

Spinel LiNi0.5Mn1.5O4 with high operating voltage (∼4.7 V vs Li/Li+), high theoretical capacity of 148 mAh g–1, fast lithium ion diffusion kinetics, and potentially low cost is the most potential candidate material for high energy density LIBs used in plug-in hybrid electric vehicles and pure electric vehicles. However, the high operating voltage of LiNi0.5Mn1.5O4 challenges the electrochemical stability of other components in the batteries and induces diverse interfacial side reactions, leading to irreversible capacity loss, poor cycling performance, and safety issues, especially at the elevated temperatures. Thus, a basic understanding of the intrinsic surface properties of LiNi0.5Mn1.5O4 and the mechanism of interfacial interactions between each component in the electrochemical system is a critical requirement for developing substantial enhancements of LiNi0.5Mn1.5O4-based batteries. In this review, we summarize the surface/interface reactions and challenges in the whole cell system of LiNi0.5Mn1.5O4-based LIBs. Perspectives and strategies for LiNi0.5Mn1.5O4-based high energy density batteries used in PHEV/EVs are also proposed at last.

Prescribing Functional Additives for Treating the Poor Performances of High‐Voltage (5 V‐class) LiNi0.5Mn1.5O4/MCMB Li‐Ion Batteries

“…And the sudden capacity failure can be possibly ascribed to the loss of electrical contact between the electrodes and current collector foils, which is indicated by the lowest Coulombic efficiency (continuous severe parasitic reactions and accumulation of byproducts) upon cycling ( Figure S2b, Supporting Information). [7][8][9][10][11][12][13][14][15] Thus, the superior cyclability/Coulombic efficiency of the cell with BE + binary functional additives suggest that the combination of TMSP and PCS can produce synergistic effects to better suppress continuous active lithium consuming parasitic reactions (especially at MCMB anode) upon cycling. [55,56] As for the cell with BE + binary functional additives, the Coulombic efficiency is the highest in the first 50 cycles and remains relatively stable in the following cycles ( Figure 2b; Figure S2b, Supporting Information).…”

Research Progress in Improving the Cycling Stability of High-Voltage LiNi0.5Mn1.5O4 Cathode in Lithium-Ion Battery

“…The high-voltage LiNi 0.5 Mn 1.5 O 4 (LNMO) cathode is the most promising candidate among the 5 V cathode materials for LIBs due to its flat plateau at 4.7 V [13], large specific capacity (146.6 mAh g −1 ), and a two-electron process Ni 2+ /Ni 4+ , where the Mn 4+ ions remain electrochemically inactive [14, 15]. However, the degradation of cyclic performance is very serious when LNMO operates over 4.2 V. As a kind of HVLIB cathode material, LNMO was widely investigated and systematically reviewed.…”

The Effects of a Mixed Precipitant on the Morphology and Electrochemical Performance of LiNi0.5Mn1.5O4 Cathode Materials

“…As an excellent energy storage system, the lithium ion battery has increasingly aroused attention due to its high energy density, long cycle life, and environmental friendliness. However, there are still some problems, such as short capacity fading, high costs, and potential safety hazards during the course of practical application [1][2][3][4][5]. It has also been considered that the improvement of energy/power density of lithium ion batteries has been a significant theme, and the development of high performance cathode materials has been the main approach for resolving it [5].…”

“…However, there are still some problems, such as short capacity fading, high costs, and potential safety hazards during the course of practical application [1][2][3][4][5]. It has also been considered that the improvement of energy/power density of lithium ion batteries has been a significant theme, and the development of high performance cathode materials has been the main approach for resolving it [5]. As a promising cathode material for lithium ion batteries, spinel LiNi 0.5 Mn 1.5 O 4 (LNMO) has caused attracted an increasing amount of attention due to its high discharge plateau around 4.7 V, its low cost, and its high energy density (630 Wh kg −1 ) [6,7].…”