Electrochemically Inert Li2MnO3: The Key to Improving the Cycling Stability of Li-Rich Manganese Oxide Used in Lithium-Ion Batteries.

Lithium-rich manganese oxide is a promising candidate for the next-generation cathode material of lithium-ion batteries because of its low cost and high specific capacity. Herein, a series of xLi2MnO3·(1 - x)LiMnO2 nanocomposites were designed via an ingenious one-step dynamic hydrothermal route. A high concentration of alkaline solution, intense hydrothermal conditions, and stirring were used to obtain nanoparticles with a large surface area and uniform dispersity. The experimental results demonstrate that 0.072Li2MnO3·0.928LiMnO2 nanoparticles exhibit a desirable electrochemical performance and deliver a high capacity of 196.4 mAh g-1 at 0.1 C. This capacity was maintained at 190.5 mAh g-1 with a retention rate of 97.0% by the 50th cycle, which demonstrates the excellent cycling stability. Furthermore, XRD characterization of the cycled electrode indicates that the Li2MnO3 phase of the composite is inert, even under a high potential (4.8 V), which is in contrast with most previous reports of lithium-rich materials. The inertness of Li2MnO3 is attributed to its high crystallinity and few structural defects, which make it difficult to activate. Hence, the final products demonstrate a favorable electrochemical performance with appropriate proportions of two phases in the composite, as high contents of inert Li2MnO3 lower the capacity, while a sufficient structural stability cannot be achieved with low contents. The findings indicate that controlling the composition through a dynamic hydrothermal route is an effective strategy for developing a Mn-based cathode material for lithium-ion batteries.

Facile One-Step Dynamic Hydrothermal Synthesis of Spinel LiMn2O4/Carbon Nanotubes Composite as Cathode Material for Lithium-Ion Batteries.

Nano-sized spinel LiMn2O4/carbon nanotubes (LMO/CNTs) composite is facilely synthesized via a one-step dynamic hydrothermal approach. The characterizations and electrochemical measurements reveal that LiMn2O4 particles with narrow size distribution are well dispersed with CNTs in the composite. The LMO/CNTs nanocomposite with 5 wt % CNTs displays a high specific discharge capacity of 114 mAh g-1 at 1C rate, and the retention rate after 180 cycles at room temperature reaches 94.5% in the potential window of 3.3 to 4.3 V vs. Li/Li+. Furthermore, the electrochemical performance of the composite with 5 wt % CNTs at elevated temperature (55 °C) is also impressive, 90% discharging capacity could be maintained after 100 cycles at 1C. Such excellent electrochemical performance of the final product is attributed to the content of CNTs added in the hydrothermal process and small particle size inherited from pretreated MnO2 precursor.