Integrating surface structure via triphenyl phosphate treatment to stabilize Li-rich Mn-based cathode materials

Li-rich Mn-based layered oxides (LLOs) have emerged as one of the most promising cathode materials for the next-generation lithium-ion batteries (LIBs) because of their high energy density, high specific capacity, and environmental friendliness. These materials, however, have drawbacks such as capacity degradation, low initial coulombic efficiency (ICE), voltage decay, and poor rate performance due to irreversible oxygen release and structural deterioration during cycling. Herein, we present a facile method of triphenyl phosphate (TPP) surface treatment to create an integrated surface structure on LLOs that includes oxygen vacancies, Li₃PO₄, and carbon. When used for LIBs, the treated LLOs show an increased initial coulombic efficiency (ICE) of 83.6% and capacity retention of 84.2% at 1C after 200 cycles. It is suggested that the enhanced performance of the treated LLOs can be attributed to the synergetic functions of each component in the integrated surface, such as the oxygen vacancy and Li₃PO₄ being able to inhibit the evolution of oxygen and accelerate the transport of lithium ions, while the carbon layer can restrain undesirable interfacial side reactions and reduce the dissolution of transition metals. Furthermore, electrochemical impedance spectroscopy (EIS) and galvanostatic intermittent titration technique (GITT) prove an enhanced kinetic property of the treated LLOs cathode, and ex-situ X-ray diffractometer shows a suppressed structural transformation of TPP-treated LLOs during the battery reaction. This study provides an effective strategy for constructing an integrated surface structure on LLOs to achieve high-energy cathode materials in LIBs.