Spinel LiNi_0.5Mn_1.5O₄ (LNMO) is a competitive cathode material for the next generation high energy density lithium ion batteries (LIBs) because of its high potential (4.7 V) and acceptable theoretical capacity (146.7 mAh g⁻¹). Nevertheless, it suffers from severe capacity decay during cycling, especially at elevated temperatures. Herein, we propose an integrated modification strategy combing Li⁺-conductive Li₂ZrO₃ coating layer with superficial Zr-doping. The coating layer of Li₂ZrO₃ avoids the direct contact between the cathode material and electrolyte, and favors Li⁺ transport kinetics and interface stability, superficial Zr-doping can greatly improve electron conductivity by inducing an appropriate amount of Mn³⁺. Electrochemical measurements demonstrate that desirable capacity retention of 82.4% can be obtained for 2 wt% Li₂ZrO₃-surface modified LNMO at 25 °C for 5 C rate after 1000 cycles, significantly higher than that of 66.1% for the pristine sample. Notably, the capacity retention of 2 wt% Li₂ZrO₃-coated LNMO sample can maintain up to 83.5% at 1 C rate after 200 cycles at 55 °C. This integrated modification strategy of synergistic coating and doping is regarded as a promising and useful choice for elevating the performance of LIBs.

尖晶石型LiNi _0.5 Mn _1.5 O ₄（LNMO）具有高电势（4.7 V）和可接受的理论容量（146.7 mAh g ^-1），是下一代高能量密度锂离子电池（LIB）的竞争性正极材料。然而，它在循环期间遭受严重的容量衰减，特别是在高温下。本文中，我们提出了一种整合改性策略，将Li ^+-导电Li ₂ ZrO ₃涂层与表面Zr掺杂相结合。Li ₂ ZrO ₃的涂层避免了正极材料和电解质之间的直接接触，并有利于Li ⁺由于传输动力学和界面稳定性，表面Zr掺杂可以通过诱导适量的Mn ³⁺来极大地提高电子电导率。电化学测量表明，经过1000次循环后，在25°C下以5 C的速率在2°C的Li ₂ ZrO _3-表面改性的LNMO可以达到82.4％的理想容量保持率，明显高于原始样品的66.1％。值得注意的是，在55°C下200个循环后，以1 C的速率涂覆2 wt％Li ₂ ZrO ₃的LNMO样品的容量保持率可以保持高达83.5％。这种协同涂覆和掺杂的集成修饰策略被认为是提高LIB性能的有希望和有用的选择。