Efficiently advancing lithium-ion batteries toward high energy density entails overcoming challenges in Li-rich layered oxides, including severe voltage and capacity fading, irreversible oxygen escape and compromised thermal robustness due to the uncontrollable oxygen anionic redox (OAR). Herein, a three-in-one modification strategy, aim at strengthening the reversibility of OAR and structural integrity of MnO6 octahedron, is rationally introduced on Li1.2Mn0.53Ni0.20Co0.07O2 cathode through a universal H3BO3-treatment. Through the introduction of oxygen vacancies and gradient B-doping, the energy level of unhybridized O 2p states is decreased to narrow the band energy gap with transition metal (TM) band, which triggers cationic/anionic hybrid redox at high voltage, thereby stabilizing the peroxo-like (O2)n- species and hindering irreversible oxygen escape, while the lithium borate nano-coating serves to mitigate side reactions, particularly during charging at elevated temperatures. As a result, the modulated cathode exhibits notable capacity retention of 96.3 % after 500 cycles at 1 C with limited voltage fading rate (1.73 mV per cycle) and even stable cyclic performance at high temperature (60 °C). This approach provides an effective and straightforward method to tackle the voltage decay and capacity fading of high-energy Li-rich layered cathode materials.

中文翻译：

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通过三合一策略触发阳离子/阴离子混合氧化还原稳定高温富锂正极材料

有效推进锂离子电池向高能量密度发展需要克服富锂层状氧化物的挑战，包括严重的电压和容量衰减、不可逆的氧气逃逸以及由于不可控的氧阴离子氧化还原（OAR）而导致的热稳定性受损。本文通过通用的 H3BO3 处理，在 Li1.2Mn0.53Ni0.20Co0.07O2 正极上合理引入了一种三合一改性策略，旨在增强 OAR 的可逆性和 MnO6 八面体的结构完整性。通过引入氧空位和梯度B掺杂，降低未杂化O 2p态的能级，缩小与过渡金属（TM）带的能带间隙，在高电压下触发阳离子/阴离子杂化氧化还原，从而稳定过氧类 (O2)n- 物质并阻碍不可逆的氧气逸出，而硼酸锂纳米涂层则用于减轻副反应，特别是在高温充电期间。结果，调制阴极在 1 C 下循环 500 次后表现出 96.3% 的显着容量保持率，电压衰减率有限（每个循环 1.73 mV），甚至在高温（60 °C）下具有稳定的循环性能。这种方法提供了一种有效且直接的方法来解决高能富锂层状正极材料的电压衰减和容量衰减问题。