The application range of nickel-rich layered oxide cathodes is seriously hampered by the structural collapse, cycling decay and self-discharge issues under extreme temperature conditions. In this study, the real-time phase evolution of the LiNi_0.8Mn_0.1Co_0.1O₂ (NMC-811) cathode is investigated at the idling charged state and upon the high temperature galvanostatic cycling. Correspondingly, a quaternary system, consisting of LiNi_0.79Mn_0.1Co_0.1Al_0.01O₂ (NMCA), with the primary particles encapsulated by the glassy LiBO₂ network is proposed; the multiscale strategy collectively suppresses the performance deterioration at the static and dynamic processes, such as the unfavorable phasic transition from the layered to rock-salt structure and the microcrack evolution. When pairing this modified NMCA cathode at high loading mass (>450 g m⁻² for double side deposition) with the Si/C composite anode in the standard 18,650 cylinder-type cells, the prototype realizes the simultaneous robust capacity retention (~ 85% for 1000 cycles at 0.5 C), practical energy density of ~ 245.8 Wh kg⁻¹, effective mitigation of the self-discharge process at the elevated temperatures as well as 92% capacity retention even upon the operation at -20 °C. The scalability of our proposed modification strategy enables the feasible practical use of NMCA cathode within a broader temperature range.

在极端温度条件下，结构崩溃，循环衰变和自放电问题严重阻碍了富镍层状氧化物阴极的应用范围。在这项研究中，研究了LiNi _0.8 Mn _0.1 Co _0.1 O ₂（NMC-811）阴极在空载状态和高温恒电流循环时的实时相演化。相应地，由LiNi _0.79 Mn _0.1 Co _0.1 Al _0.01 O ₂（NMCA）组成的四元体系，其初级粒子被玻璃状LiBO ₂封装提议网络；多尺度策略共同抑制了静态和动态过程中的性能下降，例如从层状结构到岩盐结构的不利相变以及微裂纹的演化。当将这种改良的NMCA高负载质量阴极（双面沉积> 450 gm ^-2）与标准18,650圆柱型电池中的Si / C复合阳极配对时，该原型实现了同时强大的容量保持率（对于约85％在0.5 C下进行1000次循环），实际能量密度为〜245.8 Wh kg ^-1，即使在-20°C的操作环境下，也能有效缓解高温下的自放电过程以及92％的容量保持率。我们提出的修改策略的可扩展性使NMCA阴极在更宽的温度范围内可行地实际使用。