The recharging capability of Ni-rich layered cathodes deteriorates rapidly upon cycling, mainly from mechanical instability caused by removing a large amount of Li ions from the host structure. Through multi-stage microstructural tailoring, which refers to optimal engineering of the precursor microstructure and then deliberately over-doping of Al during the lithiation stage to preserve the needle-like morphology of the precursor, we optimize the primary particle morphology of the cathode. It is demonstrated that the chemical and microstructural engineering of a Li[Ni_0.9–xCo_0.1Al_x]O₂ cathode starting from its precursor stage produces a unique structure that relieves the detrimental mechanical strain and significantly extends the battery life. Excess Al-doped Li[Ni_0.86Co_0.1Al_0.04]O₂ with the compositional partitioning of Ni produces a highly aligned microstructure in which constituent primary particles are refined to a sub-micrometer scale. Thus, the designed Li[Ni_0.86Co_0.1Al_0.04]O₂ retains 86.5% of the initial capacity after 2000 cycles and an unprecedented 78.0% even at a severe operation condition of 45 °C. The proposed Li[Ni_0.86Co_0.1Al_0.04]O₂ represents a new class of Ni-rich Li[Ni_xCo_yAl_1–x–y]O₂ cathodes that can meet the energy density required for next-generation electric vehicles, without compromising the battery life and safety.

中文翻译：

---

高性能富镍 Li[Ni0.9–xCo0.1Alx]O2 正极通过从氢氧化物前驱体到锂化氧化物的多阶段微结构定制

富镍层状正极的充电能力在循环后迅速恶化，主要是由于从主体结构中去除大量锂离子引起的机械不稳定性。通过多阶段微结构剪裁，即对前驱体微观结构进行优化设计，然后在锂化阶段故意过度掺杂 Al 以保持前驱体的针状形态，我们优化了正极的初级粒子形态。证明了 Li[Ni _{0.9– x} Co _0.1 Al _x ]O ₂的化学和微结构工程阴极从其前体阶段开始产生独特的结构，可减轻有害的机械应变并显着延长电池寿命。过量 Al 掺杂的 Li[Ni _0.86 Co _0.1 Al _0.04 ]O ₂与 Ni 的成分分配产生高度排列的微观结构，其中构成的初级粒子被细化到亚微米级。因此，所设计的 Li[Ni _0.86 Co _0.1 Al _0.04 ]O ₂在 2000 次循环后仍保持初始容量的 86.5%，即使在 45°C 的严酷运行条件下也能保持前所未有的 78.0%。建议的 Li[Ni _0.86 Co _0.1 Al _0.04]O ₂代表了一类新的富镍锂[Ni _x Co _y Al _{1– x – y} ]O ₂正极，可以满足下一代电动汽车所需的能量密度，同时不影响电池寿命和安全性。