Nickel‐rich layered oxides have developed into appealing cathode materials for lithium‐ion batteries in recent years for the sake of high energy density and low cost, but they suffer from severe capacity deterioration during long‐term cycling. Herein, Mn‐doped nickel‐rich Li(Ni_0.88Co_0.09Al_0.03)_1‐δMn_δO₂ (δ=0, 0.01, 0.02) cathode materials with a nanoscale Ni_xMn_1−xO‐type pillar layer are synthesized using a facile high‐shear dry mixing and high‐temperature calcination process in this study. The as‐fabricated M0.01−NCA electrode with a Ni_xMn_1−xO‐type layer about 20 nm exhibits excellent cycle performance compared with the pristine in coin‐cells and in pouch cells (the long‐term cycle number is four times that of the pristine). Detailed investigation of the fading mechanism is performed by HRTEM, ex‐situ XRD, XPS et al. The enhanced performance is directly related to the synergetic effects of bulk inactive Mn⁴⁺ doping and the increased nanoscale Ni_xMn_1−xO‐type pillar layer. The Mn dopants stabilize the lattice structure thus decreasing the microcracks, and the pillar layer protects the cathode from parasitic reactions with electrolytes during long‐term cycling. This work gives a new insight into the role of Mn doping on the enhanced structure of nickel‐rich layered oxides.

中文翻译：

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锰掺杂对富镍层状氧化物的本体结构稳定性和界面稳定性的作用的新见解

近年来，出于高能量密度和低成本的考虑，富镍层状氧化物已成为锂离子电池有吸引力的阴极材料，但它们在长期循环过程中会严重恶化容量。这里，Mn掺杂镍-丰富了Li（Ni _0.88钴_0.09的Al _0.03）_1-δ的Mn _δ Ô ₂（δ= 0，0.01，0.02）与纳米级的Ni的正极材料_X的Mn _1-x O形型柱层是本研究中使用方便的高剪切干混和高温煅烧工艺合成。带有Ni _x Mn _1-x的M0.01-NCA电极与原始电池相比，在纽扣电池和袋式电池中，约20 nm的O型层具有出色的循环性能（长期循环次数是原始电池的四倍）。衰落机理的详细研究是由HRTEM，异位XRD，XPS等进行的。增强的性能直接与块状惰性Mn ⁴⁺掺杂的协同效应和增加的纳米级Ni _x Mn _1-x O型柱层的协同作用有关。Mn掺杂剂可稳定晶格结构，从而减少微裂纹，柱层可保护阴极免受长期循环过程中与电解质的寄生反应的影响。这项工作为锰掺杂在富镍层状氧化物增强结构中的作用提供了新的见解。