For the sustainable development of Li[Ni_xCo_yMn_1−x−y]O₂ and Li[Ni_xCo_yAl_1−x−y]O₂ cathodes, reducing the reliance on cobalt, which is extremely expensive with a fluctuating price and supply uncertainty, is considered essential. In this study, we propose a highly stable Co-free Ni-rich layered cathode developed through a new doping strategy that incorporates heteroelements at different doping stages, including the introduction of Ti during Ni(OH)₂ synthesis and doping excess amounts of Al during the lithiation step. The multi-stage engineering strategy guarantees structural durability and electrochemical cycling stability of the inherently unstable LNO to a commercially viable level. Combined with particle surface protection, the Li[Ni_0.951Ti_0.008Al_0.041]O₂ cathode retains 72.0% of its initial capacity after 3500 cycles, which is unprecedented among previously reported Co-free cathodes. The proposed Co-free cathodes can meet the energy density required for next-generation electric vehicles, as the cathode delivers 890 Wh kg_cathode^-1, and presents a clear breakthrough for the development of commercially viable LNO cathode.

为了Li[Ni _x Co _y Mn _{1− x − y} 和 Li[Ni _x Co _y Al _{1− x −} ]O ₂ 阴极，减少对钴的依赖被认为是至关重要的，因为钴的价格极其昂贵，而且价格波动且供应不确定。在这项研究中，我们提出了一种通过新的掺杂策略开发的高度稳定的无钴富镍层状阴极，该策略在不同的掺杂阶段结合了异质元素，包括在Ni(OH) ₂ 合成过程中引入Ti以及在锂化步骤中掺杂过量的Al。多阶段工程策略保证了本质不稳定的 LNO 的结构耐久性和电化学循环稳定性达到商业可行的水平。结合颗粒表面保护，Li[Ni _0.951 Ti _0.008 Al _0.041 ]O ₂ 正极保留了初始容量的 72.0% 3500 次循环后，这在之前报道的无钴正极中是前所未有的。所提出的无钴正极可满足下一代电动汽车所需的能量密度，因为该正极可提供 890 Wh kg _cathode ^-1 ，并为商业上可行的 LNO 阴极。