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Abstract Ni‐rich layered cathode materials are progressively considered as the standard configuration of high‐energy electric vehicles by virtues of their high capacity and eliminated “range anxiety.” However, the poor cyclic stability and severe cobalt supply crisis would restrain their wide commercial applicability. Here, a cost‐effective single‐crystal Co‐free Ni‐rich cathode material LiNi 0.8 Mn 0.18 Fe 0.02 O 2 (NMF), which outperforms widely commercial polycrystalline LiNi 0.83 Co 0.11 Mn 0.06 O 2 (MNCM) and single‐crystal LiNi 0.83 Co 0.11 Mn 0.06 O 2 (SNCM) is reported. Surprisingly, NMF can compensate for the reversible capacity loss under the designed conditions of high‐temperature and elevated‐voltage, achieving a competitive energy density compared with conventional MNCM or SNCM. Combining operando characterizations and density functional theory calculation, it is revealed that NMF cathode with improved dynamic structure evolution largely alleviates the mechanical strain issue commonly found in Ni‐rich cathode, which can reduce the formation of intragranular cracks and improve the safety performance. Consequently, this new Co‐free NMF cathode can achieve a perfect equilibrium between material cost and electrochemical performance, which not only reduces the production cost by >15%, but also demonstrates excellent thermal stability and cycling performance..
Shen et al. (Wed,) studied this question.