Manganese and Cobalt-Free Ultrahigh-Ni-Rich Single-Crystal Cathode for High-Performance Lithium Batteries

Current commercial nickel (Ni)-rich Mn, Co, and Al-containing cathodes are employed in high-energy-density lithium (Li) batteries all around the globe. The presence of Mn/Co in them brings out several problems, such as high toxicity, high cost, severe transition-metal dissolution, and quick surface degradation. Herein, a Mn/Co-free ultrahigh-Ni-rich single-crystal LiNi0.94Fe0.05Cu0.01O2 (SCNFCu) cathode with acceptable electrochemical performance is benchmarked against a Mn/Co-containing cathode. Despite having a slightly lower discharge capacity, the SCNFCu cathode retaining 77% of its capacity across 600 deep cycles in full-cell outperforms comparable to a high-Ni single-crystal LiNi0.9Mn0.05Co0.05O2 (SCNMC; 66%) cathode. It is shown that the stabilizing ions Fe/Cu in the SCNFCu cathode reduce structural disintegration, undesirable side reactions with the electrolyte, transition-metal dissolution, and active Li loss. This discovery provides a new extent for cathode material development for next-generation high-energy, Mn/Co-free Li batteries due to the compositional tuning flexibility and quick scalability of SCNFCu, which is comparable to the SCNMC cathode.