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The evolution of modern society demands sustainable rechargeable lithium-ion batteries (LIBs) with higher capacity and improved safety standards. High voltage Ni-rich layered transition metal oxides (i.e., LiNi1-x-yCoxMnyO2, NCM) have emerged as one of the most promising cathode materials in meeting this demand. However, the instability of Ni-rich NCMs cathodes presents challenges in large-scale commercialization. This review examines the energy storage mechanism, e.g., possible (electro)chemical reactions, occurring at the bulk and surface and degradation mechanism of the Ni-rich NCMs cathode materials. To address the challenging instability issue, we highlight recent advances and strategies for bulk and surface engineering of Ni-rich NCMs, including lattice, composition, and microstructure engineering, and electrolyte and materials interfacial engineering. By addressing degradation mechanisms and improving overall stability, this work sheds lights on the potential avenues on the commercialization of Ni-rich cathode-based high-performance LIBs.
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