Abstract

Ni-rich layered transition metal oxides have been regarded as the most feasible way for achieving high energy density of lithium-ion batteries. Conventional Ni-rich cathodes are composed of spherical secondary particles, consisting of numerous primary particles. Unfortunately, the grain boundaries in the polycrystalline structure are vulnerable to the pulverization, leading to microcracks during cycling. The newly exposed surface from the microcrack can induce undesirable side reactions with the electrolyte, which severely deteriorates the battery performance. On the other hand, single-crystalline Ni-rich cathodes have gained significant attention for industrial applications due to their robust mechanical strength, resulting from the elimination of grain boundaries. The improved mechanical properties of single-crystalline cathodes effectively mitigate the interfacial side reactions, thereby attaining superior structural, thermal, and electrochemical performance. Herein, we have introduced various synthetic methods of the single-crystalline cathode, encompassing not only high-temperature sintering and the molten-salt method for the Ni-rich cathode but also the other strategies for different single-crystalline cathode materials. This review aims to provide a comprehensive understanding of single-crystalline cathode synthesis, with implications for the development of high-performance cathode materials.

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