Single‐Crystalline Cathodes for Advanced Li‐Ion Batteries: Progress and Challenges

Abstract Single‐crystalline cathodes are the most promising candidates for high‐energy‐density lithium‐ion batteries (LIBs). Compared to their polycrystalline counterparts, single‐crystalline cathodes have advantages over liquid‐electrolyte‐based LIBs in terms of cycle life, structural stability, thermal stability, safety, and storage but also have a potential application in solid‐state LIBs. In this review, the development history and recent progress of single‐crystalline cathodes are reviewed, focusing on properties, synthesis, challenges, solutions, and characterization. Synthesis of single‐crystalline cathodes usually involves preparing precursors and subsequent calcination, which are summarized in the details. In the following sections, the development issues of single‐crystalline cathodes, including kinetic limitations, interfacial side reactions, safety issues, reversible planar gliding and micro‐cracking, and particle size distribution and agglomeration, are systematically analyzed, followed by current solutions and characterization techniques. Finally, this review is concluded with proposed research thrusts for the future development of single‐crystalline cathodes.