Mechanism Behind the Loss of Fast Charging Capability in Nickel‐Rich Cathode Materials

Abstract Fast charging technology for electric vehicles (EVs), offering rapid charging times similar to conventional vehicle refueling, holds promise but faces obstacles owing to kinetic issues within lithium‐ion batteries (LIBs). Specifically, the significance of cathode materials in fast charging has grown because Ni‐rich cathodes are employed to enhance the energy density of LIBs. Herein, the mechanism behind the loss of fast charging capability of Ni‐rich cathodes during extended cycling is investigated through a comparative analysis of Ni‐rich cathodes with different microstructures. The results revealed that microcracks and the resultant cathode deterioration significantly compromised the fast charging capability over extended cycling. When thick rocksalt impurity phases form throughout the particles owing to electrolyte infiltration via microcracks, the limited kinetics of Li + ions create electrochemically unreactive areas under high‐current conditions, resulting in the loss of fast charging capability. Hence, preventing microcrack formation by tailoring microstructures is essential to ensure stability in fast charging capability. Understanding the relationship between microcracks and the loss of fast charging capability is essential for developing Ni‐rich cathodes that facilitate stable fast charging upon extended cycling, thereby promoting widespread EV adoption.