Air‐Stable High‐Nickel Cathode with Reinforced Electrochemical Performance Enabled by Convertible Amorphous Li 2 CO 3 Modification

High-nickel (Ni≥90%) cathodes with high specific capacity hold great potential for next-generation lithium-ion batteries (LIBs). However, their practical application is restricted by the high interfacial reactivity under continuous air erosion and electrolyte assaults. Herein, a stable high-nickel cathode was rationally designed via in-situ induction of a dense amorphous Li2CO3 on the particle surface by a preemptive atmosphere control. Among the residual lithium compounds, Li2CO3 is the most thermodynamically stable one so that the dense Li2CO3 coating layer can serve as a physical protection layer to isolate the cathodes from contact with moist air. Furthermore, amorphous Li2CO3 can be transformed into a robust F-rich cathode electrolyte interphase (CEI) during cycling, which reinforces the cathodes interfacial stability and improves electrochemical performance. The assembled coin cell with this modified cathode delivers a high discharge capacity of 232.4 mAh g–1 with a superior initial coulombic efficiency of 95.1%, and a considerable capacity retention of 90.4% after 100 cycles. Furthermore, no slurry gelation occurred during large-scale electrode fabrication process. This work opens a valuable perspective on the evolution of amorphous Li2CO3 in LIBs and provides guidance on protecting unstable high-capacity cathodes for energy storage devices. This article is protected by copyright. All rights reserved