In situ Interweaved Binder Framework Mitigating the Structural and Interphasial Degradations of High‐nickel Cathodes in Lithium‐ion Batteries

Abstract The practical viability of high‐nickel layered oxide cathodes is compromised by the interphasial and structural degradations. Herein, we demonstrate that by applying an in situ interweaved binder, the cycling stability of high‐nickel cathodes can be significantly improved. Specifically, the results show that the resilient binder network immobilizes the transition‐metal ions, suppresses electrolyte oxidative decomposition, and mitigates cathode particles pulverization, thus resulting in suppressed cathode‐to‐anode chemical crossover and ameliorated chemistry and architecture of electrode‐electrolyte interphases. Pouch full cells with high‐mass‐loading LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathodes achieve 0.02 % capacity decay per cycle at 1 C rate over 1 000 deep cycles at 4.4 V (vs. graphite). This work demonstrates a rational structural and compositional design strategy of polymer binders to mitigate the structural and interphasial degradations of high‐Ni cathodes in lithium‐ion batteries.