In Situ Lithiated Anti-Perovskite Nitride-Mediated Li-Ion Redistribution Enabling Fast-Charging Graphite Anodes.

Abstract

The transport of Li⁺ within thick graphite electrodes has been deemed to be a key factor affecting the fast-charging performance of lithium-ion batteries (LIBs). However, how to effectively enhance the kinetics of this process while regulating the Li plating behavior remains a challenge in the current research on graphite anodes. Herein, we propose a mediated ion redistribution strategy based on in situ lithiated antiperovskite nitride (LiCo₃ZnN), tailored to suppress Li dendrite growth and enhance fast-charging performance of LIBs. By integrating density functional theory (DFT) calculations, finite element analysis (FEA) simulations, and in situ spectroscopic techniques, we demonstrate that LiCo₃ZnN not only facilitates rapid Li⁺ transport within the electrode through its adsorption effect but also acts as a lithiophilic mediator to convert irreversible "dead Li" into reversible "active Li". Consequently, the modified anode (Co₃ZnN@Gr) exhibits an outstanding comprehensive performance. Specifically, it achieves a capacity retention of 88.64% after 400 cycles at 4C in Co₃ZnN@Gr||NCM622 cells with a high cathode loading of 20 mg cm^-2. Notably, in pouch cells, it maintains 85.82% capacity retention after 1000 cycles at 4C. This work holds significant promise for advancing fast-charging LIBs, thereby paving the way for the widespread adoption of electric vehicles (EVs).