Lithiophilic V2CTx/MoO3 Hosts with Electronic/Ionic Dual Conductive Gradients for Ultrahigh‐Rate Lithium Metal Anodes

Abstract

AbstractLithium (Li) metal is considered as a promising anode material for high‐energy batteries; yet, its practical application is hindered by uncontrolled Li dendrite growth, especially at a high rate. Herein, a dual conductive gradient V2CTx/MoO3 (DG‐V2CTx/MoO3) host that integrates electronic/ionic conductive gradients and lithiophilicity is prepared by layer‐by‐layer assembly for dendrite‐free Li anodes. Gradient LiF deriving from different amount of V2CTx endows a good ionic conductive gradient; while, MoO3 is regarded as a spacer to avoid the restacking of V2CTx, increasing space for Li deposition. The dual conductive gradients effectively optimize the current density and Li+ flux distribution at the bottom, achieving fast reduction of Li+ and a “bottom–up” Li deposition mode. Meanwhile, the lithiophilic V2CTx and MoO3 guide the homogeneous Li growth. As a result, the symmetrical half‐cells based on DG‐V2CTx/MoO3@Li anodes conduct 700 h at 5 mAh cm−2 and 20 mA cm−2. The DG‐V2CTx/MoO3@Li||LiFePO4 full‐cells maintain a capacity retention of 85.4% after 1350 cycles at 2 C. Remarkably, the DG‐V2CTx/MoO3@Li||LiNi0.6Co0.2Mn0.2O2 full‐cells can run 150 cycles with 80.6% capacity retention even at harsh conditions. The well‐adjusted materials and structures with both dual conductive gradients and lithiophilic properties will bring inspiration for novel material design of other metal batteries.