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

Abstract Lithium (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 V 2 CT x /MoO 3 (DG‐V 2 CT x /MoO 3 ) 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 V 2 CT x endows a good ionic conductive gradient; while, MoO 3 is regarded as a spacer to avoid the restacking of V 2 CT x , 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 V 2 CT x and MoO 3 guide the homogeneous Li growth. As a result, the symmetrical half‐cells based on DG‐V 2 CT x /MoO 3 @Li anodes conduct 700 h at 5 mAh cm −2 and 20 mA cm −2 . The DG‐V 2 CT x /MoO 3 @Li||LiFePO 4 full‐cells maintain a capacity retention of 85.4% after 1350 cycles at 2 C. Remarkably, the DG‐V 2 CT x /MoO 3 @Li||LiNi 0.6 Co 0.2 Mn 0.2 O 2 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.