A Self-Reconfigured, Dual-Layered Artificial Interphase Towards High-Current-Density Quasi-Solid-State Lithium Metal Batteries.

The uncontrollable dendrite growth and unstable solid electrolyte interphase have long plagued the practical application of Li metal batteries. Herein, we demonstrate a dual-layered artificial interphase LiF/LiBO-Ag that is simultaneously reconfigured via an electrochemical process to stabilize the lithium anode. This dual-layered interphase consists of a heterogeneous LiF/LiBO glassy top layer with ultrafast Li-ion conductivity and lithiophilic Li-Ag alloy bottom layer, which synergistically regulates the dendrite-free Li deposition, even at high current densities. As a result, Li||Li symmetric cells with LiF/LiBO-Ag interphase achieve an ultralong lifespan (4500 h) at an ultrahigh current density and area capacity (20 mA cm -2 , 20 mAh cm -2 ). LiF/LiBO-Ag@Li anodes were successfully applied in quasi-solid-state batteries, showing excellent cycling performances in symmetric cells (8 mA cm -2 , 8 mAh cm -2 , 5000 h) and full cells. Furthermore, a practical quasi-solid-state pouch cell coupling with a high-nickel cathode exhibits a stable cycling with a capacity retention of over 91% after 60 cycles at 0.5 C, which is comparable or even better than that in liquid-state pouch cells. Additionally, a high-energy-density quasi-solid-state pouch cell (10.75 Ah, 448.7 Wh kg -1 ) were successfully accomplished. This well-orchestrated interphase design provides new guidance in engineering highly stable interphase towards practical high-energy-density lithium metal batteries. This article is protected by copyright. All rights reserved.