Scalable Interfacial Engineering with Lithiophilic‐Lithiophobic Layers for High‐Performance All‐Solid‐State Li‐Metal Batteries
Pengfei Ren, Nicholas S. Grundish, Sidong Zhang, Lihai Zhou, Ruiping Liu, Nan Wu, Yutao Li
Abstract
Abstract The stability of the lithium‐metal/solid electrolyte interface remains a critical challenge in the development of all‐solid‐state lithium‐metal batteries (ASSLMBs), as it directly influences their cycling performance, rate capability, and safety. Here, a thin, flexible, and lithium‐stable sulfide electrolyte membrane is presented with high ionic conductivity (3.25 × 10 −3 S cm −1 ) and low electronic conductivity (1.45 × 10 −9 S cm −1 ) at room temperature, prepared with an AlCl 3 coating in a low‐cost wet process. The in situ formation of a lithiophilic Li‐Al alloy and a lithiophobic LiCl layer at the interface creates a stable dual‐layer structure, effectively suppressing Li‐dendrite growth and enhancing Li‐transport across the interface. Symmetric Li/Li cells with this coated membrane exhibit exceptional cycling stability, operating for over 10000 h at 0.5 mA cm −2 . ASSLMBs assembled with a LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode and a metallic lithium anode exhibit excellent cycling performance, highlighting the potential of this coating strategy to stabilize the Li/solid electrolyte interface and expedite the commercialization of ASSLBs.