Rechargeable Lithium Metal Batteries with an In‐Built Solid‐State Polymer Electrolyte and a High Voltage/Loading Ni‐Rich Layered Cathode

Abstract

Solid-state batteries enabled by solid-state polymer electrolytes (SPEs) are under active consideration for their promise as cost-effective platforms that simultaneously support high-energy and safe electrochemical energy storage. The limited oxidative stability and poor interfacial charge transport in conventional polymer electrolytes are well known, but difficult challenges must be addressed if high-voltage intercalating cathodes are to be used in such batteries. Here, ether-based electrolytes are in situ polymerized by a ring-opening reaction in the presence of aluminum fluoride (AlF₃ ) to create SPEs inside LiNi_0.6 Co_0.2 Mn_0.2 O₂ (NCM) || Li batteries that are able to overcome both challenges. AlF₃ plays a dual role as a Lewis acid catalyst and for the building of fluoridized cathode-electrolyte interphases, protecting both the electrolyte and aluminum current collector from degradation reactions. The solid-state NCM || Li metal batteries exhibit enhanced specific capacity of 153 mAh g^-1 under high areal capacity of 3.0 mAh cm^-2 . This work offers an important pathway toward solid-state polymer electrolytes for high-voltage solid-state batteries.