Structurally integrated asymmetric polymer electrolyte with stable Janus interface properties for high-voltage lithium metal batteries

Solid-state polymer electrolytes are outstanding candidates for next-generation lithium metal batteries in the realm of high specific energy densities, high safeties and tight contact with electrodes. However, their applications are still hindered by the limitations that no single polymer is electrochemically stable with the oxidizing high-voltage cathode and the highly reductive Li anode, simultaneously. Herein, a bilayer asymmetric polymer electrolyte (SL-SPE) without accessional interface resistance that using poly (ethylene glycol) diacrylate (PEGDA) as a “bridge” to connect the sulfonyl (OS = O)-contained oxidation-tolerated layer and polyether-derived reduction-tolerated layer (SPE), is proposed and synthesized by sequential two-step UV polymerizations. SL-SPE can provide widened electrochemical stability window up to 5 V, while simultaneously deploying a stable Janus interface property. Eventually, the superior high-voltage (4.4 V) cycling durability can be displayed in LiNi0.6Co0.2Mn0.2O2|SL-SPE|Li batteries. This finding provides a bran-new idea for designing multifunctional polymer electrolytes in the application of solid-state batteries.