Dual-type gel polymer electrolyte for high-voltage lithium metal batteries with excellent cycle life

The most attractive approach for maximizing the energy density of rechargeable lithium batteries is to combine a lithium metal anode with a high-voltage cathode. However, the dendritic formation of lithium at the anode and the highly oxidizing conditions that cause electrolyte decomposition at the cathode have hindered the practical development of lithium metal batteries (LMBs). In this study, we report a dual-type gel polymer electrolyte (GPE) composed of an anolyte and a catholyte that can address the drawbacks of both the anode and cathode sides. The anolyte is a poly(ethylene oxide)-based composite solid polymer electrolyte that is chemically stable with lithium metal and has a high mechanical strength for suppressing lithium dendrite growth. A cross-linked gel polymer electrolyte with high lithium-ion conductivity and oxidative stability was used as the catholyte. The Li/LiCoO2 cell assembled with a dual-type GPE exhibited a high discharge capacity of 181.1 mAh g−1 (areal capacity: 3.15 mAh cm−2) in the voltage range of 3.0–4.5 V and excellent cycle life, with a capacity retention of 74 % after 700 cycles at 25 °C and 0.5 C rate. Our study proposes a promising electrolyte system for LMBs with high energy density and good cycle life.