Garnet Li₇La₃Zr₂O₁₂-Based Solid-State Lithium Batteries Achieved by In Situ Thermally Polymerized Gel Polymer Electrolyte

Garnet Li7La3Zr2O12 (LLZO) is a potential solid electrolyte for solid-state batteries (SSBs) because of its high ionic conductivity, electrochemical stability, and mechanical strength. However, large interface resistances arising from deserted cathodes and rigid garnet/electrode interfaces block its application. In order to deal with this issue, a gel polymer electrolyte (GPE) was introduced into the cathode and both sides of LLZO to achieve a solid-state battery. Especially, the provided GPE could be thermally polymerized and solidified in situ, which would integrate LLZO with both anode and cathode and dramatically simplify the battery manufacturing process. Since the interface from rigid LLZO is improved by the flexible GPE buffer, the inability of flexible GPE to inhibit lithium dendrites is compensated by the rigid LLZO in return. As a result, the interface resistances are reduced from 6880 to 473 Ω, the Li symmetric cell exhibits a flat galvanostatic charge/discharge for 400 h without lithium dendrites, and the solid-state Li|GPE@LLZO|LiCoO2 battery exerts a capacity retention of 82.6% after 100 cycles at 0.5 C at room temperature. Such an interfacial engineering approach represents a promising strategy to address solid-solid interface issues and provides a new design for SSBs with high performance.