Preparation and Failure Behavior of Gel Electrolytes for Multilayer Structure Lithium Metal Solid-State Batteries

High safety gel polymer electrolyte (GPE) is used in lithium metal solid state batteries, which has the advantages of high energy density, wide temperature range, high safety, and is considered as a subversive new generation battery technology. However, solid-state lithium batteries with multiple layers and large capacity currently have poor cycle life and a large gap between the actual output cycle capacity retention rate and the theoretical level. In this paper, polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP)/polyacrylonitrile (PAN)-lithium perchlorate (LiClO₄)-lithium lanthanum zirconium tantalate (LLZTO) gel polymer electrolytes was prepared by UV curing process using a UV curing machine at a speed of 0.01 m/min for 10 s, with the temperature controlled at 30 °C and wavelength 365 nm. In order to study the performance and failure mechanism of multilayer solid state batteries, single and three layers of solid state batteries with ceramic/polymer composite gel electrolyte were assembled. The results show that the rate and cycle performance of single-layer solid state battery with gel electrolyte are better than those of three-layer solid state battery. As the number of cycles increases, the interface impedance of both single-layer and three-layer electrolyte membrane solid-state batteries shows an increasing trend. Specifically, the three-layer battery impedance increased from 17 Ω to 42 Ω after 100 cycles, while the single-layer battery showed a smaller increase, from 2.2 Ω to 4.8 Ω, indicating better interfacial stability. After 100 cycles, the interface impedance of multi-layer solid-state batteries increases by 9.61 times that of single-layer batteries. After 100 cycles, the corresponding capacity retention rates were 48.9% and 15.6%, respectively. This work provides a new strategy for large capacity solid state batteries with gel electrolyte design.