Constructing Effective Interfaces for Li_1.5Al_0.5Ge_1.5(PO₄)₃ Pellets To Achieve Room-Temperature Hybrid Solid-State Lithium Metal Batteries

Solid electrolytes are considered as strong alternatives for conventional liquid electrolytes to overcome the safety issues of next-generation high-energy-density lithium metal batteries (LMBs). Although Li_1.5Al_0.5Ge_1.5(PO₄)₃ (LAGP) has satisfied ionic conductivity at room temperature (∼10^–4 S cm^–1), high stability in air, and can be easily sintered, it still suffers from instability of the lithium metal. Moreover, the large interfacial resistance between solid electrolytes and solid electrodes and the stress generated by the volumetric change of lithium metal anodes during cycling would deteriorate the performance of LMBs. Here, we report an effective solution to overcome the abovementioned problems by introducing a three-dimensional gel polymer electrolyte at the interface between LAGP pellets and lithium metal anodes, achieving stable cycling of LiFePO₄//Li cells at room temperature for 300 cycles. Besides, the degeneration mechanisms of the interfaces of LAGP pellets under different conditions are compared, and peculiar properties different from their counterparts were found.