Tandem Interface and Bulk Li-Ion Transport in a Hybrid Solid Electrolyte with Microsized Active Filler

In common hybrid solid electrolytes (HSEs), either the ionic conductivity of the polymer electrolyte is enhanced by the presence of a nanosized inorganic filler, which effectively decrease the glass-transition temperature, or the polymer solid electrolyte acts mostly as a flexible host for the inorganic solid electrolyte, the latter providing the conductivity. Here a true HSE is developed that makes optimal use of the high conductivity of the inorganic solid electrolyte and the flexibility of the polymer matrix. It is demonstrated that the LAGP (Li_1.5Al_0.5Ge_1.5(PO₄)₃) participates in the overall conductivity and that the interface environment between the poly(ethylene oxide) (PEO) and LAGP plays a key role in utilizing the high conductivity of the LAGP. This HSE demonstrates promising cycling versus Li-metal anodes and in a full Li-metal solid-state battery. This strategy offers a promising route for the development of Li-metal solid-state batteries, aiming for safe and reversible high-energy-density batteries.