Abstract
In this work we introduce an approach to fabricate a solid composite electrolyte film that is thin, ionically conductive, and mechanically robust with good potential for manufacturability, in the application of lithium metal batteries. First a doped-lithium aluminum titanium phosphate ceramic thin film with thickness of ~25 μm is formed by aqueous spray coating, a scalable process. The film is partially sintered to form a three-dimensionally interconnected structure with a dense backbone. It is then backfilled with a crosslinkable poly(ethylene oxide) (PEO)-based polymer electrolyte. The composite has very high ceramic loading of 77 wt% (61 vol%) and an ionic conductivity of 3.5 × 10-5 S/cm at 20 °C with an activation energy of 0.43 eV. The main ion transport pathway is through the ceramic network, predicted by modelling and verified by experiments. Owing to the interconnected structure of the ceramic, the composite electrolyte exhibits much improved mechanical strength.
