Hybrid solid electrolytes are promising alternatives for high energy density metallic lithium batteries. Scalable manufacturing of multi-material electrolytes with tailored transport pathways can provide an avenue toward controlling Li stripping and deposition mechanisms in all-solid-state devices. A novel roll-to-roll compatible coextrusion device is demonstrated to investigate mesostructural control during manufacturing. Solid electrolytes with 25 and 75 wt % PEO-LLZO compositions are investigated. The coextrusion head is demonstrated to effectively process multimaterial films with strict compositional gradients in a single pass. An average manufacturing variability of 5.75 ± 1.2 μm is observed in the thickness across all the electrolytes manufactured. Coextruded membranes with 1 mm stripes show the highest room temperature conductivity of 8.8 × 10-6 S cm-1 compared to the conductivity of single-material films (25 wt %, 1.2 × 10-6 S cm-1; 75 wt %, 1.8 × 10-6 S cm-1). Distribution of relaxation times and effective mean field theory calculations suggest that the interface generated between the two materials possesses high ion-conducting properties. Computational simulations are used to further substantiate the influence of macroscale interfaces on ion transport.
Keywords: coextrusion; hybrid solid electrolyte; interfaces; ion transport; process control; scalable manufacturing; solid-state battery.