Scalable Manufacturing of Hybrid Solid Electrolytes with Interface Control

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 7S 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 mu m 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 x 10(-6) S cm(-1) compared to the conductivity of single-material films (25 wt %, 1.2 x 10(-6) S 75 wt %, 1.8 x 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.