Geometry-driven design of 3D-printed gyroid solid electrolyte separators: tortuosity control for enhanced ionic conductivity
摘要
Three-dimensional (3D) printed solid-electrolyte separators offer a tunable structural platform for next-generation batteries, enabling thickness gradients, curvature-conforming interfaces, and architected transport pathways that are not achievable with conventional planar films. However, most separator studies still treat geometry as a packaging constraint rather than a functional design variable, and ionic conductivity is typically interpreted primarily through material chemistry, porosity, or microscale infill features. As a result, there remains a limited mechanistic and quantitative linkage between macroscopic separator topology (global shape and form factor) and effective ionic transport in additively manufactured porous electrolytes. Here, we establish an experimental linkage between 3D separator topology and ionic conductivity using porous polylactic acid (PLA) solid electrolytes fabricated by fused deposition modeling (FDM). Different macroscopic separator geometries were designed and manufactured via an gyroid infill and a fixed 40% infill density to ensure comparable porosity and mesoscale structure. All specimens were sintered with lithium hexafluorophosphate (LiPF₆) under the same thermal conditions to introduce ionic functionality. Effective ionic conductivity was quantified by electrochemical impedance spectroscopy (EIS) at 25 °C and 0 °C. Under identical composition, density, and processing conditions, the separators exhibited topology-dependent transport, with geometry-driven differences in effective ionic conductivity on the order of 10⁻³ S·cm⁻¹. The results demonstrate that macroscopic 3D topology, beyond the shared gyroid micro-architecture plays a decisive role in governing ionic transport in porous polymer solid electrolytes. This work positions separator topology as a design lever for architected solid electrolytes and provides a foundation for topology-transport optimization in 3D-printed battery separators.