Solid-State Electrodes and Electrolytes with Tunable and Low-Tortuosity Micro-Architected Structures from Nonequilibrium Processing

The miniaturization of electronics and development of the internet of things (IOT) demands dense and solid-state energy storage on the square millimeter scale, as well as the ability to supply energy over a spectrum of response times. These goals require reimagined processing methods that move beyond planar architectures to create free-standing and active material dense architectures which can serve as the backbone for energy and power dense solid-state batteries (SSBs). Here we introduce a material-agnostic hybrid inorganic phase inversion (HIPI) process as an advanced scalable manufacturing method that results in free-standing solid-state low-tortuosity architectures with anisotropic through-plane material orientation. Critical to their deployment as an active framework in SSBs is the accessible porosity present in the HIPI architectures, resulting from the use of an oligo(ethylene oxide)-based organogel support. The HIPI process can enable both interdigitated electrodes and low-tortuosity solid electrolytes whose relevant feature sizes between 1-20 µm can be tailored by tuning the gelation temperature and nucleation density of the inorganic suspension during the nonequilibrium HIPI process. By tailoring these architectures, the pitch and areal enhancement factor can be adjusted within a multiparameter space to meet both shape constraints and performance demands of specific energy storage applications.