All-Solid-State Batteries Using Rationally Designed Garnet Electrolyte Frameworks

Functioning bulk-type all-solid-state batteries in a practical form factor with composite positive electrodes, using Al-substituted Li7La3Zr2O12 (LLZO) as the solid electrolyte, have been demonstrated for the first time. The devices incorporate bilayers composed of dense LLZO membranes and porous LLZO scaffolds infiltrated with LiNi0.6Mn0.2Co0.2O2 and other components as positive electrodes, combined with lithium anodes. The porous scaffolds are prepared using an easily scaled freeze-tape-casting method. The unidirectional pores of the scaffold facilitate infiltration of cathode components and shorten lithium ion diffusion path lengths, while the addition of a soft ionically conductive solid to the scaffold ensures good contact among the components.