Half-Covered ‘Glitter-Cake’ AM@SE Composite: A Novel Electrode Design for High Energy Density All-Solid-State Batteries

Abstract

Highlights

A novel electrode design for high energy density all-solid-state batteries (ASSBs) is realized through the control of nano- and microstructures.

An active materials@solid electrolyte composite with a half-covered “glitter-cake” morphology is adopted to optimize the transport of electrons and ions in the electrode.

The optimized electrode design exhibited a volumetric energy density of 1258 Wh L⁻¹ at an active material content of 85 wt%, exceeding the performance of the reported ASSB cells.

All-solid-state batteries (ASSBs) are pursued due to their potential for better safety and high energy density. However, the energy density of the cathode for ASSBs does not seem to be satisfactory due to the low utilization of active materials (AMs) at high loading. With small amount of solid electrolyte (SE) powder in the cathode, poor electrochemical performance is often observed due to contact loss and non-homogeneous distribution of AMs and SEs, leading to high tortuosity and limitation of lithium and electron transport pathways. Here, we propose a novel cathode design that can achieve high volumetric energy density of 1258 Wh L⁻¹ at high AM content of 85 wt% by synergizing the merits of AM@SE core–shell composite particles with conformally coated thin SE shell prepared from mechanofusion process and small SE particles. The core–shell structure with an intimate and thin SE shell guarantees high ionic conduction pathway while unharming the electronic conduction. In addition, small SE particles play the role of a filler that reduces the packing porosity in the cathode composite electrode as well as between the cathode and the SE separator layer. The systematic demonstration of the optimization process may provide understanding and guidance on the design of electrodes for ASSBs with high electrode density, capacity, and ultimately energy density.