Concerted ionic-electronic conductivity enables high-rate capability Li-metal solid-state batteries

Abstract

Enabling the fast charge and discharge of Li-metal solid-state batteries paves the way towards their deployment in electro-mobility applications, which require high-energy and power with safety guaranteed. Solid-state batteries using polyethylene oxide as the polymer matrix are appealing candidates although currently limited to relatively slow rate capability arising from high solid-solid interfacial resistance and sluggish lithium-ion mobility at the solid electrolyte. In this work, the engineering design and optimization of composite electrodes with multi-walled carbon nanotubes lead to high performance Li metal solid-state cells, showing a high-capacity retention at rates up to 4C. The electrode formulations including the elongated architectures exhibit a concerted ionic-electronic diffusion in the catholyte polymer enabling fast Li-ion transport, enhancing the electronic percolation and increasing the interfacial reaction kinetics and exchange current density. The solid-state battery with LiFePO4 electrode shows an unprecedented capacity retention of 92% during 800 cycles at 2C. The promising performance at high-rates of this approach is also extended to electrodes with a high-voltage active material.