Modeling of Porous Lithium Metal Electrodes: Turning the Li-Dendrite Problem Around

The properties of rechargeable lithium-ion batteries are determined by the electrochemical and kinetic properties of their constituent materials as well as by their underlying microstructure. Microstructural design can be leveraged to achieve a leap in performance and durability. Here we investigate a porous electrode structure, as a strategy to increase the surface area, and provide structural stability for Li-metal anodes. The porous architecture consists of a mixed electron/ion conductor that function as a scaffold for lithium metal deposition. A new finite element model was developed to simulate the large topological changes associated with Li plating/stripping. This model is used to predict the current density distribution as a function of material and structural properties. A dimensionless quantity that combines Li-ion conductivity, surface impedance and average pore size is shown to be a good indicator to predict the peak current density. Preventing current localization at the separator reduces the risk of cell shorting. The analyses show that the peak current scales as (hG)(1/2), where h is the ratio between surface and bulk conductivity and G is the average pore size. Stability analyses suggest that the growth is morphologically stable, and that confining Li-plating into pores can enable high-energy density solid-state batteries.