Mechanical Deformation of a Lithium-Metal Anode Due to a Very Stiff Separator

This work builds on the two-dimensional model presented by Ferrese et al. [J. Electrochem. Soc., 159, A1615 (2012)], which captures the movement of lithium metal at the negative electrode during cycling in a Li-metal/LiCoO2 cell. In this paper, the separator is modeled as a dendrite-inhibiting polymer separator with an elastic modulus of 16 GPa. The separator resists the movement of lithium through the generation of stresses in the cell. These stresses affect the negative electrode through two mechanisms –altering the thermodynamics of the negative electrode and deforming the negative electrode mechanically. From this analysis, we find that the dendrite-inhibiting separator causes plastic and elastic deformation of the lithium at the negative electrode which flattens the electrode considerably when compared to the liquid-electrolyte case. This flattening of the negative electrode causes only very slight differences in the local state of charge in the positive electrode. When comparing the magnitude of the effects flattening the negative electrode, we find that the plastic deformation plays a much larger role than either the pressure-modified reaction kinetics or elastic deformation. This is due to the low yield strength of the lithium metal, which limits the stresses such that they have only a small effect on the reaction kinetics.