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The potential advantages of lithium metal anodes have received widespread attention (highest capacity, lowest reduction potential, etc). However, the poor stability of Li metal / liquid electrolyte interfaces leads to chronic problems, such as dendrite formation and capacity loss. The possible impact of mechanical effects on interface stability and dendrite formation are difficult to probe directly. In this study, stress evolution during lithium plating and stripping was monitored with precise in situ measurements. The data obtained with different film thicknesses made it possible to separate the stresses associated with the lithium metal and the solid electrolyte interphase (SEI). The results show that significant stresses are created in the SEI films. Based on this, a basic model of wrinkling-ratcheting-delamination is also presented. This analysis indicates that plasticity in a growing Li film can enhance surface wrinkling, and thus lead to morphological destabilization of a planar growth front.

The potential advantages of lithium (Li) metal anodes have been widely touted (lowest reduction potential, etc.). However, the poor stability of Li metal / liquid electrolyte interfaces leads to chronic problems, such as dendrite formation and capacity loss. The possible impact of mechanical effects on interface stability and dendrite formation is a critical question that is difficult to probe directly. In-situ curvature measurements are an important tool for monitoring stresses during battery cycling. Using this technique during Li plating and examining film thickness effects, it is possible to separate contributions from the bulk lithium metal and the solid electrolyte interphase (SEI). These investigations show that significant stresses are created in the SEI films. Similar stress evolution measurements were also performed during lithium plating and stripping using both soft (PEO) and hard (LiF) artificial surface layers. The results indicate that stresses in surface films can be tuned to improve performance when artificial SEI layers are employed. A basic chemo-mechanical model indicates that hybridizing the two layers may benefit interface stability and performance in Li metal anodes.