In situ observation of cracking and self-healing of solid electrolyte interphases during lithium deposition

The growth of lithium (Li) whiskers is detrimental to Li batteries. However, it remains a challenge to directly track Li whisker growth. Here we report in situ observations of electrochemically induced Li deposition under a CO₂ atmosphere inside an environmental transmission electron microscope. We find that the morphology of individual Li deposits is strongly influenced by the competing processes of cracking and self-healing of the solid electrolyte interphase (SEI). When cracking overwhelms self-healing, the directional growth of Li whiskers predominates. In contrast, when self-healing dominates over cracking, the isotropic growth of round Li particles prevails. The Li deposition rate and SEI constituent can be tuned to control the Li morphologies. We reveal a new "weak-spot" mode of Li dendrite growth, which is attributed to the operation of the Bardeen-Herring growth mechanism in the whisker's cross section. This work has implications for the control of Li dendrite growth in Li batteries.