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Cycling and Failing of Lithium Metal Anodes in Carbonate Electrolyte

Lithium metal electrodes promise high energy density, but their poor cycling stability has been limiting applications in real batteries. In this study, we examine the cycling and failing behaviors of Li metal electrodes in a commercial carbonate electrolyte and their dependence on the electrode thickness and cycling conditions. We find that thick and thin Li metal electrodes fail for different reasons. The cycle life of a Li||Cu cell with a thick (∼80 mAh cm–2) Li foil electrode can be divided into three stages, and the cell stops functioning when ionic transport is blocked by the accumulated solid electrolyte interphase layer on the Cu electrode. In contrast, thin (2 mAh cm–2) Li metal electrodes fail because of Li metal depletion caused by side reactions with the electrolyte, and their cycle life is determined by Coulombic efficiency. The results suggest that application-relevant performance of Li metal anodes should be assessed using thin and deeply cycled electrodes rather than the currently prevalent...