Suppressed lithium dendrite growth in lithium batteries using ionic liquid electrolytes: Investigation by electrochemical impedance spectroscopy, scanning electron microscopy, and in situ7Li nuclear magnetic resonance spectroscopy

In this work, the formation of lithium dendrites in lithium/Li4Ti5O12 battery cells is studied using different experimental techniques. Electrochemical impedance spectroscopy is presented as a tool to investigate non-invasively the dendritic growth on a lithium metal surface in lithium/Li4Ti5O12 cells during numerous discharging/charging cycles. Scanning electron microscopy is used for visual inspection of the dendrite formation. In situ7Li nuclear magnetic resonance spectroscopy is sensitive to quantitative changes at the lithium metal surface. Application to symmetrical lithium/lithium battery cells allows for a careful comparison of the investigated electrolytes. All these experimental methods provide consistent results. It is demonstrated that the growth of lithium dendrites is significantly correlated to the electrolyte employed. All electrolytes based on the ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethane-sulfonyl)azanide (EMIM-TFSA) show reduced dendrite growth in comparison to the standard electrolyte for Li-ion batteries, lithium hexafluorophosphate (LiPF6) in ethylene carbonate/dimethyl carbonate (EC/DMC). LiPF6 in EMIM-TFSA and LiPF6 in EMIM-TFSA/propylene carbonate suppress lithium dendrites most efficiently.

► Non-invasive and quantitative investigation of Li dendrite formation in Li batteries by 7Li NMR and impedance spectroscopy.
► SEM images show good agreement with NMR and impedance results.
► The growth of lithium dendrites is significantly correlated to the electrolyte employed.
► Li dendrite growth can be suppressed by electrolytes containing ionic liquids.