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A novel fluorine-free ionic liquid electrolyte comprising lithium dicyanamide (LiDCA) and trimethyl(isobutyl)phosphonium tricyanomethanide (P 111i4 TCM) in a 1:9 molar ratio is studied as an electrolyte for lithium metal batteries. At room temperature, it demonstrates high ionic conductivity and viscosity of about 4.5 mS cm −1 and 64.9 mPa s, respectively, as well as a 4 V electrochemical stability window (ESW). Li stripping/ plating tests prove the excellent electrolyte compatibility with Li metal, evidenced by the remarkable cycling stability over 800 cycles. The evolution of the Li−electrolyte interface upon cycling was investigated via electrochemical impedance spectroscopy, displaying a relatively low impedance increase after the initial formation cycles. Finally, the solid electrolyte interphase (SEI) formed on Li metal appeared to have a bilayer structure mostly consisting of DCA and TCM reduction products. Additionally, decomposition products of the phosphonium cation were also detected, despite prior studies reporting its stability against Li metal.

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