Abstract

Magnesium‐based batteries are one of the most promising candidates as postlithium electrochemical energy storage devices. Despite considerable research progress, suitable electrolytes supporting long‐term reversible stripping/deposition of magnesium metal in a low content or halide‐free electrolyte are still of great interest. Moreover, the electrolytes should possess certain properties to be a good match with candidate cathode materials. Herein, the electrochemical performance of a novel indolyl‐based electrolyte is presented. Theoretical modeling combined with NMR analysis identifies the magnesium species in the electrolyte. Reversible stripping/deposition of Mg metal in indolyl‐based electrolyte shows long‐term cycling with high coulombic efficiency of >99.5% and yields dendrite‐free magnesium deposition in compact and smooth layers. The X‐ray diffraction shows different preferential structural orientations depending on the electrode substrate. Finally, a proof‐of‐concept Mg║Mo6S8 full cell using the newly developed electrolyte is proposed.

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