High-entropy Electrolyte Enables High Reversibility and Long Lifespan for Magnesium Metal Anodes.

The stable cycling of Mg-metal anodes is limited by several problems, including sluggish electrochemical kinetics and passivation at the Mg surface. In this study, we present a high-entropy electrolyte composed of lithium triflate (LiOTf) and trimethyl phosphate (TMP) co-added to magnesium bis(trifluoromethane sulfonyl)imide (Mg(TFSI) /1,2-dimethoxyethane (DME) to significantly improve the electrochemical performance of Mg-metal anodes. The as-formed high-entropy Mg -2DME-OTf -Li -DME-TMP solvation structure effectively reduced the Mg -DME interaction in comparison with that observed in traditional Mg(TFSI) /DME electrolytes, thereby preventing the formation of insulating components on the Mg-metal anode and promoting its electrochemical kinetics and cycling stability. Comprehensive characterization revealed that the high-entropy solvation structure brought OTf and TMP to the surface of the Mg-metal anode and promoted the formation of a Mg (PO ) -rich interfacial layer, which is beneficial for enhancing Mg conductivity. Consequently, the Mg-metal anode achieved excellent reversibility with a high Coulombic efficiency of 98 % and low voltage hysteresis. This study provides new insights into the design of electrolytes for Mg-metal batteries.