A Novel Regulation Strategy of Solid Electrolyte Interphase Based on Anion‐Solvent Coordination for Magnesium Metal Anode

Abstract

Magnesium (Mg) metal anode is a highly desirable candidate among various high energy density metal anodes, possessing higher volumetric capacity and better safety characteristic compared to lithium metal. However, most Mg salts in conventional Mg electrolytes easily react with Mg metal to form blocking layers, leading to inferior reversibility of Mg plating/stripping. Here, a stable Mg²⁺ -conducting solid electrolyte interphase (SEI) is successfully constructed on Mg metal anode by regulating the molecular-orbital-energy-level toward an aluminum(III)-centered anion Mg salt through anion-solvent coordination. Of which, the LUMO energy level of perfluorinated pinacolatoaluminate (Al(O₂ C₂ (CF₃ )₄ )₂ ^- , abbreviated as FPA) anion has been adjusted by coordinating with solvent molecule (tetrahydrofuran) for facilitating the formation of advantageous SEI. The existence of SEI formed by FPA anion greatly improves the reversibility and long-term stability of Mg plating/stripping process. More importantly, based on this aluminum(III)-centered Mg electrolyte, the Mo₆ S₈ /Mg batteries can achieve a fantastic cycle performance of 9000 cycles, proving the beneficial effect of SEI on the cycling stability of Mg battery system. These findings open up a promising avenue to construct stable and compatible SEI on Mg metal anode, and lay significant foundations for the successful development of rechargeable Mg metal batteries.