Abstract
Magnesium metal batteries (MMBs) currently face challenges suffering from severe Mg metal passivation and extremely high overpotential in conventional electrolytes. Herein, a strategy of using a low-cost deep eutectic solution (DES) is proposed to modify Mg anode with the monolithic and compact coating of a MgCl2-Al-MgCl2 sandwich structure, enabling the stable and reversible Mg plating-stripping behavior. An organic/nanocrystal hybrid interphase is in-situ built through a facile Mg-Al displacement reaction between aluminum-chloro clusters and Mg in AlCl3/Et3NHCl solution, and it can effectively minimize the adverse interfacial passivation reaction and surface diffusion barrier, affording the high ion-conduction and electronic insulation. This DES-assisted method guarantees a highly reversible cycling of Mg metal anode (over 5000h at 0.1mA cm-2 and 400h at 2.0 mAh cm-2) in Mg(TFSI)2/DME electrolyte with the improved interfacial kinetics and low overpotential. Even at a much higher current density of 1mA cm-2, the overpotential only undergoes a slight increase from 0.2V (at 0.1mA cm-2) to 0.23V. The corresponding full cells with CuS and phenanthraquinone cathodes deliver satisfactory cyclic performance. The DES modification strategy provides a new solution to the design of robust and conductive solid electrolyte interphase for achieving high-voltage and durable MMBs.
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