RESUMEN
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 /Et3 NHCl 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 5000 h at 0.1 mA cm-2 and 400 h 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 1 mA cm-2 , the overpotential only undergoes a slight increase from 0.2 V (at 0.1 mA cm-2 ) to 0.23 V. 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.
RESUMEN
The development of high-voltage Mg metal batteries is hampered by the incompatibility between a Mg metal anode and conventional electrolyte, leading to a high overpotential for Mg plating/stripping processes. In this work, we tailored a hybrid functional layer consisting of Bi/MgCl2/polytetrahydrofuran (PTHF) by an in situ THF polyreaction during the reaction of the Mg anode with BiCl3 solution. The introduction of PTHF inhibits the growth of Bi particles and fills the layer interstice with MgCl2-containing PTHF, improving the structural integrity of the functional layer and insulation between the electrolyte and Mg anode. As a result, compared to a simply modified Bi/MgCl2 layer, the Bi/MgCl2/PTHF functional layer exhibits a lower polarization voltage of 0.25 V and longer cycling life of more than 2000 h at 0.1 mA cm-2. Mechanism analysis shows that Mg is plated on the surface of Bi particles within the layer. The Mo6S8/Mg full battery with the hybrid functional layer achieved a low voltage hysteresis of â¼0.25 V and long cycling life over 500 cycles at 50 mA g-1. This work provides a facile and effective hybrid functional layer strategy to realize Mg metal batteries in conventional electrolytes.