Reversible Magnesium Metal Cycling in Additive-Free Simple Salt Electrolytes Enabled by Spontaneous Chemical Activation

Abstract

Rechargeable magnesium (Mg) batteries can offer higher volumetric energy densities and be safer than their conventional counterparts, lithium-ion batteries. However, their practical implementation is impeded due to the passivation of the Mg metal anode or the severe corrosion of the cell parts in conventional electrolyte systems. Here, we present a chemical activation strategy to facilitate the Mg deposition/ stripping process in additive-free simple salt electrolytes. By exploiting the simple immersion-triggered spontaneous chemical reaction between reactive organic halides and Mg metal, the activated Mg anode exhibited an overpotential below 0.2 V and a Coulombic efficiency as high as 99.5% in a Mg(TFSI)2 electrolyte. Comprehensive analyses reveal simultaneous evolution of morphology and interphasial chemistry during the activation process, through which stable Mg cycling over 990 cycles was attained. Our activation strategy enabled the efficient cycling of Mg full-cell candidates using commercially available electrolytes, thereby offering possibilities of building practical Mg batteries.