The Influence of Interfacial Chemistry on Magnesium Electrodeposition in Non-nucleophilic Electrolytes Using Sulfone-Ether Mixtures

One of the limiting factors in the development of magnesium batteries is the reversibility of magnesium electrodeposition and dissolution at the anode. Often irreversibility is related to impurities and decomposition. Herein we report on the cycling behavior of magnesium metal anodes in different electrolytes, Mg(HMDS)2 – 4 MgCl2 in tetrahydrofuran (THF) and a butyl sulfone/THF mixture. The deposition morphology and anode-electrolyte interface is studied and related to Mg/Mg cell cycling performance. It is found that adding the sulfone caused the formation of a boundary layer at the electrode-electrolyte interface, which, in turn, resulted in a particle-like deposition morphology. This type of deposition has a high surface area, which alters the effective local current density and results in electronically isolated deposits. Extended cycling resulted in magnesium growth through a separator. Electrolyte decomposition is observed with and without the addition of the sulfone, however the addition of the sulfone increased the degree of decomposition.