Electrolyte Solutions with a Wide Electrochemical Window for Rechargeable Magnesium Batteries

Electrolyte solutions for rechargeable Mg batteries were developed, based on reaction products of phenyl magnesium chloride (PhMgCl) Lewis base and Alcl 3 Lewis acid in ethers. The transmetallation of these ligands forms solutions with Mg x Cl + y and AlCl 4-n Ph n - ions as the major ionic species, as analyzed by multinuclei nuclear magnetic resonance spectroscopy. Tetrahydrofuran (THF) solutions of (PhMgCl) 2 -Alcl 3 exhibit optimal properties: highly reversible Mg deposition (100% cycling efficiency) with low overvoltage: <0.2 V and electrochemical windows wider than 3 V. A specific conductivity of 2-5 X 10 -3 Ω -1 cm -1 could be measured between -10 and 30°C for these solutions, similar to that of standard electrolyte solutions for Li batteries. Mg ions intercalate reversibly with Chevrel phase (Mg x Mo 6 S 8 ) cathodes in these solutions. These systems exhibit high thermal stability. The solutions may enable the use of high voltage, high-capacity Mg insertion materials as cathodes and hence open the door for research and development of high-energy density, rechargeable Mg batteries.