Boosting adsorption and dissociation kinetics of magnesium-chloride ion pair via bismuth/indium-based artificial interface

The formation of passivating interphases on Mg-metal anode is impeding the wide employment of rechargeable Mg-metal batteries with less safety and cost concerns. Despite engineering artificial interlayers offers an efficient solution, it still falls short of expectation because of the compromised Mg plating/stripping performances in conventional electrolyte systems. In this work, a unique bismuth/indium-based artificial interface is introduced, which enables an exceptional reversibility (lowest nucleation overpotential of 189 mV than that (583 mV) of pristine Mg anode), high rate capability (a stable charge and discharge operation at 5.0 mA cm-2 without short circuit) and good temperature tolerance (being cyclable over 10 degrees C and 50 degrees C) for the first time. This bismuth/ indium-based artificial interface is constructed by facile displacement reactions between Bi(CF3SO3)3/In (CF3SO3)3 and Mg. The dominant interphases, including Bi, In and BiOx species, can be controllably tailored via adjusting the relative ratio and concentration of Bi(CF3SO3)3/In(CF3SO3)3. Theoretical calculation results accompanied by electrochemical experiments indicate that kinetically favorable adsorption and dissociation processes of Mg-Cl ion pair on this interface, affording good magnesiophilic property and fast charge transfer kinetics, are responsible for the improved Mg-metal anode properties.