Taming Interfacial Instability in Lithium–Oxygen Batteries: A Polymeric Ionic Liquid Electrolyte Solution

Abstract There is a growing concern about the cyclability and safety, in particular, of the high‐energy density lithium–metal batteries. This concern is even greater for Li–O 2 batteries because O 2 that is transported from the cathode to the anode compartment, can exacerbate side reactions and dendrite growth of the lithium metal anode. The key to solving this dilemma lays in tailoring the solid electrolyte interphase (SEI) formed on the lithium metal anode in Li–O 2 batteries. Here it is reported that a new electrolyte, formed from LiFSI as the salt and a mixture of tetraethylene glycol dimethyl ether and polymeric ionic liquid of P[C 5 O 2 N MA,11 ]FSI as the solvent, can produce a stable electrode (both cathode and anode)|electrolyte interface in Li–O 2 batteries. Specifically, this new electrolyte, when in contact with lithium metal anodes, has the ability to produce a uniform SEI with high ionic conductivity for Li + transport and desired mechanical property for suppression of dendritic lithium growth. Moreover, the electrolyte possesses a high oxidation tolerance that is very beneficial to the oxygen electrochemistry on the cathode of Li–O 2 batteries. As a result, enhanced reversibility and cycle life are realized for the resultant Li–O 2 batteries.