Anode interfacial layer formation via reductive ethyl detaching of organic iodide in lithium-oxygen batteries.

As soluble catalysts, redox mediators can reduce the high charging overpotential of lithium-oxygen batteries by providing sufficient liquid-solid interface for lithium peroxide decomposition. However, the redox mediators usually introduce undesirable reactions. In particular, the so-called "shuttle effect" leads to the loss of both the redox mediators and electrical energy efficiency. In this study, an organic compound, triethylsulfonium iodide, is found to act bifunctionally as both a redox mediator and a solid electrolyte interphase-forming agent for lithium-oxygen batteries. During charging, the organic iodide exhibits comparable lithium peroxide-oxidizing capability with inorganic iodides. Meanwhile, it in situ generates an interfacial layer on lithium anode via reductive ethyl detaching and the subsequent oxidation. This layer prevents the lithium anode from reacting with the redox mediators and allows efficient lithium-ion transfer leading to dendrite-free lithium anode. Significantly improved cycling performance has been achieved by the bifunctional organic iodide redox mediator.