Ammonium Ionic Liquid-Functionalized Phenothiazine as a New Redox Mediator for High Chemical Stability on the Anode Surface in Lithium–Air Batteries

The application of redox mediators (RMs) as soluble catalysts can address the problem of insufficient contact between conventional solid catalysts for lithium-air batteries (LABs). However, oxidized RM molecules migrate to the lithium anode and react with lithium, which results in the accumulation of surface corrosion products that weaken the redox activity of the RM. This paper presents a new combination of phenothiazine (PTZ) as an RM and an ammonium-based ionic liquid (IL) source as a protective agent to prevent the side reactions with lithium and to enhance the electrochemical performance of LABs. IL-functionalized PTZ (IL-PTZ) was successfully synthesized through N-alkylation, quaternization, and anion-exchange reactions. IL-PTZ improved the chemical stability of the RM molecules on the lithium surface as well as the electrochemical performance. A microstructural analysis revealed that the IL group in the IL-PTZ molecules facilitated smooth lithium stripping/plating by blocking the side reactions between the RM and lithium. Compared with the LAB with the PTZ electrolyte, that with the IL-PTZ electrolyte exhibited a significantly higher discharge capacity (2500 mA h/g vs 1500 mA h/g) and a cycle life that was 2 times longer. The IL-PTZ molecule was demonstrated to exhibit great potential as a novel soluble catalyst for application in high-performance LABs.