Although the soluble
redox mediator (RM) has been effectively applied
in Li–O2 batteries, parasitic reactions between
the lithium anode and RM+ can result in poor cycle performance.
Herein, we proposed a nonelectroactive surfactant (sodium dodecyl
sulfate, SDS) that could adsorb on the hydrophobic carbon surface
and form a stable anionic layer upon charge, which can effectively
suppress the diffusion of oxidized RM+ and facilitate charge
transfer at the electrode–solution interface. To coordinate
with SDS, a new RM named 2-phenyl-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide
(PTIO) was adopted due to its oxidation process following after in
situ formation of the anionic layer. Moreover, as a bifunctional mediator,
PTIO cannot only get a low charge plateau but also greatly enhance
the discharge capacity when applied in Li–O2 batteries.
The electrochemical results demonstrated that the cycling performance,
energy efficiency, and discharge capacity were significantly improved
owing to the synergistic effect of PTIO and SDS.