Redox
mediators (RMs) are solution-based additives that have been
extensively used to reduce the charge potential and increase the energy
efficiency of Li–oxygen (Li–O2) batteries.
However, in the presence of RMs, achieving a long cycle-life operation
of Li–O2 batteries at a high current rate is still
a major challenge. In this study, we discover a novel synergy among
InX3 (X = I and Br) bifunctional RMs, molybdenum disulfide
(MoS2) nanoflakes as the air electrode, dimethyl sulfoxide/ionic
liquid hybrid electrolyte, and LiTFSI as a salt to achieve long cycle-life
operations of Li–O2 batteries in a dry air environment
at high charge–discharge rates. Our results indicate that batteries
with InI3 operate up to 450 cycles with a current density
of 0.5 A g–1 and 217 cycles with a current density
of 1 A g–1 at a fixed capacity of 1 A h g–1. Batteries with InBr3 operate up to 600 cycles with a
current density of 1 A g–1. These batteries can
also operate at a higher charge rate of 2 A g–1 up
to 200 cycles (for InBr3) and 160 cycles (for InI3). Our experimental and computational results reveal that while X3
– is the source of the redox mediator, LiX
at the MoS2 cathode, In3+ reacts on the lithium
anode side to form a protective layer on the surface, thus acting
as an effective bifunctional RM in a dry air environment. This evidence
for a simultaneous improvement in the current rates and cycle life
of a battery in a dry air atmosphere opens a new direction for research
for advanced energy storage systems.