PNNL

Abstract

The temperature dependence of the oxygen reduction mechanism in Li-O2 batteries was investigated using carbon nanotube-based air electrodes and 1,2-dimethoxyethane-based electrolyte within a temperature range of 20C to 40C. It is found that the discharge capacity of the Li-O2 batteries decreases from 7,492 mAh g-1 at 40C to 2,930 mAh g-1 at 0C. However, a sharp increase in capacity was found when the temperature was further decreased and a very high capacity of 17,716 mAh g-1 was observed at 20C at a current density of 0.1 mA cm-2. When the temperature increases from 20C to 40C, the morphologies of the Li2O2 formed varied from ultra-small spherical particles to small flakes and then to large flake-stacked toroids. The lifetime of superoxide and the solution pathway play a dominate role on the battery capacity in the temperature range of -20C to 0C, but the electrochemical kinetics of oxygen reduction and the surface pathway dominate the discharge behavior in the temperature range of 0C to 40C. These findings provide fundamental understanding on the temperature dependence of oxygen reduction process in a Li-O2 battery and will enable a more rational design of Li-O2 batteries.