Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 6, Issue 15, Pages 12083-12092Publisher
AMER CHEMICAL SOC
DOI: 10.1021/am5010943
Keywords
electrochemical growth; oxidation; Li2O2 toroid; lithium superoxide; electrolyte decomposition; metal-air battery
Funding
- German Federal Ministry of Education and Research (BMBF)
- state of Hessen (Laboratory for Materials Research, ElCh platform)
- Store-E project (LOEWE Program, State of Hessen)
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Lithium peroxide (Li2O2), the solid and intrinsically electronic insulating discharge product of Li-O-2 batteries strongly influences the discharge and charge kinetics. In a series of experiments, we investigated the growth of Li2O2 upon discharge and the corresponding reduction and oxidation processes by varying the depth of discharge. The results indicate that insulating Li2O2 particles with a disc-like shape were formed during the initial discharge stage. Afterward, the nucleation and growth of Li2O2 resulted in the formation of conducting Li2O2 shells. When the discharge voltage dropped below 2.65 V, the Li2O2 discs evolved to toroid-shaped particles and defective superoxide-like phase presumably with high conductivity was formed on the rims of Li2O2 toroids. Both Li2O2 and the superoxide-like phase are unstable in ether-based electrolytes resulting in the degradation of the corresponding cells. Nevertheless, by controlling the growth of Li2O2, the chemical reactivity of the discharge product can be suppressed to improve the reversibility of Li-O-2 batteries.
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