Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 3, Issue 8, Pages 997-1001Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz300243r
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Funding
- Department of Energy, Basic Energy Sciences through the SUNCAT Center for Interface Science and Catalysis
- UTRC fellowship
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We use XPS and isotope labeling coupled with differential electrochemical mass spectrometry (DEMS) to show that small amounts of carbonates formed during discharge and charge of Li-O-2 cells in ether electrolytes originate from reaction of Li2O2 (or LiO2) both with the electrolyte and with the C cathode. Reaction with the cathode forms approximately a monolayer of Li2CO3 at the C-Li2O2 interface, while reaction with the electrolyte forms approximately a monolayer of carbonate at the Li2O2 electrolyte interface during charge. A simple electrochemical model suggests that the carbonate at the electrolyte-Li2O2 interface is responsible for the large potential increase during charging (and hence indirectly for the poor rechargeability). A theoretical charge-transport model suggests that the carbonate layer at the C-Li2O2 interface causes a 10-100 fold decrease in the exchange current density. These twin interfacial carbonate problems are likely general and will ultimately have to be overcome to produce a highly rechargeable Li-air battery.
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