Twin problems of interfacial carbonate formation in nonaqueous Li-O2 batteries

B. D. McCloskey, A. Speidel, R. Scheffler, D. C. Miller, V. Viswanathan, J. S. Hummelshøj, J. K. Nørskov, A. C. Luntz*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

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-O2 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.

Original languageEnglish
JournalJournal of Physical Chemistry Letters
Volume3
Issue number8
Pages (from-to)997-1001
Number of pages5
ISSN1948-7185
DOIs
Publication statusPublished - 2012
Externally publishedYes

Bibliographical note

Copyright © 2012 American Chemical Society. This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

Cite this

McCloskey, B. D., Speidel, A., Scheffler, R., Miller, D. C., Viswanathan, V., Hummelshøj, J. S., Nørskov, J. K., & Luntz, A. C. (2012). Twin problems of interfacial carbonate formation in nonaqueous Li-O2 batteries. Journal of Physical Chemistry Letters, 3(8), 997-1001. https://doi.org/10.1021/jz300243r