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Reactions in the Rechargeable Lithium-O-2 Battery with Alkyl Carbonate Electrolytes

Research output: Contribution to journalJournal article

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  • Stefan A. Freunberger
  • Yuhui Chen
  • Zhangquan Peng
  • John M. Griffin
  • Laurence J. Hardwick
  • Fanny Barde
  • Petr Novak
  • Peter G. Bruce
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<mark>Journal publication date</mark>25/05/2011
<mark>Journal</mark>Journal of the American Chemical Society
Issue number20
Volume133
Number of pages8
Pages (from-to)8040-8047
StatePublished
Early online date27/04/11
Original languageEnglish

Abstract

The nonaqueous rechargeable lithium-O-2 battery containing an alkyl carbonate electrolyte discharges by formation of C3H6(OCO2Li)(2), Li2CO3, HCO2Li, CH3CO2Li, CO2, and H2O at the cathode, due to electrolyte decomposition. Charging involves oxidation of C3H6(OCO2Li)(2), Li2CO3, HCO2Li, CH3CO2Li accompanied by CO2 and H2O evolution. Mechanisms are proposed for the reactions on discharge and charge. The different pathways for discharge and charge are consistent with the widely observed voltage gap in Li-O-2 cells. Oxidation of C3H6(OCO2Li)(2) involves terminal carbonate groups leaving behind the OC3H6O moiety that reacts to form a thick gel on the Li anode. Li2CO3, HCO2Li, CH3CO2Li, and C3H6(OCO2Li)(2) accumulate in the cathode on cycling correlating with capacity fading and cell failure. The latter is compounded by continuous consumption of the electrolyte on each discharge.