Reactions in the rechargeable lithium-O2 battery with alkyl carbonate electrolytes

Stefan A. Freunberger; Yuhui Chen; Zhangquan Peng; John M. Griffin; Laurence J. Hardwick; Fanny Bardé; Petr Novák; Peter G. Bruce

doi:10.1021/ja2021747

Reactions in the rechargeable lithium-O₂ battery with alkyl carbonate electrolytes

Stefan A. Freunberger, Yuhui Chen, Zhangquan Peng, John M. Griffin, Laurence J. Hardwick, Fanny Bardé, Petr Novák, Peter G. Bruce

Research output: Contribution to journal › Article › peer-review

1186 Scopus citations

Abstract

The nonaqueous rechargeable lithium-O₂ battery containing an alkyl carbonate electrolyte discharges by formation of C₃H ₆(OCO₂Li)₂, Li₂CO₃, HCO₂Li, CH₃CO₂Li, CO₂, and H ₂O 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-O₂ cells. Oxidation of C₃H₆(OCO ₂Li)₂ involves terminal carbonate groups leaving behind the OC₃H₆O moiety that reacts to form a thick gel on the Li anode. Li₂CO₃, HCO₂Li, CH₃CO ₂Li, 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.

Original language	English
Pages (from-to)	8040-8047
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	133
Issue number	20
DOIs	https://doi.org/10.1021/ja2021747
State	Published - 25 May 2011
Externally published	Yes

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@article{edbb6967212346aab2ae3100144de42b,

title = "Reactions in the rechargeable lithium-O2 battery with alkyl carbonate electrolytes",

abstract = "The nonaqueous rechargeable lithium-O2 battery containing an alkyl carbonate electrolyte discharges by formation of C3H 6(OCO2Li)2, Li2CO3, HCO2Li, CH3CO2Li, CO2, and H 2O 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-O2 cells. Oxidation of C3H6(OCO 2Li)2 involves terminal carbonate groups leaving behind the OC3H6O moiety that reacts to form a thick gel on the Li anode. Li2CO3, HCO2Li, CH3CO 2Li, 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.",

author = "Freunberger, {Stefan A.} and Yuhui Chen and Zhangquan Peng and Griffin, {John M.} and Hardwick, {Laurence J.} and Fanny Bard{\'e} and Petr Nov{\'a}k and Bruce, {Peter G.}",

year = "2011",

month = may,

day = "25",

doi = "10.1021/ja2021747",

language = "英语",

volume = "133",

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T1 - Reactions in the rechargeable lithium-O2 battery with alkyl carbonate electrolytes

AU - Freunberger, Stefan A.

AU - Chen, Yuhui

AU - Peng, Zhangquan

AU - Griffin, John M.

AU - Hardwick, Laurence J.

AU - Bardé, Fanny

AU - Novák, Petr

AU - Bruce, Peter G.

PY - 2011/5/25

Y1 - 2011/5/25

N2 - The nonaqueous rechargeable lithium-O2 battery containing an alkyl carbonate electrolyte discharges by formation of C3H 6(OCO2Li)2, Li2CO3, HCO2Li, CH3CO2Li, CO2, and H 2O 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-O2 cells. Oxidation of C3H6(OCO 2Li)2 involves terminal carbonate groups leaving behind the OC3H6O moiety that reacts to form a thick gel on the Li anode. Li2CO3, HCO2Li, CH3CO 2Li, 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.

AB - The nonaqueous rechargeable lithium-O2 battery containing an alkyl carbonate electrolyte discharges by formation of C3H 6(OCO2Li)2, Li2CO3, HCO2Li, CH3CO2Li, CO2, and H 2O 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-O2 cells. Oxidation of C3H6(OCO 2Li)2 involves terminal carbonate groups leaving behind the OC3H6O moiety that reacts to form a thick gel on the Li anode. Li2CO3, HCO2Li, CH3CO 2Li, 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.

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U2 - 10.1021/ja2021747

DO - 10.1021/ja2021747

M3 - 文章

AN - SCOPUS:79957673636

SN - 0002-7863

VL - 133

SP - 8040

EP - 8047

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 20

ER -

Reactions in the rechargeable lithium-O₂ battery with alkyl carbonate electrolytes

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