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Singlet oxygen generation as a major cause for parasitic reactions during cycling of aprotic lithium–oxygen batteries

Singlet oxygen generation as a major cause for parasitic reactions during cycling of aprotic lithium–oxygen batteries
Singlet oxygen generation as a major cause for parasitic reactions during cycling of aprotic lithium–oxygen batteries
Non-aqueous metal–oxygen batteries depend critically on the reversible formation/decomposition of metal oxides on cycling. Irreversible parasitic reactions cause poor rechargeability, efficiency, and cycle life, and have predominantly been ascribed to the reactivity of reduced oxygen species with cell components. These species, however, cannot fully explain the side reactions. Herewe showthat singlet oxygen forms at the cathode of a lithium–oxygen cell during discharge and from the onset of charge, and accounts for the majority of parasitic reaction products. The amount increases during discharge, early stages of charge, and charging at higher voltages, and is enhanced by the presence of tracewater. Superoxide and peroxide appear to be involved in singlet oxygen generation. Singlet oxygen traps and quenchers can reduce parasitic reactions effectively. Awareness of the highly reactive singlet oxygen in non-aqueous metal–oxygen batteries gives a rationale for future research towards achieving highly reversible cell operation.
2058-7546
Mahne, Nika
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Schafzahl, Bettina
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Leypold, Christian
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Leypold, Mario
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Grumm, Sandra
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Leitgeb, Anita
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Strohmeier, Gernot A.
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Wilkening, Martin
02f550aa-0cd1-449c-ac9f-3571d8474474
Fontaine, Olivier
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Kramer, Denis
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Slugovc, Christian
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Borisov, Sergey M.
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Freunberger, Stefan A.
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Mahne, Nika
cca1ea21-ff28-4e75-894e-e261db192a57
Schafzahl, Bettina
de884fe1-3793-42d7-bb6e-dd075530de74
Leypold, Christian
b0aeee7d-f112-47ed-94da-0179014c5251
Leypold, Mario
e81c2d78-2bc8-4a35-bd4f-2235298e8c8d
Grumm, Sandra
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Leitgeb, Anita
156fd5d3-439f-40ce-b728-faf8c7d0da54
Strohmeier, Gernot A.
1deaf740-ec89-4304-ae57-fa822a3459bc
Wilkening, Martin
02f550aa-0cd1-449c-ac9f-3571d8474474
Fontaine, Olivier
75f3a470-acf6-46e9-9cb1-df8a1331c140
Kramer, Denis
1faae37a-fab7-4edd-99ee-ae4c30d3cde4
Slugovc, Christian
37d175ef-a9d4-42b4-9dbb-0060227fc5e9
Borisov, Sergey M.
eceeb922-0fb8-4425-813e-71cd23601921
Freunberger, Stefan A.
06c34029-253f-4f83-94e5-7dde9aa53f07

Mahne, Nika, Schafzahl, Bettina, Leypold, Christian, Leypold, Mario, Grumm, Sandra, Leitgeb, Anita, Strohmeier, Gernot A., Wilkening, Martin, Fontaine, Olivier, Kramer, Denis, Slugovc, Christian, Borisov, Sergey M. and Freunberger, Stefan A. (2017) Singlet oxygen generation as a major cause for parasitic reactions during cycling of aprotic lithium–oxygen batteries. Nature Energy, 2, [17036]. (doi:10.1038/nenergy.2017.36).

Record type: Article

Abstract

Non-aqueous metal–oxygen batteries depend critically on the reversible formation/decomposition of metal oxides on cycling. Irreversible parasitic reactions cause poor rechargeability, efficiency, and cycle life, and have predominantly been ascribed to the reactivity of reduced oxygen species with cell components. These species, however, cannot fully explain the side reactions. Herewe showthat singlet oxygen forms at the cathode of a lithium–oxygen cell during discharge and from the onset of charge, and accounts for the majority of parasitic reaction products. The amount increases during discharge, early stages of charge, and charging at higher voltages, and is enhanced by the presence of tracewater. Superoxide and peroxide appear to be involved in singlet oxygen generation. Singlet oxygen traps and quenchers can reduce parasitic reactions effectively. Awareness of the highly reactive singlet oxygen in non-aqueous metal–oxygen batteries gives a rationale for future research towards achieving highly reversible cell operation.

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Accepted/In Press date: 19 February 2017
e-pub ahead of print date: 20 March 2017
Organisations: Engineering Mats & Surface Engineerg Gp, Energy Technology Group

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Local EPrints ID: 407220
URI: http://eprints.soton.ac.uk/id/eprint/407220
ISSN: 2058-7546
PURE UUID: 27c9f94c-cd04-4c3e-b1ee-537ae28c482b

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Date deposited: 01 Apr 2017 01:07
Last modified: 16 Mar 2024 05:11

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Contributors

Author: Nika Mahne
Author: Bettina Schafzahl
Author: Christian Leypold
Author: Mario Leypold
Author: Sandra Grumm
Author: Anita Leitgeb
Author: Gernot A. Strohmeier
Author: Martin Wilkening
Author: Olivier Fontaine
Author: Denis Kramer
Author: Christian Slugovc
Author: Sergey M. Borisov
Author: Stefan A. Freunberger

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