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

Nika Mahne, Bettina Schafzahl, Christian Leypold, Mario Leypold, Sandra Grumm, Anita Leitgeb, Gernot A. Strohmeier, Martin Wilkening, Olivier Fontaine, Denis Kramer, Christian Slugovc, Sergey M. Borisov and Stefan A. Freunberger ()
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Nika Mahne: Institute for Chemistry and Technology of Materials, Graz University of Technology
Bettina Schafzahl: Institute for Chemistry and Technology of Materials, Graz University of Technology
Christian Leypold: Institute for Chemistry and Technology of Materials, Graz University of Technology
Mario Leypold: Institute of Organic Chemistry, Graz University of Technology
Sandra Grumm: Institute for Chemistry and Technology of Materials, Graz University of Technology
Anita Leitgeb: Institute for Chemistry and Technology of Materials, Graz University of Technology
Gernot A. Strohmeier: Institute of Organic Chemistry, Graz University of Technology
Martin Wilkening: Institute for Chemistry and Technology of Materials, Graz University of Technology
Olivier Fontaine: Institut Charles Gerhardt Montpellier
Denis Kramer: Engineering Sciences, University Road, University of Southampton
Christian Slugovc: Institute for Chemistry and Technology of Materials, Graz University of Technology
Sergey M. Borisov: Institute for Analytical Chemistry and Food Chemistry, Graz University of Technology
Stefan A. Freunberger: Institute for Chemistry and Technology of Materials, Graz University of Technology

Nature Energy, 2017, vol. 2, issue 5, 1-9

Abstract: 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. Here we show that 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 trace water. 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.

Date: 2017
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DOI: 10.1038/nenergy.2017.36

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