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Oxygen redox chemistry without excess alkali-metal ions in Na2/3[Mg0.28Mn0.72]O2
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2018 (English)In: Nature Chemistry, ISSN 1755-4330, E-ISSN 1755-4349, Vol. 10, p. 288-295Article in journal (Refereed) Published
Abstract [en]

The search for improved energy-storage materials has revealed Li-and Na-rich intercalation compounds as promising high-capacity cathodes. They exhibit capacities in excess of what would be expected from alkali-ion removal/reinsertion and charge compensation by transition-metal (TM) ions. The additional capacity is provided through charge compensation by oxygen redox chemistry and some oxygen loss. It has been reported previously that oxygen redox occurs in O 2p orbitals that interact with alkali ions in the TM and alkali-ion layers (that is, oxygen redox occurs in compounds containing Li+-O(2p)-Li+ interactions). Na-2/3[Mg0.28Mn0.72]O-2 exhibits an excess capacity and here we show that this is caused by oxygen redox, even though Mg2+ resides in the TM layers rather than alkali-metal (AM) ions, which demonstrates that excess AM ions are not required to activate oxygen redox. We also show that, unlike the alkali-rich compounds, Na-2/3[Mg0.28Mn0.72]O-2 does not lose oxygen. The extraction of alkali ions from the alkali and TM layers in the alkalirich compounds results in severely underbonded oxygen, which promotes oxygen loss, whereas Mg2+ remains in Na-2/3[Mg0.28Mn0.72]O-2, which stabilizes oxygen.

Place, publisher, year, edition, pages
2018. Vol. 10, p. 288-295
National Category
Condensed Matter Physics
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URN: urn:nbn:se:uu:diva-344548DOI: 10.1038/nchem.2923ISI: 000425589000009PubMedID: 29461536OAI: oai:DiVA.org:uu-344548DiVA, id: diva2:1188111
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EU, FP7, Seventh Framework Programme, 290605Available from: 2018-03-06 Created: 2018-03-06 Last updated: 2018-04-25Bibliographically approved

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Massel, FelixDuda, Laurent

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